1,016 results on '"time-resolved"'
Search Results
2. Impact of MoS2 Monolayers on the Thermoelastic Response of Silicon Heterostructures.
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Soranzio, Davide, Puntel, Denny, Tuniz, Manuel, Majchrzak, Paulina E., Milloch, Alessandra, Olsen, Nicholas M., Bronsch, Wibke, Jessen, Bjarke S., Fainozzi, Danny, Pelli Cresi, Jacopo S., De Angelis, Dario, Foglia, Laura, Mincigrucci, Riccardo, Zhu, Xiaoyang, Dean, Cory R., Ulstrup, Søren, Banfi, Francesco, Giannetti, Claudio, Parmigiani, Fulvio, and Bencivenga, Filippo
- Abstract
Understanding the thermoelastic response of a nanostructure is crucial for the choice of materials and interfaces in electronic devices with improved and tailored transport properties at the nanoscale. Here, we show how the deposition of a MoS
2 monolayer can strongly modify the nanoscale thermoelastic dynamics of silicon substrates close to their interface. We demonstrate this by creating a transient grating with extreme ultraviolet light, using ultrashort free-electron laser pulses, whose ≈84 nm period is comparable to the size of elements typically used in nanodevices, such as electric contacts and nanowires. The thermoelastic response, featuring coherent acoustic waves and incoherent relaxation, is tangibly modified by the presence of monolayer MoS2 . Namely, we observed a major reduction of the amplitude of the surface mode, which is almost suppressed, while the longitudinal mode is basically unperturbed, aside from a faster decay of the acoustic modulations. We interpret this behavior as a selective modification of the surface elasticity, and we discuss the conditions to observe such effect, which may be of immediate relevance for the design of Si-based nanoscale devices. [ABSTRACT FROM AUTHOR]- Published
- 2024
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3. Exploring the interaction of a potent anti‐cancer drug Selumetinib with bovine serum albumin: Spectral and computational attributes.
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Jalan, Ankita, Sangeet, Satyam, Pradhan, Amit Kumar, and Moyon, N. Shaemningwar
- Subjects
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SERUM albumin , *FLUORESCENCE resonance energy transfer , *ANTINEOPLASTIC agents , *BLOOD proteins , *CIRCULAR dichroism - Abstract
The binding of drugs to plasma proteins determines its fate within the physiological system, hence profound understanding of its interaction within the bloodstream is important to understand its pharmacodynamics and pharmacokinetics and thereby its therapeutic potential. In this regard, our work delineates the mechanism of interaction of Selumetinib (SEL), a potent anti‐cancer drug showing excellent effect against multiple solid tumors, with plasma protein bovine serum albumin (BSA), using methods such as absorption, steady‐state fluorescence, time‐resolved, fluorescence resonance energy transfer, Fourier transform infrared spectra (FTIR), circular dichroism (CD), synchronous and 3D‐fluorescence, salt fluorescence, molecular docking and molecular dynamic simulations. The BSA fluorescence intensity was quenched with increasing concentration of SEL which indicates interactions of SEL with BSA. Stern–Volmer quenching analysis and lifetime studies indicate the involvement of dynamic quenching. However, some contributions from the static quenching mechanism could not be ruled out unambiguously. The association constant was found to be 5.34 × 105 M−1 and it has a single binding site. The Förster distance (r) indicated probable energy transmission between the BSA and SEL. The positive entropy changes and enthalpy change indicate that the main interacting forces are hydrophobic forces, also evidenced by the results of molecular modeling studies. Conformation change in protein framework was revealed from FTIR, synchronous and 3D fluorescence and CD studies. Competitive binding experiments as well as docking studies suggest that SEL attaches itself to site I (subdomain IIA) of BSA where warfarin binds. Molecular dynamic simulations indicate the stability of the SEL–BSA complex. The association energy between BSA and SEL is affected in the presence of different metals differently. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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4. Scanning transmission X-ray microscopy at the Advanced Light Source
- Author
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Feggeler, Thomas, Levitan, Abraham, Marcus, Matthew A, Ohldag, Hendrik, and Shapiro, David A
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Astronomical Sciences ,Physical Sciences ,Bioengineering ,Affordable and Clean Energy ,X-rays ,Microscopy ,Ptychography ,Tomography ,STXM ,Time-resolved ,Magnetic resonance ,Atomic ,Molecular ,Nuclear ,Particle and Plasma Physics ,Condensed Matter Physics ,Physical Chemistry (incl. Structural) ,Chemical Physics ,Physical chemistry ,Condensed matter physics - Abstract
Over 50 years of development, synchrotron based X-ray microscopy has become a routine and powerful tool for the analysis of nanoscale structure and chemistry in many areas of science. Scanning X-ray microscopy is particularly well suited to the study of chemical and magnetic states of matter and has become available at most synchrotron light sources using a variety of optical schemes, detectors and sample environments. The Advanced Light Source at Lawrence Berkeley National Laboratory has an extensive program of soft X-ray scanning microscopy which supports a broad range of scientific research using a suite of advanced tools for high spatio-temporal resolution and control of active materials. Instruments operating within an energy range between 200–2500 eV with spatial resolution down to 7 nm and sub 20 picosecond time resolution are available. These capabilities can be routinely used in combination with a variety of sample stimuli, including gas or fluid flow, temperature control from 100 to 1200 K, DC bias and pulsed or continuous microwave excitation. We present here a complete survey of our instruments, their most advanced capabilities and a perspective on how they complement each other to solve complex problems in energy, materials and environmental science.
- Published
- 2023
5. Sampling-Based Two-Dimensional Temporal Imaging
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Fang, Qiyin, Richards, Morgan, Wang, Yiping, and Liang, Jinyang, editor
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- 2024
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6. Time-Resolved Sensitivity of a Cadmium-Doped Copper Oxide Thin Film as a Chlorine Gas Detector
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Turki Alotibi, Waleed Shirbeeny, Ahmed Alshahrie, Mohammed Aida, and Jawid Iqbal
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sensor ,bandgap ,affinity ,spray pyrolysis ,time-resolved ,Engineering (General). Civil engineering (General) ,TA1-2040 - Abstract
Due to its strong affinity for chlorine gas, Cd can potentially form CdCl2. Cd-doped CuO thin films are sensitive to chlorine gas, as careful inclusion of Cd in the CuO crystal structure modifies the energy gap depending on the dopant concentration. We employed spray pyrolysis to deposit Cd-doped CuO on FTO (Fluorine Tin Oxide) while heating the substrate to 500 oC. The XRD (X-ray Diffraction) analysis revealed that Cd was interstitially incorporated in the CuO lattice structure, as verified by SEM (Scanning Electron Microscopy imaging). The photoluminescence study demonstrated that increasing the Cd concentration in CuO resulted in higher emission intensity, providing valuable insights into Cu2+ and O2- energy levels. Exposing a Cd-doped CuO thin film to chlorine gas modifies the bandgap, depending on the Cd concentration. The fluctuation in the bandgap energy of copper oxide doped with cadmium indicates the chlorine gas concentration nearby. Time-resolved measurements for the I-V characteristics of the thin film revealed considerable current variation during the exposure to chlorine gas.
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- 2024
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7. Time-resolved scRNA-seq reveals transcription dynamics of polarized macrophages with influenza A virus infection and antigen presentation to T cells
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Jiapei Yu, Congcong Shang, Xiaoyan Deng, Ju Jia, Xiao Shang, Zeyi Wang, Ying Zheng, Rongling Zhang, Yeming Wang, Hui Zhang, Hongyu Liu, William J. Liu, Hui Li, and Bin Cao
- Subjects
Influenza A virus ,time-resolved ,polarized macrophages ,antigen presentation ,specific T cell response ,Infectious and parasitic diseases ,RC109-216 ,Microbiology ,QR1-502 - Abstract
Throughout history, the influenza A virus has caused numerous devastating global pandemics. Macrophages, as pivotal innate immune cells, exhibit a wide range of immune functions characterized by distinct polarization states, reflecting their intricate heterogeneity. In this study, we employed the time-resolved single-cell sequencing technique coupled with metabolic RNA labelling to elucidate the dynamic transcriptional changes in distinct polarized states of bone marrow-derived macrophages (BMDMs) upon infection with the influenza A virus. Our approach not only captures the temporal dimension of transcriptional activity, which is lacking in conventional scRNA-seq methods, but also reveals that M2-polarized Arg1_macrophage cluster is the sole state supporting successful replication of influenza A virus. Furthermore, we identified distinct antigen presentation capabilities to CD4+ T and CD8+ T cells across diverse polarized states of macrophages. Notably, the M1 phenotype, exhibited by (BMDMs) and murine alveolar macrophages (AMs), demonstrated superior conventional and cross-presentation abilities for exogenous antigens, with a particular emphasis on cross-presentation capacity. Additionally, as CD8+ T cell differentiation progressed, M1 polarization exhibited an enhanced capacity for cross-presentation. All three phenotypes of BMDMs, including M1, demonstrated robust presentation to CD4+ regulatory T cells, while displaying limited ability to present to naive CD4+ T cells. These findings offer novel insights into the immunological regulatory mechanisms governing distinct polarized states of macrophages, particularly their roles in restricting the replication of influenza A virus and modulating antigen-specific T cell responses through innate immunity.
- Published
- 2024
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8. Time-Resolved Sensitivity of a Cadmium-Doped Copper Oxide Thin Film as a Chlorine Gas Detector.
- Author
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Alotibi, Turki, Shirbeeny, Waleed, Alshahrie, Ahmed, Aida, Mohammed, and Iqbal, Jawid
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CHLORINE ,COPPER oxide films ,GAS detectors ,CADMIUM oxide ,TIN oxides ,COPPER oxide ,THIN films - Abstract
Due to its strong affinity for chlorine gas, Cd can potentially form CdCl
2 . Cd-doped CuO thin films are sensitive to chlorine gas, as careful inclusion of Cd in the CuO crystal structure modifies the energy gap depending on the dopant concentration. We employed spray pyrolysis to deposit Cd-doped CuO on fluorine tin oxide (FTO) while heating the substrate to 500 °C. The X-ray diffraction (XRD) analysis revealed that Cd was interstitially incorporated in the CuO lattice structure, as verified by scanning electron microscopy (SEM) imaging. The photoluminescence study demonstrated that increasing the Cd concentration in CuO resulted in higher emission intensity, providing valuable insights into Cu2+ and O2- energy levels. Exposing a Cd-doped CuO thin film to chlorine gas modifies the bandgap, depending on the Cd concentration. The fluctuation in the bandgap energy of copper oxide doped with cadmium indicates the chlorine gas concentration nearby. Time-resolved measurements for the I-V characteristics of the thin film revealed considerable current variation during the exposure to chlorine gas. [ABSTRACT FROM AUTHOR]- Published
- 2024
- Full Text
- View/download PDF
9. HyperTRCSS: A hyperspectral time-resolved compressive sensing spectrometer for depth-sensitive monitoring of cytochrome-c-oxidase and blood oxygenation.
- Author
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Li, Natalie C., Ioussoufovitch, Seva, and Diop, Mamadou
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SPECTRAL imaging , *OXYGEN in the blood , *SPECTROMETERS , *IMAGING phantoms , *NEAR infrared spectroscopy - Abstract
Significance: Hyperspectral time-resolved (TR) near-infrared spectroscopy offers the potential to monitor cytochrome-c-oxidase (oxCCO) and blood oxygenation in the adult brain with minimal scalp/skull contamination. We introduce a hyperspectral TR spectrometer that uses compressive sensing to minimize acquisition time without compromising spectral range or resolution and demonstrate oxCCO and blood oxygenation monitoring in deep tissue. Aim: Develop a hyperspectral TR compressive sensing spectrometer and use it to monitor oxCCO and blood oxygenation in deep tissue. Approach: Homogeneous tissue-mimicking phantom experiments were conducted to confirm the spectrometer's sensitivity to oxCCO and blood oxygenation. Twolayer phantoms were used to evaluate the spectrometer's sensitivity to oxCCO and blood oxygenation in the bottom layer through a 10 mm thick static top layer. Results: The spectrometer was sensitive to oxCCO and blood oxygenation changes in the bottom layer of the two-layer phantoms, as confirmed by concomitant measurements acquired directly from the bottom layer. Measures of oxCCO and blood oxygenation by the spectrometer were highly correlated with "gold standard" measures in the homogeneous and two-layer phantom experiments. Conclusions: The results show that the hyperspectral TR compressive sensing spectrometer is sensitive to changes in oxCCO and blood oxygenation in deep tissue through a thick static top layer. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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10. Dynamics of Anions: From Bound to Unbound States and Everything In Between.
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Clarke, Connor J. and Verlet, Jan R.R.
- Abstract
Gas-phase anions present an ideal playground for the exploration of excited-state dynamics. They offer control in terms of the mass, extent of solvation, internal temperature, and conformation. The application of a range of ion sources has opened the field to a vast array of anionic systems whose dynamics are important in areas ranging from biology to star formation. Here, we review recent experimental developments in the field of anion photodynamics, demonstrating the detailed insight into photodynamical and electron-capture processes that can be uncovered. We consider the electronic and nuclear ultrafast dynamics of electronically bound excited states along entire reaction coordinates; electronically unbound states showing that photochemical concepts, such as chromophores and Kasha's rule, are transferable to electron-driven chemistry; and nonvalence states that straddle the interface between bound and unbound states. Finally, we consider likely developments that are sure to keep the field of anion dynamics buoyant and impactful. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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11. The dynamics beamline at SSRF
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Liu, Zhen, Wang, Li-Hua, Jiang, Yong, Tong, Ya-Jun, Zhu, Hua-Chun, Ji, Te, Chen, Min, Jiang, Zheng, and Wei, Xiang-Jun
- Published
- 2024
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12. Using Training Samples as Transitive Information Bridges in Predicted 4D MRI
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Gulamhussene, Gino, Bashkanov, Oleksii, Omari, Jazan, Pech, Maciej, Hansen, Christian, Rak, Marko, Goos, Gerhard, Founding Editor, Hartmanis, Juris, Founding Editor, Bertino, Elisa, Editorial Board Member, Gao, Wen, Editorial Board Member, Steffen, Bernhard, Editorial Board Member, Yung, Moti, Editorial Board Member, Xue, Zhiyun, editor, Antani, Sameer, editor, Zamzmi, Ghada, editor, Yang, Feng, editor, Rajaraman, Sivaramakrishnan, editor, Huang, Sharon Xiaolei, editor, Linguraru, Marius George, editor, and Liang, Zhaohui, editor
- Published
- 2023
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13. Synergising single-cell resolution and 4sU labelling boosts inference of transcriptional bursting
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David M. Edwards, Philip Davies, and Daniel Hebenstreit
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Transcription ,Bursting ,Dynamics ,Inference ,Time-resolved ,4sU ,Biology (General) ,QH301-705.5 ,Genetics ,QH426-470 - Abstract
Abstract Despite the recent rise of RNA-seq datasets combining single-cell (sc) resolution with 4-thiouridine (4sU) labelling, analytical methods exploiting their power to dissect transcriptional bursting are lacking. Here, we present a mathematical model and Bayesian inference implementation to facilitate genome-wide joint parameter estimation and confidence quantification (R package: burstMCMC). We demonstrate that, unlike conventional scRNA-seq, 4sU scRNA-seq resolves temporal parameters and furthermore boosts inference of dimensionless parameters via a synergy between single-cell resolution and 4sU labelling. We apply our method to published 4sU scRNA-seq data and linked with ChIP-seq data, we uncover previously obscured associations between different parameters and histone modifications.
- Published
- 2023
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14. Time-resolved experiments on gas-phase atoms and molecules with XUV and X-ray free-electron lasers
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Daniel Rolles
- Subjects
Free-electron lasers ,atomic and molecular physics ,time-resolved ,pump-probe ,Physics ,QC1-999 - Abstract
ABSTRACTOver the last 20 years, XUV and X-ray free-electron lasers have enabled a wide variety of time-resolved experiments that have dramatically advanced our understanding of ultrafast molecular dynamics on atomic length scales and femtosecond time scales. This review focuses on experimental studies of ultrafast dynamics of atoms and molecules in the gas phase, tracing the development of the field from early proof-of-principle studies to recent pump-probe experiments that elucidate the coupled electronic and nuclear dynamics during photochemical reactions with a temporal resolution that is now extending into the attosecond domain.
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- 2023
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15. Time-resolved transcriptomic and proteomic profiling of Heyndrickxia coagulans during NaOH-buffered L-lactic acid production
- Author
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Xing Huang, Wenzhe Tian, Xiuwen Wang, and Jiayang Qin
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Heyndrickxia coagulans ,L-lactic acid ,sodium hydroxide ,time-resolved ,transcriptomic and proteomic profiling ,Microbiology ,QR1-502 - Abstract
The L-lactic acid (L-LA) fermentation process, based on sodium hydroxide neutralization, demonstrates environmental friendliness during product extraction. However, lactate fermentation is hindered by the pronounced stress effect of sodium lactate on the strain compared with calcium lactate. In this study, we performed time-resolved transcriptomic and proteomic analyses of Heyndrickxia coagulans DSM1 during NaOH-buffered L-LA production. The expression levels of the glycolytic genes demonstrated an initial increase followed by a subsequent decrease, whereas the tricarboxylic acid cycle genes exhibited an initial decrease followed by a subsequent increase throughout the fermentation process. Moreover, we identified clusters of genes consisting of transcription factors and ATP-binding cassette (ABC) transporters that demonstrate a progressive elevation of expression levels throughout the fermentation process, with significant upregulation observed at later stages. This investigation yields valuable insights into the response mechanisms of H. coagulans during NaOH-buffered L-LA fermentation and presents potential targets for metabolic engineering.
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- 2023
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16. Diagnostics of laser-induced plasma from a thin film of oil on a silica wafer
- Author
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Vinić Milica, Kuzmanović Miroslav, Savović Jelena, and Ivković Milivoje
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electron number density ,plasma temperature ,time-integrated ,time-resolved ,Chemistry ,QD1-999 - Abstract
In this study, plasma induced by a nanosecond Nd:YAG laser on thin oil films deposited on a silica wafer was characterized by evaluating the main plasma parameters. Spatially and temporally integrated spectral measurements were performed under experimental conditions optimized for elemental analysis of trace metals in oil. Time-resolved values of the spectral line intensities, electron number density, and plasma temperature were obtained from time-integrated measurements by subtracting averaged spectra recorded at different time delays. The electron number density was estimated using the Stark broadened profile of the hydrogen Balmer alpha line. Ionization temperatures were derived from Mg ionic to atomic line intensity ratios. The obtained apparent values of time-resolved plasma parameters were in the range of 1.1×1017 cm-3 (1.5 μs) to 1.5×1016 cm-3 (4 μs) and 9400 K (3 μs) to 7200 K (5 μs), depending on the delay time. Emission spectra of C2 and CN molecules were used to evaluate the rotational and vibrational temperature.
- Published
- 2023
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17. Ultrafast spectroscopy of photoactive nanomaterials
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Taylor, Victoria C. A., Oliver, Tom, and Gersen, Henkjan
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Ultrafast ,Time-resolved ,Nanomaterials ,Femtosecond ,TA ,TRIR ,2DIR ,Transient absorption ,Two-dimensional infrared ,Localised surface plasmon polaritons ,Excitons ,J-aggregates ,Formamidinium ,Perovskite ,Hybrid perovskite ,Ferroelectric ,Large polaron ,Transient absorption microscope ,Ultrafast microscopy - Abstract
Time-resolved spectroscopy is a versatile tool to investigate ultrafast dynamics. The photoinduced dynamics of photoactive nanomaterials occur over a range of timescales and can be initiated by femtosecond processes. Understanding these dynamics is paramount to inform rational design of new materials. In this thesis I detail ultrafast spectroscopic measurements of several photoactive nanomaterials. Ultrafast transient absorption (TA) was used to investigate the dynamics of localised surface plasmon polaritons on hollow gold nanoshells (HGNs) coupled with excitons in J-aggregates. I determined for the first time, a power dependence to the phonon breathing mode period of HGNs, and investigated the transient response of a novel sample of HGNs, with J-aggregates inside as well as on the outer surface, with TA. Through my pump dependent TA measurements, I was able to isolate the transient signatures associated with J-aggregate HGN hybrid system and I propose that the picosecond response is primarily due to hot electrons rather than plexcitons as has been reported for similar systems. I used two-dimensional infrared spectroscopy to directly measure 470 ± 50 fs and 2.8 ± 0.5 ps time constants associated with the reorientation of formamidinium cations in formamidinium lead iodide perovskite thin films. Molecular dynamics simulations facilitated association of these time constants with the cation agitating about an equilibrium position, with NH2 groups pointing at opposite faces of the inorganic lattice cube, and the cation undergoing 90° flips, respectively. These timescales preclude the existence of stable (anti)ferroelectric domains in formamidinium lead iodide perovskite films which had been theorised to be the source of the unusually high power conversion efficiencies observed in this material. In addition, time-resolved infrared measurements revealed a prominent vibrational transient feature arising from a vibrational Stark shift. In the final results chapter of my thesis, I describe the ultrafast transient absorption microscopy experiment that I constructed, discuss functionality tests on the apparatus, and consider the associated design principles.
- Published
- 2020
18. Multibeam X-ray tomography optical system for narrow-energy-bandwidth synchrotron radiation
- Author
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Wolfgang Voegeli, Haruki Takayama, Xiaoyu Liang, Tetsuroh Shirasawa, Etsuo Arakawa, Hiroyuki Kudo, and Wataru Yashiro
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X-ray tomography ,Time-resolved ,X-ray optics ,X-ray CT ,Multi-beam optics ,Physics ,QC1-999 - Abstract
The design and evaluation experiments of a multibeam X-ray tomography optical system that can be used with synchrotron radiation from sources with a narrow energy bandwidth, i.e. undulator sources, are reported. It consists of silicon single crystals that diffract the incident X-rays to 27 beams, which are used to image a sample. The energy of the beams was aligned with an accuracy sufficient for use at typical undulator beamlines. Projection images of a test sample were collected and successfully reconstructed, showing the feasibility of a high-speed X-ray tomography instrument based on the optical system.
- Published
- 2024
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19. Multi‐Dimensional Characterization of Battery Materials.
- Author
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Ziesche, Ralf F., Heenan, Thomas M. M., Kumari, Pooja, Williams, Jarrod, Li, Weiqun, Curd, Matthew E., Burnett, Timothy L., Robinson, Ian, Brett, Dan J. L., Ehrhardt, Matthias J., Quinn, Paul D., Mehdi, Layla B., Withers, Philip J., Britton, Melanie M., Browning, Nigel D., and Shearing, Paul R.
- Subjects
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SCANNING transmission electron microscopy , *FOCUSED ion beams , *LITHIUM cells - Abstract
Demand for low carbon energy storage has highlighted the importance of imaging techniques for the characterization of electrode microstructures to determine key parameters associated with battery manufacture, operation, degradation, and failure both for next generation lithium and other novel battery systems. Here, recent progress and literature highlights from magnetic resonance, neutron, X‐ray, focused ion beam, scanning and transmission electron microscopy are summarized. Two major trends are identified: First, the use of multi‐modal microscopy in a correlative fashion, providing contrast modes spanning length‐ and time‐scales, and second, the application of machine learning to guide data collection and analysis, recognizing the role of these tools in evaluating large data streams from increasingly sophisticated imaging experiments. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
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20. X‐ray Tomography and Tomoscopy on Metals: A Review.
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García-Moreno, Francisco, Neu, Tillmann Robert, Kamm, Paul Hans, and Banhart, John
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X-rays ,TOMOGRAPHY ,METALS ,THREE-dimensional imaging ,INHOMOGENEOUS materials - Abstract
X‐ray tomography is a versatile tool in materials research and engineering since it allows for a non‐destructive and three‐dimensional mapping of the constituents of a heterogeneous material as long as they differ in their interactions with X‐rays. Recent developments of the technique have brought down the time needed for the acquisition of a single tomogram by many orders of magnitude compared to what was needed 25 years ago. Nowadays, up to 1000 full tomograms can be recorded in a second, which enables real‐time studies of changes in samples caused by reactions or by applied processing operations. The term tomoscopy has been coined for such sequences of 3D images. We review the application of X‐ray tomography and tomoscopy on metals and describe each step required and the associated challenges. A selection of representative investigations is presented with a focus on time‐resolved phenomena in metals and alloys ranging from mechanical deformation, solidification to metals processing processes such as welding and additive manufacturing. Finally likely future developments are discussed. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
21. Photoemission studies of charge transport, passivation and electronic structure for quantum dot solar cells
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Clark, Philippa, Flavell, Wendy, and O'Brien, Paul
- Subjects
620 ,CdO ,synchrotron ,quantum dot solid ,PbS ,electronic structure ,charge transport ,passivation ,photoemission ,time-resolved ,surface chemistry ,solar cell ,ARPES ,XPS ,colloidal quantum dots ,carrier dynamics - Abstract
Colloidal quantum dot (CQD)-based solar cells are a promising technology that could provide low-cost energy in the future. In this thesis the passivation of PbS CQD surfaces, carrier dynamics in PbS CQD-based solar cell systems, and the electronic structure of a potential photoanode material (CdO) are studied using a variety of photoemission spectroscopies and complementary techniques. The surface passivation of PbS CQDs is investigated using X-ray photoelectron spectroscopy (XPS) and synchrotron radiation-excited depth profiling XPS, which gives information on the chemical composition and oxidation state of the surface. PbS CQDs were studied after treatments including Cd cation exchange, halide (Cl, Br, I) ligand exchanges, short organic ligand (EDT) exchange, and combinations of these treatments. For Cd cation exchanged PbS CQDs a thicker Cd shell results in less oxidation, and an optimum effective shell thickness of 0.1 nm provides suffcient protection against oxidation without introducing a large insulating barrier which can hinder charge transfer from the CQD. For combined ligand treatments, evidence of passivants being etched from the surface is found. This significantly reduces the air stability and device performance, which is found to be strongly connected to the number of passivants present on the PbS CQD surface. Laser-pump photoemission-probe spectroscopy is used to investigate both charge transport at the PbS CQD-ZnO photoanode interface, and band bending and carrier dynamics at the surface of PbS CQD solids. Charge injection was observed from PbS CQDs into ZnO, the dynamics of which are limited by the persistent photoconductivity of the ZnO. For PbS CQD solids passivated with EDT, MPA, PbI2, and a quasiperovskite MAI/PbI2 shell, band bending at the solid-vacuum interface is observed for the first time. Comparison of the charge carrier dynamics for different CQD solids show that the dynamics can occur on timescales between microseconds (MAI/PbI2) and seconds (MPA, PbI2). Oxygen contaminants (observed with XPS), creating deep traps, is suggested as the reason for the slower dynamics. The origin of the two-dimensional electron gas (2DEG) on the surface of CdO is also investigated with angle-resolved photoemission and core-level XPS. Surface adsorbates and interstitial hydrogen are found to donate electrons to the surface, occupying conduction band states. The effects on the occupancy of the 2DEG with removal of adsorbates and diffusion of atomic hydrogen via cracking are explored.
- Published
- 2019
22. Time-resolved imaging of magnetisation dynamics using X-ray holography with extended reference and autocorrelation by linear differential operator (HERALDO)
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Bukin, N., Ogrin, F., and van der Laan, G.
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500 ,Magnetisation dynamics ,Landau magnetic vortex domain structure ,X-ray holography ,HERALDO ,Time-resolved ,Stroboscopic measurements ,Micromagnetic simulations - Abstract
Within this thesis the theory and practicality of the holography with extended reference autocorrelation by linear differential operator (HERALDO) technique will be presented and discussed in detail along with the results of a series of experiments performed on nano-scale magnetic elements using this technique. The aim was to investigate the static and dynamic time-dependent behaviour of thin-film square magnetic elements. The magnetic elements were predominantly Permalloy (Py) squares however some contained topological structures whilst others were formed from multiple square elements, creating a larger conjoined structure. Magnetic dynamics were studied by exciting the ground state of the magnetic elements with a pulsed Oersted field produced by applying an electronic pulse through the central signal line of an integrated co-planar waveguide (CPW) which supported the elements. These dynamics were then observed by utilising circularly polarised x-rays from synchrotron sources and exploiting the x-ray magnetic circular dichroism (XMCD) effect. The experimental set-up, data collection and analytical process for each experiment will be discussed in detail with a particular focus on the HERALDO technique and any remarkable results obtained on each of the samples. These results have been supplemented with micromagnetic simulations in order to gain a deeper understanding of what is causing the effects seen. The results of the experiments show that for thicker Py elements (>50 nm) there is a complex three-dimensional structure to the magnetic states that exist within, specifically that out-of-plane magnetic moments are more prominent. Interpretation of the experimental results with micromagnetic simulations showed that the square elements contained out-of-plane magnetic singularities at each corner of the square which could be switched in polarity by magnetic bullet-modes which propagate along the domain walls when the vortex core is excited to gyrate. In addition, when the element is exposed to a moderate strength magnetic field that remains below its saturation magnetisation strength the vortex core distorts into an extended domain wall-like region of both in-plane and out-of-plane magnetisation. Concerning simulations of an element with an off-centre topological structure (defect), when the vortex core gyrates, a series of events occur that cause the polarity of the core to switch. Regarding a structure formed of multiple elements, these samples are able to exhibit one of two ground states: an antivortex (AV) state or a continuous state. The continuous state was observed to result in a more regular vortex core gyration pattern. This result opens up potential for gyration synchronisation of multiple vortex cores which could overcome the limitations of current methods by allowing direct interaction between vortices via the exchange interaction, as opposed to the weaker stray field effects or complex nano-contact spin-torque driven devices.
- Published
- 2019
23. A Sequence Study on the Enhanced Charge Transfer of SWCNTs and CuO-Reinforced Poly(o-anisidine-co-o-toluidine) Nanocomposites.
- Author
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Alsulami, Qana A. and Hussein, Mahmoud A.
- Subjects
- *
CHARGE transfer , *METALLIC composites , *NANOCOMPOSITE materials , *CHARGE exchange , *SCANNING electron microscopy , *COPPER oxide , *POLYMERIC nanocomposites - Abstract
In this study, we investigated the enhanced charge transfer (CT) behaviors of single-walled carbon nanotubes (f-SWCNTs) and copper oxide (CuO)-reinforced poly(o-anisidine-co-o-toluidine) nanocomposites. Prior this study, the targeted nanocomposite materials were fabricated using an in situ oxidative polymerization tool. FT-IR, XRD, and SEM techniques were used to confirm the formation of the pure POA-co-POT copolymer and its related nanocomposites in the presence of f-SWCNTs and CuO nanoparticles. The enhancement of the thermal behavior and conductivity in the presence of either f-SWCNTs or f-SWCNTs/CuO confirms the well-dispersed filler on the polymeric matrix. Additionally, steady-state and time-resolved measurements were performed to monitor the influence of f-SWCNTs and CuO on the optical properties and CT related to the copolymerization process. Our fabricated materials showed a quenching of 25% and 31% in the presence of 10% f-SWCNTs, and 2% f-SWCNTs + 15% CuO, respectively. These findings provided strong evidence for the fast charge transfer within the fabricated nanocomposite, which matched the time-resolved results. The fs measurements showed that the ground state bleach (GSB) kinetics was more rapid in the presence of 10% f-SWCNTs compared to that of the free copolymer, while in the presence of 10% CuO, the electron transfer (ET) was faster, which decayed rapidly with a 0.6 ps time constant supporting the metallic nature of the composite. Our findings suggested that the incorporation of f-SWCNTs and CuO into a polymer matrix can close the gap resulting from polymer limitation. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
24. Dynamic Computed Tomography Angiography as Imaging Method for Endoleak Classification after Endovascular Aneurysm Repair: A Case Series and Systematic Review of the Literature.
- Author
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Boer, Gert Jan, van Engen, Ludo A. H., van Dam, Lievay, van de Luijtgaarden, Koen M., Bokkers, Reinoud P. H., de Vries, Jean-Paul P. M., and Fioole, Bram
- Subjects
- *
ENDOVASCULAR aneurysm repair , *ENDOVASCULAR surgery , *COMPUTED tomography , *ANGIOGRAPHY - Abstract
Introduction: This study evaluated our experience with dynamic computed tomography angiography (dCTA) as a diagnostic tool after endovascular aortic aneurysm repair (EVAR) with respect to the endoleak classification and the available literature. Methods: We reviewed all patients who underwent dCTA because of suspected endoleaks after the EVAR and classified the endoleaks in these patients based on standard CTA (sCTA) and dCTA. We systematically reviewed all available publications that investigated the diagnostic accuracy of dCTA compared with other imaging techniques. Results: In our single-center series, 16 dCTAs were performed in 16 patients. In 11 patients, the undefined endoleaks that appeared on sCTA scans were successfully classified using dCTA. In three patients with a type II endoleak and aneurysm sac growth, inflow arteries were successfully identified using dCTA, and in two patients, aneurysm sac growth was observed without a visible endoleak on both sCTA and dCTA scans. The dCTA revealed four occult endoleaks, all of which were type II endoleaks. The systematic review identified six series comparing dCTA with other imaging methods. All articles reported an excellent outcome regarding the endoleak classification. In published dCTA protocols, the number and timing of phases varied greatly, affecting radiation exposure. Time attenuation curves of the current series show that some phases do not contribute to the endoleak classification and that the use of a test bolus improves the timing of the dCTA. Conclusions: The dCTA is a valuable additional tool that can identify and classify endoleaks more accurately than the sCTA. Published dCTA protocols vary greatly and should be optimized to decrease radiation exposure as long as accuracy can be maintained. The use of a test bolus to improve the timing of the dCTA is recommended, but the optimal number of scanning phases is yet to be determined. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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25. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer.
- Published
- 2024
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- View/download PDF
26. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer.
- Published
- 2024
- Full Text
- View/download PDF
27. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer.
- Published
- 2024
- Full Text
- View/download PDF
28. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer., Validerad;2023;Nivå 2;2023-09-18 (joosat);CC BY 4.0 License
- Published
- 2024
- Full Text
- View/download PDF
29. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer.
- Published
- 2024
- Full Text
- View/download PDF
30. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer., Validerad;2023;Nivå 2;2023-09-18 (joosat);CC BY 4.0 License
- Published
- 2024
- Full Text
- View/download PDF
31. Role of surface morphology in bed particle layer formation on quartz bed particles in fluidized bed combustion of woody biomass
- Abstract
The influence of quartz bed particle surface morphology on the bed particle layer and crack layer formation process in fluidized bed combustion of woody biomass was investigated in this work. Bed material samples were collected at different sampling times from the startup with a fresh bed in industrial scale bubbling fluidized bed (BFB) and circulating fluidized bed (CFB) boilers, both utilizing woody biomass. X-ray microtomography (XMT) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) were employed to characterize bed particle layers and crack layers in the samples. Results showed that there is a noticeable difference between the bed layer characteristics over the so-called “concave” and “convex”-shaped morphologies on the bed particle surface with respect to layer formation. The concave areas are mainly covered with a thin inner layer, whilst the convex display a comparably thick inner layer and an outer layer. In addition, 3D images of the particles revealed that the crack layers mainly originate from concave areas where the particle is less protected by an outer bed particle layer in conjunction with cracks in the inner layer.
- Published
- 2024
- Full Text
- View/download PDF
32. A 512×512 SPAD Image Sensor with Integrated Gating for Widefield FLIM.
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Ulku, Arin C, Bruschini, Claudio, Antolovic, Ivan Michel, Charbon, Edoardo, Kuo, Yung, Ankri, Rinat, Weiss, Shimon, and Michalet, Xavier
- Subjects
CMOS ,FLIM ,SPAD ,fluorescence lifetime imaging microscopy ,image sensor ,phasor analysis ,single-photon avalanche diodes ,time gating ,time-resolved ,widefield ,Optical Physics ,Electrical and Electronic Engineering ,Quantum Physics ,Optoelectronics & Photonics - Abstract
We report on SwissSPAD2, an image sensor with 512×512 photon-counting pixels, each comprising a single-photon avalanche diode (SPAD), a 1-bit memory, and a gating mechanism capable of turning the SPAD on and off, with a skew of 250ps and 344ps, respectively, for a minimum duration of 5.75ns. The sensor is designed to achieve a frame rate of up to 97,700 binary frames per second and sub-40ps gate shifts. By synchronizing it with a pulsed laser and using multiple successive overlapping gates, one can reconstruct a molecule's fluorescent response with picosecond temporal resolution. Thanks to the sensor's number of pixels (the largest to date) and the fully integrated gated operation, SwissSPAD2 enables widefield FLIM with an all-solid-state solution and at relatively high frame rates. This was demonstrated with preliminary results on organic dyes and semiconductor quantum dots using both decay fitting and phasor analysis. Furthermore, pixels with an exceptionally low dark count rate and high photon detection probability enable uniform and high quality imaging of biologically relevant fluorescent samples stained with multiple dyes. While future versions will feature the addition of microlenses and optimize firmware speed, our results open the way to low-cost alternatives to commercially available scientific time-resolved imagers.
- Published
- 2019
33. A 512 × 512 SPAD Image Sensor With Integrated Gating for Widefield FLIM
- Author
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Ulku, Arin Can, Bruschini, Claudio, Antolovic, Ivan Michel, Kuo, Yung, Ankri, Rinat, Weiss, Shimon, Michalet, Xavier, and Charbon, Edoardo
- Subjects
Bioengineering ,CMOS ,image sensor ,FLIM ,fluorescence lifetime imaging microscopy ,single-photon avalanche diodes ,SPAD ,time gating ,time-resolved ,widefield ,phasor analysis ,Optical Physics ,Quantum Physics ,Electrical and Electronic Engineering ,Optoelectronics & Photonics - Abstract
We report on SwissSPAD2, an image sensor with 512×512 photon-counting pixels, each comprising a single-photon avalanche diode (SPAD), a 1-bit memory, and a gating mechanism capable of turning the SPAD on and off, with a skew of 250ps and 344ps, respectively, for a minimum duration of 5.75ns. The sensor is designed to achieve a frame rate of up to 97,700 binary frames per second and sub-40ps gate shifts. By synchronizing it with a pulsed laser and using multiple successive overlapping gates, one can reconstruct a molecule's fluorescent response with picosecond temporal resolution. Thanks to the sensor's number of pixels (the largest to date) and the fully integrated gated operation, SwissSPAD2 enables widefield FLIM with an all-solid-state solution and at relatively high frame rates. This was demonstrated with preliminary results on organic dyes and semiconductor quantum dots using both decay fitting and phasor analysis. Furthermore, pixels with an exceptionally low dark count rate and high photon detection probability enable uniform and high quality imaging of biologically relevant fluorescent samples stained with multiple dyes. While future versions will feature the addition of microlenses and optimize firmware speed, our results open the way to low-cost alternatives to commercially available scientific time-resolved imagers.
- Published
- 2019
34. Perspective: Structure determination of protein-ligand complexes at room temperature using X-ray diffraction approaches
- Author
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Michael A. Hough, Filippo Prischi, and Jonathan A. R. Worrall
- Subjects
X-ray crystallography ,time-resolved ,ambient temperature ,spectroscopy ,protein-ligand complexes ,Biology (General) ,QH301-705.5 - Abstract
The interaction between macromolecular proteins and small molecule ligands is an essential component of cellular function. Such ligands may include enzyme substrates, molecules involved in cellular signalling or pharmaceutical drugs. Together with biophysical techniques used to assess the thermodynamic and kinetic properties of ligand binding to proteins, methodology to determine high-resolution structures that enable atomic level interactions between protein and ligand(s) to be directly visualised is required. Whilst such structural approaches are well established with high throughput X-ray crystallography routinely used in the pharmaceutical sector, they provide only a static view of the complex. Recent advances in X-ray structural biology methods offer several new possibilities that can examine protein-ligand complexes at ambient temperature rather than under cryogenic conditions, enable transient binding sites and interactions to be characterised using time-resolved approaches and combine spectroscopic measurements from the same crystal that the structures themselves are determined. This Perspective reviews several recent developments in these areas and discusses new possibilities for applications of these advanced methodologies to transform our understanding of protein-ligand interactions.
- Published
- 2023
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35. Time and Angle-Resolved Time-of-Flight Electron Spectroscopy for Functional Materials Science.
- Author
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Sorgenfrei, Nomi Lucia Ada Nathalie, Giangrisostomi, Erika, Kühn, Danilo, Ovsyannikov, Ruslan, and Föhlisch, Alexander
- Subjects
- *
X-ray photoelectron spectroscopy , *MATERIALS science , *TIME-of-flight spectroscopy , *PHASE transitions , *PICOSECOND pulses , *ELECTRON spectroscopy - Abstract
Electron spectroscopy with the unprecedented transmission of angle-resolved time-of-flight detection, in combination with pulsed X-ray sources, brings new impetus to functional materials science. We showcase recent developments towards chemical sensitivity from electron spectroscopy for chemical analysis and structural information from photoelectron diffraction using the phase transition properties of 1T-TaS2. Our development platform is the SurfaceDynamics instrument located at the Femtoslicing facility at BESSY II, where femtosecond and picosecond X-ray pulses can be generated and extracted. The scientific potential is put into perspective to the current rapidly developing pulsed X-ray source capabilities from Lasers and Free-Electron Lasers. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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- View/download PDF
36. Photophysical Study on the Rigid Pt(II) Complex [Pt(naphen)(Cl)] (Hnaphen = Naphtho[1,2- b ][1,10]Phenanthroline and Derivatives.
- Author
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Krause, Maren, Maisuls, Iván, Buss, Stefan, Strassert, Cristian A., Winter, Andreas, Schubert, Ulrich S., Nair, Shruthi S., Dietzek-Ivanšić, Benjamin, and Klein, Axel
- Subjects
- *
PHENANTHROLINE derivatives , *PHOSPHORESCENCE spectroscopy , *ELECTROPHILES , *CYCLIC voltammetry , *PHENANTHROLINE , *PHOTOLUMINESCENCE , *PHOSPHORESCENCE , *ATOMS - Abstract
The electrochemistry and photophysics of the Pt(II) complexes [Pt(naphen)(X)] (Hnaphen = naphtho[1,2-b][1,10]phenanthroline, X = Cl or C≡CPh) containing the rigid tridentate C^N^N-coordinating pericyclic naphen ligand was studied alongside the complexes of the tetrahydro-derivative [Pt(thnaphen)(X)] (Hthnaphen = 5,6,8,9-tetrahydro-naphtho[1,2-b][1,10]phenanthroline) and the N^C^N-coordinated complex [Pt(bdq)(Cl)] (Hbdq = benzo[1,2-h:5,4-h']diquinoline. The cyclic voltammetry showed reversible reductions for the C^N^N complexes, with markedly fewer negative potentials (around −1.6 V vs. ferrocene) for the complexes containing the naphen ligand compared with the thnaphen derivatives (around −1.9 V). With irreversible oxidations at around +0.3 V for all of the complexes, the naphen made a difference in the electrochemical gap of about 0.3 eV (1.9 vs. 2.2 eV) compared with thnaphen. The bdq complex was completely different, with an irreversible reduction at around −2 V caused by the N^C^N coordination pattern, which lacked a good electron acceptor such as the phenanthroline unit in the C^N^N ligand naphen. Long-wavelength UV-Vis absorption bands were found around 520 to 530 nm for the C^N^N complexes with the C≡CPh coligand and were red-shifted when compared with the Cl derivatives. The N^C^N-coordinated bdq complex was markedly blue-shifted (493 nm). The steady-state photoluminescence spectra showed poorly structured emission bands peaking at around 630 nm for the two naphen complexes and 570 nm for the thnaphen derivatives. The bdq complex showed a pronounced vibrational structure and an emission maximum at 586 nm. Assuming mixed 3LC/3MLCT excited states, the vibronic progression for the N^C^N bdq complex indicated a higher LC character than assumed for the C^N^N-coordinated naphen and thnaphen complexes. The blue-shift was a result of the different N^C^N vs. C^N^N coordination. The photoluminescence lifetimes and quantum yields ΦL massively increased from solutions at 298 K (0.06 to 0.24) to glassy frozen matrices at 77 K (0.80 to 0.95). The nanosecond time-resolved study on [Pt(naphen)(Cl)] showed a phosphorescence emission signal originating from the mixed 3LC/3MLCT with an emission lifetime of around 3 µs. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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- View/download PDF
37. Experimental Investigation of a Roughness Element Wake on a Hypersonic Flat Plate.
- Author
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Han, Junhao, He, Lin, Xu, Xiwang, and Wu, Zhengbang
- Subjects
BOUNDARY layer (Aerodynamics) ,HYPERSONIC aerodynamics ,LASERS - Abstract
An experimental investigation was performed on the wake flow field of an isolated roughness element of a flat plate at Mach 6 by employing the nanoparticle-based planar laser scattering (NPLS) approach. The three-dimensional features and causes of the flow field structure were scrutinized by transient flow field images of roughness elements on various planes. The time-resolved NPLS technique was implemented to examine the time evolution characteristics of the wake flow field of roughness elements. In the following, the process of dynamic evolution of large-scale vortex structures in the wake flow field was methodically assessed. Additionally, the influences of roughness element heights on the wake vortex structure were evaluated and the obtained results were compared. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
38. Recent advances in structural characterization of biomacromolecules in foods via small-angle X-ray scattering
- Author
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Yang Sun, Xiujuan Li, Ruixin Chen, Fei Liu, and Song Wei
- Subjects
SAXS ,structural characterization ,food biomacromolecules ,modeling ,in situ capabilities ,time-resolved ,Nutrition. Foods and food supply ,TX341-641 - Abstract
Small-angle X-ray scattering (SAXS) is a method for examining the solution structure, oligomeric state, conformational changes, and flexibility of biomacromolecules at a scale ranging from a few Angstroms to hundreds of nanometers. Wide time scales ranging from real time (milliseconds) to minutes can be also covered by SAXS. With many advantages, SAXS has been extensively used, it is widely used in the structural characterization of biomacromolecules in food science and technology. However, the application of SAXS in charactering the structure of food biomacromolecules has not been reviewed so far. In the current review, the principle, theoretical calculations and modeling programs are summarized, technical advances in the experimental setups and corresponding applications of in situ capabilities: combination of chromatography, time-resolved, temperature, pressure, flow-through are elaborated. Recent applications of SAXS for monitoring structural properties of biomacromolecules in food including protein, carbohydrate and lipid are also highlighted, and limitations and prospects for developing SAXS based on facility upgraded and artificial intelligence to study the structural properties of biomacromolecules are finally discussed. Future research should focus on extending machine time, simplifying SAXS data treatment, optimizing modeling methods in order to achieve an integrated structural biology based on SAXS as a practical tool for investigating the structure-function relationship of biomacromolecules in food industry.
- Published
- 2022
- Full Text
- View/download PDF
39. Performance of Boltzmann and crossover single-emitter luminescent thermometers and their recommended operation modes
- Author
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Markus Suta
- Subjects
Luminescence thermometry ,Boltzmann ,Crossover ,TADF ,Ratiometric ,Time-resolved ,Applied optics. Photonics ,TA1501-1820 ,Optics. Light ,QC350-467 - Abstract
Despite its simplicity, Boltzmann thermometry suffers from limited relative sensitivities since the energy gap must be in the order of magnitude of the thermal energy used for probing. Luminescent crossover thermometry is a potential alternative to exploit high energy gaps at low temperatures based on a generally high non-radiative coupling rate via a configurational crossover. The number of possible candidates for this type of temperature-dependent luminescence is quite versatile. Inorganic systems include transition metal ions with split d orbitals in a ligand field such as Cr3+ and Mn4+, mercury-like s2 ions such as Bi3+ or Pb2+ with coupled 3P0 and 3P1 levels, or lanthanoid ions with low energetic 4fn-15d1 levels next to their 4fn spin-orbit levels. In the case of organic emitters, thermally activated delayed fluorescence (TADF) has become increasingly popular, which relies on thermal coupling between an excited singlet and triplet state via intersystem crossing. While the general concept of two thermally excited radiatively emitting states is valid for each of the mentioned types of luminophores and thus, thermometry is in principle possible, the mechanistic details of the thermal coupling can be different. In this tutorial and theoretically motivated article, I will shortly review the relevant aspects of the excited state kinetics of two thermally coupled levels and demonstrate how the ratio between radiative and intrinsic non-radiative coupling rates affects the possible readout choices for optical signals used as a measure for temperature and how this influences the relative sensitivity of ratiometric and lifetime-based thermometers. An overview over various possible inorganic and organic emitters with the potential for thermometry will be given and based on these kinetic considerations, it will be assessed what readout mode is most recommendable for a given luminescent center.
- Published
- 2022
- Full Text
- View/download PDF
40. Insights into the oxygen-evolving mechanism of photosynthesis using XFELs
- Author
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Young, Iris Diane, Ibrahim, Mohamed, Chatterjee, Ruchira, Fuller, Franklin, Gul, Sheraz, Brewster, Aaron, Sauter, Nicholas, Kern, Jan, Yachandra, Vittal, and Yano, Junko
- Subjects
Inorganic Chemistry ,Chemical Sciences ,photosynthesis ,XFEL ,time-resolved ,Condensed Matter Physics ,Analytical Chemistry ,Physical Chemistry (incl. Structural) ,Inorganic & Nuclear Chemistry - Published
- 2017
41. Time‐Resolved Luminescent Sensing and Imaging for Enzyme Catalytic Activity Based on Responsive Probes.
- Author
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Wang, Jiawei, Jin, Yibiao, Li, Mingdang, Liu, Shujuan, Kam‐Wing Lo, Kenneth, and Zhao, Qiang
- Subjects
- *
CATALYTIC activity , *HIGH throughput screening (Drug development) , *ENZYMES , *METAL catalysts , *BIOMACROMOLECULES , *SIGNAL-to-noise ratio - Abstract
Enzymes, as a kind of biomacromolecules, play an important role in many physiological processes and relate directly to various diseases. Developing an efficient detection method for enzyme activity is important to achieve early diagnosis of enzyme‐relevant diseases and high throughput screening of potential enzyme‐relevant drugs. Time‐resolved luminescence assay provide a high accuracy and signal‐to‐noise ratios detection methods for enzyme activity, which has been widely used in high throughput screening of enzyme‐relevant drugs and diagnosis of enzyme‐relevant diseases. Inspired by these advantages, various responsive probes based on metal complexes and metal‐free organic compounds have been developed for time‐resolved bioimaging and biosensing of enzyme activity owing to their long luminescence lifetimes, high quantum yields and photostability. In this review, we comprehensively reviewed metal complex‐ and metal‐free organic compound‐based responsive probes applied to detect enzyme activity through time‐resolved imaging, including their design strategies and sensing principles. Current challenges and future prospects in this rapidly growing field are also discussed. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
42. Free-breathing time-resolved 4D MRI with improved T1-weighting contrast.
- Author
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Chen J, Xia D, Huang C, Shanbhogue K, Chandarana H, and Feng L
- Abstract
This work proposes MP-Grasp4D (magnetization-prepared golden-angle radial sparse parallel 4D) MRI, a free-breathing, inversion recovery (IR)-prepared, time-resolved 4D MRI technique with improved T1-weighted contrast. MP-Grasp4D MRI acquisition incorporates IR preparation into a radial gradient echo sequence. MP-Grasp4D employs a golden-angle navi-stack-of-stars sampling scheme, where imaging data of rotating radial stacks and navigator stacks (acquired at a consistent rotation angle) are alternately acquired. The navigator stacks are used to estimate a temporal basis for low-rank subspace-constrained reconstruction. This allows for the simultaneous capture of both IR-induced contrast changes and respiratory motion. One temporal frame of the imaging volume in MP-Grasp4D MRI is reconstructed from a single stack and an adjacent navigator stack on average, resulting in a nominal temporal resolution of 0.16 seconds per volume. Images corresponding to the optimal inversion time (TI) can be retrospectively selected for providing the best image contrast. Reader studies were conducted to assess the performance of MP-Grasp4D MRI in liver imaging across 30 subjects in comparison with standard Grasp4D MRI without IR preparation. MP-Grasp4D MRI received significantly higher scores (P < 0.05) than Grasp4D in all assessment categories. There was a moderate to almost perfect agreement (kappa coefficient from 0.42 to 0.9) between the two readers for image quality assessment. When the scan time is reduced, MP-Grasp4D MRI preserves image contrast and quality, demonstrating additional acceleration capability. MP-Grasp4D MRI improves T1-weighted contrast for free-breathing time-resolved 4D MRI and eliminates the need for explicit motion compensation. This method is expected to be valuable in different MRI applications such as MR-guided radiotherapy., (© 2024 John Wiley & Sons Ltd.)
- Published
- 2024
- Full Text
- View/download PDF
43. Global transcription regulation revealed from dynamical correlations in time-resolved single-cell RNA sequencing.
- Author
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Volteras D, Shahrezaei V, and Thomas P
- Subjects
- Humans, Bayes Theorem, Transcriptome genetics, Stochastic Processes, Single-Cell Analysis methods, Sequence Analysis, RNA methods, Transcription, Genetic genetics, Gene Expression Regulation genetics, Cell Cycle genetics
- Abstract
Single-cell transcriptomics reveals significant variations in transcriptional activity across cells. Yet, it remains challenging to identify mechanisms of transcription dynamics from static snapshots. It is thus still unknown what drives global transcription dynamics in single cells. We present a stochastic model of gene expression with cell size- and cell cycle-dependent rates in growing and dividing cells that harnesses temporal dimensions of single-cell RNA sequencing through metabolic labeling protocols and cel lcycle reporters. We develop a parallel and highly scalable approximate Bayesian computation method that corrects for technical variation and accurately quantifies absolute burst frequency, burst size, and degradation rate along the cell cycle at a transcriptome-wide scale. Using Bayesian model selection, we reveal scaling between transcription rates and cell size and unveil waves of gene regulation across the cell cycle-dependent transcriptome. Our study shows that stochastic modeling of dynamical correlations identifies global mechanisms of transcription regulation. A record of this paper's transparent peer review process is included in the supplemental information., Competing Interests: Declaration of interests The authors declare no competing interests., (Copyright © 2024 The Authors. Published by Elsevier Inc. All rights reserved.)
- Published
- 2024
- Full Text
- View/download PDF
44. Towards Visualising and Understanding Patient-Specific Biomechanics of Abdominal Aortic Aneurysms
- Author
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Beinart, K. R., Bourantas, George C., Miller, Karol, Miller, Karol, editor, Wittek, Adam, editor, Joldes, Grand, editor, Nash, Martyn P., editor, and Nielsen, Poul M. F., editor
- Published
- 2020
- Full Text
- View/download PDF
45. Photophysical studies of 2-Aminopurine in DNA
- Author
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McKenzie, Grant, Jones, Anita, and Alexander, Andrew
- Subjects
photophysical ,fluorescence ,2-aminopurine ,DNA ,ultrafast ,time-resolved - Abstract
Deoxyribonucleic acid (DNA) forms the basis of all known living organisms. Despite the essential role played by DNA, its dynamic system and functional behaviour are still not completely understood. The work presented in this thesis aims to explore the structural dynamics of DNA systems, using fluorescence-based approaches, and to attempt to develop a technique for the measurement of fluorescence decays of biological molecules on the ultrafast (femtosecond) timescale. Absorption of UV radiation by DNA is known to lead to mutations and damage to DNA structure and functionality. For the majority of absorbed photons, the excitation energy dissipates harmlessly as heat, but in some instances this energy transfers to regions of DNA that are more susceptible to damage. 2-Aminopurine (2AP), a fluorescent analogue of the native DNA base adenine, can be incorporated into DNA with minimal perturbation to the DNA structure, and can be used to investigate inter-base electronic energy transfer. By selectively exciting the native DNA base in 2AP-containing dinucleotides and utilising 2AP fluorescence as an energy acceptor, the mechanism of electronic energy transfer has been investigated. Analysis of the resulting fluorescence lifetimes of 2AP has revealed that energy transfer preferentially excites conformations in which the bases are highly stacked, and the fluorescence of 2AP is highly quenched. This has led to a re-evaluation of energy transfer efficiencies between the natural bases and 2AP, and has shown that transfer efficiencies cannot be determined correctly from steady-state fluorescence measurements. To investigate the influence of base dynamics on the quenching of 2AP fluorescence in DNA, time-resolved fluorescence measurements were carried out on 2AP-containing systems in frozen solution at 77 K. These studies included dinucleotides, single–strand oligonucleotides and their corresponding duplexes. In all cases, comparison of the fluorescence decay parameters measured at room temperature with those measured at 77 K showed that elimination of base dynamics prevented rapid quenching, on the 10s of ps timescale or faster, although quenching on the 100s of ps timescale persisted for 2AP in single strands and duplexes. The multi-exponential fluorescence decay of 2AP in DNA and its high sensitivity to local environment is commonly exploited to investigate DNA-enzyme interactions. Transposases are enzymes involved in the movement of sections of DNA (transposons) within the genome. The Mos1 transposase catalyses the movement of a transposon via a cut-and-paste mechanism involving several intermediate complexes. Understanding the complex mechanism by which the transposase can remove and insert a section of DNA would allow these enzymes to be used as biomolecular tools. The structure of the intermediate Mos1 strand-transfer complex (STC) has been investigated by incorporating 2AP into several regions of the transposon and analysing the fluorescence decay. The involvement of a base-flipping-like mechanism has been identified in the mechanism of strand transfer for the Mos1 transposon. The time-resolved fluorescence measurements performed in this thesis are limited to time resolution of ~20 ps and longer using TSCPC. However, an abundance of photophysical events in DNA occur on the femtosecond timescale. Development of a methodology utilising fluorescence gating techniques (such as sum-frequency generation or diffraction from a transient grating) have been attempted, in order to construct an experimental system that enables the broadband detection of ultrafast fluorescence decays. Despite the lack of immediate success in recording the fluorescence decay from a sample, due to technical issues and time-constraints, initial characterisation of the set-up was performed and the prospect of broadband detection was demonstrated. Overall, this thesis gives insight into some of the dynamic processes taking place in DNA and presents work performed to develop a system that would allow the extension of these studies to processes occurring on the fs timescale.
- Published
- 2017
46. Light-induced radical formation and isomerization of an aromatic thiol in solution followed by time-resolved x-ray absorption spectroscopy at the sulfur K-edge
- Author
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Huse, Nils [Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany). Dept. of Physics; Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)] (ORCID:0000000232817600)
- Published
- 2017
- Full Text
- View/download PDF
47. Internal quantum efficiency and carrier dynamics in semipolar (2021) InGaN/GaN light-emitting diodes
- Author
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Feezell, Daniel [Univ. of New Mexico, Albuquerque, NM (United States)]
- Published
- 2017
- Full Text
- View/download PDF
48. Time-resolved photoacoustic response of thin solids measured using minimal volume cell.
- Author
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Galovic, S.P., Stanimirovic, Z., Stanimirovic, I., Djordjevic, K.Lj., Milicevic, D., and Suljovrujic, E.
- Subjects
- *
CELL size , *PHOTOACOUSTIC effect , *MATERIALS testing , *INVERSE problems , *TRANSFER functions , *PHOTOPLETHYSMOGRAPHY - Abstract
The photoacoustic effect was explained more than half a century ago and has since been used to develop non-destructive and non-contact techniques for testing materials. Most existing experimental setups are time-consuming. In this paper, we deal with the development of time-resolved photoacoustics to use all the advantages of photoacoustic techniques in the development of real-time characterization of various samples. We propose a model for a time-resolved photoacoustic signal of thin samples measured in a gas-microphone setup with a minimal volume cell, assuming that the gas column in the cell can be shorter than the thermal diffusion length in air. The derived model additionally includes the influence of thermal relaxations and detector transfer function. We also suggest a methodology for inverse problem solving, i.e., to determine the sample properties from measured signals using the presented model. The model has been validated by comparing the model predictions with an experimentally measured signal for a thin metallic sample excited by an optical pulse train of a repetition rate of 12 Hz. The results obtained by the suggested inverse-problem solving methodology are in accordance with the literature, thus confirming the validity of the proposed methodology. We have shown that the proposed model and the methodology of inverse time-resolved photoacoustic problems give the same results as the widespread time-consuming frequency photoacoustic measurements. This means that the presented model and methodology enable the employment of low-frequency time-resolved gas-microphone photoacoustics in the real-time characterization of thin solids. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
49. Dynamic Computed Tomography Angiography as Imaging Method for Endoleak Classification after Endovascular Aneurysm Repair: A Case Series and Systematic Review of the Literature
- Author
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Gert Jan Boer, Ludo A. H. van Engen, Lievay van Dam, Koen M. van de Luijtgaarden, Reinoud P. H. Bokkers, Jean-Paul P. M. de Vries, and Bram Fioole
- Subjects
abdominal aortic aneurysm ,EVAR ,endoleak ,computed tomography angiography ,dynamic ,time-resolved ,Medicine (General) ,R5-920 - Abstract
Introduction: This study evaluated our experience with dynamic computed tomography angiography (dCTA) as a diagnostic tool after endovascular aortic aneurysm repair (EVAR) with respect to the endoleak classification and the available literature. Methods: We reviewed all patients who underwent dCTA because of suspected endoleaks after the EVAR and classified the endoleaks in these patients based on standard CTA (sCTA) and dCTA. We systematically reviewed all available publications that investigated the diagnostic accuracy of dCTA compared with other imaging techniques. Results: In our single-center series, 16 dCTAs were performed in 16 patients. In 11 patients, the undefined endoleaks that appeared on sCTA scans were successfully classified using dCTA. In three patients with a type II endoleak and aneurysm sac growth, inflow arteries were successfully identified using dCTA, and in two patients, aneurysm sac growth was observed without a visible endoleak on both sCTA and dCTA scans. The dCTA revealed four occult endoleaks, all of which were type II endoleaks. The systematic review identified six series comparing dCTA with other imaging methods. All articles reported an excellent outcome regarding the endoleak classification. In published dCTA protocols, the number and timing of phases varied greatly, affecting radiation exposure. Time attenuation curves of the current series show that some phases do not contribute to the endoleak classification and that the use of a test bolus improves the timing of the dCTA. Conclusions: The dCTA is a valuable additional tool that can identify and classify endoleaks more accurately than the sCTA. Published dCTA protocols vary greatly and should be optimized to decrease radiation exposure as long as accuracy can be maintained. The use of a test bolus to improve the timing of the dCTA is recommended, but the optimal number of scanning phases is yet to be determined.
- Published
- 2023
- Full Text
- View/download PDF
50. Novel developments in time-of-flight particle imaging
- Author
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Lee, Jason W. L. and Vallance, Claire
- Subjects
539.7 ,Chemistry, Physical and theoretical ,Particles (Nuclear physics) ,Dynamics ,physics ,particle imaging ,time-of-flight ,chemistry ,dynamics ,PImMS ,electron impact ,velocity-map imaging ,neutron imaging ,time-resolved ,CMOS sensors - Abstract
In the field of physical chemistry, the relatively recently developed technique of velocity-map imaging has allowed chemical dynamics to be explored with a greater depth than could be previously achieved using other methods. Capturing the scattering image associated with the products resulting from fragmentation of a molecule allows the dissociative pathways and energy landscape to be investigated. In the study of particle physics, the neutron has become an irreplaceable spectroscopic tool due to the unique nature of the interaction with certain materials. Neutron spectroscopy is a non-destructive imaging technique that allows a number of properties to be discerned, including chemical identification, strain tensor measurements and the identification of beneath the sample surface using radiography and tomography. In both of these areas, as well as a multitude of other disciplines, a flight tube is used to separate particles, distinguishing them based upon their mass in the former case and their energy in the latter. The experiments can be vastly enhanced by the ability to record both the position and arrival time of the particle of interest. This thesis describes several new developments made in instrumentation for experiments involving time-of-flight particle imaging. The first development described is the construction of a new velocity-map imaging instrument that utilises electron ionisation to perform both steps of molecular fragmentation and ionisation. Data from CO2 is presented as an example of the ability of the instrument, and a preliminary analysis of the images is performed. The second presented project is the design of a time-resolved and position-resolved detector developed for ion imaging experiments. The hardware, software and firmware are described and presented alongside data from a variety of the experiments showcasing the breadth of investigations that are possible using the sensor. Finally, the modifications made to the detector to allow time-resolved neutron imaging are detailed, with an in-depth description of the various proof-of-concept experiments carried out as part of the development process.
- Published
- 2016
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