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Metal halide perovskite quantum dots (PQDs) have emerged as promising materials due to their exceptional photoluminescence (PL) properties. A wide range of applications could benefit from adjustable luminescence properties, while preserving the physical and chemical properties of the PQDs. Therefore, post‐synthesis engineering has gained attention recently, involving the use of ion‐exchange or external stimuli, such as extreme pressure, magnetic and electric fields. Nevertheless, these methods typically suffer from spectrum broadening, intensity quenching or yield multiple bands. Alternatively, photonic antennas can modify the radiative decay channel of perovskites via the Purcell effect, with the largest wavelength shift being 8 nm to date, at an expense of fivefold intensity loss. Here, this work presents an optical nanoantenna array with polarization‐controlled quasi‐bound‐states‐in‐the‐continuum resonances, which can engineer and shift the photoluminescence wavelength over a ≈39 nm range and confers a 21‐fold emission enhancement of FAPbI3 perovskite QDs. The spectrum is engineered in a non‐invasive manner via lithographically defined antennas and the pump laser polarization at ambient conditions. This research provides a path toward advanced optoelectronic devices, such as spectrally tailored quantum emitters and lasers. [ABSTRACT FROM AUTHOR]

Surface crack detection and sizing is essential for the manufacturing and maintenance of engines, run parts, and other metal elements of aircrafts. Among various non-destructive detection methods, the fully non-contact and non-intrusive technique based on laser-stimulated lock-in thermography (LLT) has recently attracted a lot of attention from the aerospace industry. We propose and demonstrate a system of reconfigurable LLT for three-dimensional surface crack detection in metal alloys. For large area inspection, the multi-spot LLT can speed up the inspection time by a factor of the number of spots. The minimum resolved size of micro-holes is ~50 µm in diameter limited by the magnification of the camera lens. We also study the crack length ranging from 0.8 to 3.4 mm by varying the modulation frequency of LLT. An empirical parameter related to the thermal diffusion length is found to show the linear dependence with the crack length. With the proper calibration, this parameter can be used to predict the sizing of the surface fatigue cracks. Reconfigurable LLT allows us to quickly locate the crack position and accurately measure its dimensions. This method is also applicable to the non-destructive detection of surface or sub-surface defect in other materials used in various industries. [ABSTRACT FROM AUTHOR]

Label-free optical biosensors using nanophotonic concepts have made substantial progress in the past few years because of their ability to realize fast, compact, and cost-effective chemical detection devices. Among those, high-refractive-index dielectric Mie nanoresonators hold promise for deep miniaturization of biosensing devices while maintaining high sensitivity and low dissipative losses. In this work, we report a high-sensitivity and small-footprint refractive index sensor based on this concept. The device consists of a one-dimensional chain of coupled silicon nanoresonators supporting high-quality-factor collective Mie modes. Measurements with aqueous glycerol solutions show a high sensitivity range of 420-440 nm/refractive index unit (RIU) and a maximum figure of merit of 2700 RIU-1. Being fully compatible with standard complementary metal-oxide semiconductor processes and having a small sensing area of only 0.5 × 18.2 μm2, this design, once arranged in arrays functionalized for different analytes, we believe could become an attractive solution to realizing lab-on-a-chip sensor arrays for high-performance, label-free multiplexing in a cost-effective way. [ABSTRACT FROM AUTHOR]

A Novel scalable approach using Terahertz (THz) waves together with the electromagnetic field simulation was applied to investigate four rabbits of eight rabbit corneas in vivo. One eye of each rabbits' corneas was edema induced; the other eye of the corneas served as the control. The simulation revealed the propagation of THz waves at a certain distance along the sub‐surface of the cornea. THz spectra have been collected close to the corneal surface by deviating the direct reflection of the THz beam for the edema cornea, the reflected wave intensity for edema corneas is generally larger compared with the control cornea. Upon edema becomes severe at the end of the observation, the reflected wave intensities obtained by detector corresponding to the corneal deep stroma layer approach to the same value for all observed corneas. Good correlation is observed between central corneal thickness measurements and THz wave reflection signal intensities. Our results demonstrated that THz spectroscopy technique could obtain the information from different corneal sublayers. [ABSTRACT FROM AUTHOR]

The relationship between charge carrier lifetime and mobility in a bulk heterojunction based organic solar cell, utilizing diketopyrrolopyrole-naphthalene co-polymer and PC71BM in the photoactive blend layer, is investigated using the photoinduced charge extraction by linearly increasing voltage technique. Light intensity, delay time, and temperature dependent experiments are used to quantify the charge carrier mobility and density as well as the temperature dependence of both. From the saturation of photoinduced current at high laser intensities, it is shown that Langevin-type bimolecular recombination is present in the studied system. The charge carrier lifetime, especially in Langevin systems, is discussed to be an ambiguous and unreliable parameter to determine the performance of organic solar cells, because of the dependence of charge carrier lifetime on charge carrier density, mobility, and type of recombination. It is revealed that the relation between charge mobility (μ) and lifetime (τ) is inversely proportional, where the μτ product is independent of temperature. The results indicate that in photovoltaic systems with Langevin type bimolecular recombination, the strategies to increase the charge lifetime might not be beneficial because of an accompanying reduction in charge carrier mobility. Instead, the focus on non-Langevin mechanisms of recombination is crucial, because this allows an increase in the charge extraction rate by improving the carrier lifetime, density, and mobility simultaneously. [ABSTRACT FROM AUTHOR]

Infrared Free electron laser (FEL) is used that induced isotopically selective multiphoton dissociation of PhSiF3 molecules in the gaseous phase. The longer and broader FEL pulse is partially responsible for the lower selectivity. FEL experiments with PhSiF3 performed in a batch mode may also be responsible for the lower selectivity.

Polymer-grafted porous hollow silica nanoparticles prepared by reversible addition–fragmentation chain transfer polymerisation have an upper critical solution temperature of 45 °C. Conjugation of 5 nm gold nanoparticles onto polymer-grafted porous hollow silica nanoparticles enables remarkable specific photothermally-induced controlled release of encapsulated Rhodamine B by laser-stimulation at physiological temperature. [ABSTRACT FROM AUTHOR]

Herein, we report the solution phase self-assembly between Eu(iii) and a rigid ditopic tridentate terpyridine ligand which results in the formation of supramolecular metallo-networks in the solid state. Depending on the ligand to metal ratio used for the initial self-assembly process, the morphology of these materials can be altered from one-dimensional micron-sized fibres to a three-dimensional coordination network. The terpyridine-based ditopic ligand can act as an efficient sensitizer for Eu(iii) emission whereby the emission lifetimes and ligand triplet state energies of the metallo-polymers strongly depend on the ligand to metal ratio. The obtained micron-sized fibres can act as an efficient optical wave-guide for Eu(iii) emission. [ABSTRACT FROM AUTHOR]

A new class of soluble Eu(iii) coordination polymers based on a tridentate ditopic pybox ligand has been developed displaying high metal emission quantum yields of up to 73% as well as a unique dynamic behaviour in solution. [ABSTRACT FROM AUTHOR]

Patterned arrays of light-responsive microchambers are suggested as candidates for site-specific release of chemicals in small and precisely defined quantities on demand. A composite film is made of poly(allylammonium)-poly(styrene sulfonate) multilayers and gold nanoparticles incorporated between subsequent stacks of polyelectrolytes. The film shaped as microchambers is loaded with colloid particles or oil-soluble molecules. The microchambers are sealed onto a glass slide precoated with an adhesive poly(diallyldimethylammonium)-poly(styrene sulfonate) multilayer film. A focused laser beam is used for remote addressing the individual microchambers and site-specific release of the loaded cargo. [ABSTRACT FROM AUTHOR]

A new apparatus for nanosecond-time-resolved Brewster angle reflectometry is described that can be used to measure transient angle-resolved reflectivity changes in thin films and monolayers in a single pulsed laser shot. In order to achieve this, a cylindrical lens is placed in the probe beam path replacing the goniometer that is usually used for angular scanning in other systems. Using two synchronized nanosecond pulsed lasers in pump-probe configuration it is possible to measure the kinetics of photo induced conformational changes by altering the delay between pump and probe pulses. The system was used to observe nanosecond time-resolved photodynamics in a spiropyran monolayer at the air-water interface. After UV excitation the spiropyran converted to its merocyanine form in two stages. The first stage occurred with a timescale close to the instrument time resolution (tens of nanoseconds) whereas the second stage occurred over a few hundred nanoseconds. [ABSTRACT FROM AUTHOR]

We report the photochromic properties of amorphous MoO3 films deposited by dc sputtering with different O2 flow rates. The kinetics of film coloration under UV light irradiation is determined using optical transmission spectroscopy. Changes in the absorbance and refractive index were derived from the analysis of transmittance spectra. The absorbance spectra exhibited a growing broad peak centered around 830 nm, which was induced by the UV irradiation. In the early stages of irradiation, the absorbance of the films did not change but their refractive indices did change. This induction time was correlated with the O2 partial pressure during the film deposition, which was controlled by the O2 flow rate. The origins of this observation are discussed. [ABSTRACT FROM AUTHOR]

Triethylamine (TEA)-water mixtures have a critical-temperature (Tc). Below Tc the mixture exists as one phase and above Tc it exists in two phases. The de-mixed volume is different to the mixed volume. A nanosecond pulsed-laser heated a TEA-water mixture so that it de-mixed. The resulting dynamics of volume expansion were monitored using interferometry. For T-jumps within the one phase region the dynamics of volume change were limited by the speed of sound. However, T-jumps between the one and two phase regions also manifested a slower volume change associated with the de-mixing process. After 150 ns, the volume of the de-mixed TEA-water was consistent with the equilibrium volume change. This suggests that, within 150 ns, the system had split into phase-domains having equilibrium compositions of TEA and water. Subsequently the phase domains would simply merge and grow resulting in no further volume change to reduce surface tension between the phases. [ABSTRACT FROM AUTHOR]

Infrared multiphoton absorption and dissociation of chloromethyltrifluorosilane molecules under the action of pulsed transversely excited atmospheric pressure CO2 laser were experimentally studied. Dissociation products were analyzed. The dissociation proceeds via chlorine atom transfer from carbon to silicone. High degrees of silicon isotope separation were achieved. The presence of α-chlorine atom in a silicon organic compound brings about a significant improvement in multiple photon dissociation characteristics and an essential increase in isotopic selectivity. [ABSTRACT FROM AUTHOR]

A method is presented that enables the determination of transient absorption in Langmuir films made from a monolayer of spiropyran on water. This is achievable even though the optical pathlength of such a monolayer is < 10-9 m. The approach is to monitor reflectivity changes close to the Brewster angle, where the background of reflected light is minimized. This is the key to the sensitivity of the method. Relatively speaking the small changes in reflectivity due to changes in both real and imaginary parts of the refractive index are easier to observe with the intrinsically low backgrounds at the Brewster angle. Notably using Fresnel equations we can show that the real and imaginary parts of the refractive index can be independently assessed for ultrathin films and monolayers using the approach presented. [ABSTRACT FROM AUTHOR]

A nanosecond pulsed IR (1.9 μm) laser rapidly heated water, in an open vessel, to temperatures well below the boiling point. The subsequent dynamics of volume expansion were monitored using time-resolved interferometry in order to measure the increase in the water level in the heated area. The water expanded at less than the speed of sound, taking just less than 100 ns to increase its height by ∼500 nm at surface temperature jumps of 20 K. The initial expansion was followed by an apparent contraction and then a re-expansion. The first expansion phase occurred more slowly than the timescale for bulk H-bond re-structuring of the water, as determined from vibrational bands in the Raman spectra, and represents the limit to the rate at which the overpressure caused by sudden heating can be released. The second phase of the expansion was caused by hydrodynamic effects and is accompanied by morphological changes resulting in light scattering as well as droplet spallation. [ABSTRACT FROM AUTHOR]

The possibility of positional isomer separation induced by radiation of an infrared free electron laser has been demonstrated. Experiments were carried out in 1:1 mixture of para- and meta-hexafluoroxylenes in gaseous phase. Wide tunability of free electron laser allowed for enrichment of the reaction mixture either by meta- or para-isomer. The maximum isomer selectivity achieved, defined as a ratio of dissociation yields per laser pulse of corresponding species, was higher than 300. [ABSTRACT FROM AUTHOR]

Development of composite polymer/graphene oxide (GO) materials attracts significant attention due to their unique properties. In this work, highly ordered arrays of hollow microchambers made of composite polyelectrolyte/GO multilayers (PEGOMs) are successfully fabricated via layer‐by‐layer assembly on sacrificial or sustainable templates having imprinted patterns of microwells on their surface. Mechanical and optical properties of PEGOMs are studied by nanoindentation and near‐infrared (NIR) absorption spectroscopy. Incorporation of three GO layers in between the polyelectrolyte multilayer stacks increases Young's modulus and critical stress of the microchambers by a factor of 5.6 and 2.6, respectively. Optical density of this PEGOM film is found to decrease gradually from 0.14 at λ = 800 nm to 0.06 at λ = 1500 nm. Remote opening of PEGOM microchambers with NIR laser beam is also demonstrated. One of the possible applications of the developed structures includes micropackaging and delivery systems in biological tissues with remote triggering. Highly ordered arrays of hollow microchambers made of polyelectrolyte/GO multilayers (PEGOMs) withstand mechanical demolding, demonstrate enhanced Young's modulus and critical stress, and allow remote opening with NIR light. One of the possible applications of the developed PEGOM microchambers includes micropackaging and delivery systems in biological tissues with remote triggering. [ABSTRACT FROM AUTHOR]

We investigate the photoexcited state dynamics in a donor–acceptor copolymer, poly{3,6-dithiophene-2-yl-2,5-di(2-octyldodecyl)-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-naphthalene} (pDPP-TNT), by picosecond fluorescence and femtosecond transient absorption spectroscopies. Time-resolved fluorescence lifetime measurements of pDPP-TNT thin films reveal that the lifetime of the singlet excited state is 185 ± 5 ps and that singlet–singlet annihilation occurs at excitation photon densities above 6 × 1017 photons/cm3. From the results of singlet–singlet annihilation analysis, we estimate that the single-singlet annihilation rate constant is (6.0 ± 0.2) × 10−9 cm3 s−1 and the singlet diffusion length is ~7 nm. From the comparison of femtosecond transient absorption measurements and picosecond fluorescence measurements, it is found that the time profile of the photobleaching signal in the charge-transfer (CT) absorption band coincides with that of the fluorescence intensity and there is no indication of long-lived species, which clearly suggests that charged species, such as polaron pairs and triplet excitons, are not effectively photogenerated in the neat pDPP-TNT polymer. [ABSTRACT FROM AUTHOR]

Two-dimensional condensation was initiated in a self-assembled mixed monolayer of spiropyran and octadecanol by a nanosecond laser pulse. The dynamics of the process were monitored using nanosecond pump-probe Brewster angle microscopy. Domain growth followed a power law with a growth exponent of 0.47 at a velocity approaching 20 ms-1. This represents a limit for the rate of longitudinal signaling of pressure waves through a self-assembled amphiphilic layer at an interface and adds to our understanding of signal transmission rates in biomimetic membranes where morphological change in one region can be signaled to a more remote region. [ABSTRACT FROM AUTHOR]

The article discusses that long-standing problem of achieving Schrödinger's red demands sharp transitions from stopband to a high-reflectance passband with total suppression of higher-order resonances at blue/green wavelengths. It mentions about the proposed paradigm of the Schrödinger's color pixels.

To achieve sensitive biomolecular detection, a gold nanohole array sensing chip was designed by plasmonic simulation and fabricated by high fidelity nanoimprinting technology. The gold nanohole array on a glass substrate serves as an optical antenna array, to produce localized surface plasmon resonance (LSPR) of 10–100 times stronger than the illumination light for quantum dot (QD) excitation. In this work, a robust sandwich bioassay of primary aptamer/thrombin/secondary aptamer with QD655 was established on the chip, to detect thrombin at a limit of detection (LOD) of 1 ng/ml (27 pM), with low non-specific binding even at the presence of 1000 times more concentrated bovine serum albumin (BSA). The conformation and QD enhancement mechanism of the sandwich assay were characterized by atom force microscopy (AFM) and dual polarization interferometry (DPI). This is the first time that DNA is surface functionalized on gold nanostructures for protein detection by plasmon enhanced QD emission. Considering the low-cost, easy regeneration and long shelf-life of the capturing aptamer, low non-specific binding and high sensitivity of the bioassay, as well as the inexpensive mass fabrication of the high quality chips, this novel aptasensor platform is particularly useful for a point-of-care system on medical diagnostics. [ABSTRACT FROM AUTHOR]

Electron transfer dynamics in the oxide layers of the working electrodes in both dye-sensitized solar cells and photocatalysts greatly influences their performance. A proper understanding of the distribution of surface and bulk energy states on/in these oxide layers can provide insights into the associated electron transfer processes. Metal ions like Iron (Fe), Copper (Cu) and Tin (Sn) doped onto TiO 2 have shown enhanced photoactivity in these processes. In this work, the structural, optical and transient properties of Fe, Cu and Sn doped TiO 2 nanocrystalline powders have been investigated and compared using EDX, Raman spectroscopy, X-ray Photoelectron spectroscopy (XPS), and Transient Absorption spectroscopy (TAS). Surface free energy states distributions were probed using Electrochemical Impedance spectroscopy (EIS) on Dye Sensitized Solar Cells (DSSC) based on the doped TiO 2 photoanodes. Raman and XPS Ti2p 3/2 peak shifts and broadening showed that the concentration of defects were in the order: Cu doped TiO 2 > Fe doped TiO 2 > Sn doped TiO 2 > pure TiO 2 . Nanosecond laser flash photolysis of Fe and Cu doped TiO 2 indicated slower transient decay kinetics than that of Sn doped TiO 2 or pure TiO 2 . A broad absorption peak and fast transient decay at 430 nm for Fe doped TiO 2 was ascribed to an increase in surface hole concentration resulting in poor current density in the Fe doped TiO 2 photoanodes relative to pure TiO 2 , Sn or Cu doped anodes. The charge transfer capacitance and the calculated electron lifetimes correlated well with the trend in current density of the photoanodes (Sn > Cu > pure TiO 2 ). The poor performance of Fe doped cells is due to faster recombination of injected electrons with surface holes while those of Sn and Cu were more influenced by the concentration of their bulk defects. These results demonstrate that the choice of selected metal ions doping onto TiO 2 for a desired application should take into consideration the influence of bulk defect concentrations, the energy state distribution and the electron transfer properties in/on the oxide photoanodes. [ABSTRACT FROM AUTHOR]

Abstract: We investigate the role of oxygen vacancies in photochromism of molybdenum oxide amorphous films. MoO3−x films with a wide range of initial stoichiometries are deposited using R.F. unbalanced magnetron sputtering. The evolution of visible light absorption in conjunction with Raman spectra for these films is studied in detail during the course of UV-irradiation to correlate the color change to the Mo6+ to Mo5+ conversion. For films which have an initially more complete stoichiometry, and hence lower oxygen vacancy concentration, the color change fully correlates with conversion of Mo6+ to Mo5+. This behavior is consistent with the group of models of photochromism of transition metal oxides which disregard the presence of oxygen vacancies in the films. However, coloration of the films with initially greater deviation from complete stoichiometry, and hence higher oxygen vacancy concentration, is not accompanied by any significant conversion of Mo6+ to Mo5+. This behavior is consistent with the group of models of photochromism of transition metal oxides which rely on the presence of oxygen vacancies. Overall, the reported results demonstrate the importance of the initial stoichiometry in the photochromism of MoO3−x amorphous films, particularly in the initial stages of UV-irradiation. [Copyright &y& Elsevier]

Abstract: We report the effect of deposition conditions on the intrinsic color and photochromic properties of amorphous MoO3 thin films (a-films) deposited by R.F. unbalanced magnetron sputtering. Optical transmission spectroscopy was used to measure optical properties of the films. The conversion between Mo6+ and Mo5+ for as-deposited and UV irradiated films was characterized using XPS. Raman spectroscopy was used to confirm that the results of XPS were consistent with the bulk of the films. It is shown that absorption coefficient of as-deposited films increases with Mo5+ content. The temporal evolution of absorption coefficients for all films under UV light irradiation is measured using optical transmission spectroscopy. The largest change in absorption was observed for the film with the highest initial Mo5+ content. The temporal evolution of absorption coefficients for all the films shows initial fast rise within first minute of irradiation. XPS and Raman results show that for all films Mo5+ content increases as a result of UV irradiation except for the film with the highest initial Mo5+ content, for which the Mo5+ content decreases relative to Mo6+ despite the fact that the absorption of the film continues to rise. Further understanding of this mechanism is important since it will lead to enhanced photochromism and extend the photo-colorability of the films beyond the point at which the conversion of Mo6+ to Mo5+ is saturated. [Copyright &y& Elsevier]

While structural colors are ubiquitous in nature, saturated reds are mysteriously absent. This long-standing problem of achieving Schrödinger's red demands sharp transitions from "stopband" to a high-reflectance "passband" with total suppression of higher-order resonances at blue/green wavelengths. Current approaches based on nanoantennas are insufficient to satisfy all conditions simultaneously. Here, we designed Si nanoantennas to support two partially overlapping quasi-bound-states-in-the-continuum modes with a gradient descent algorithm to achieve sharp spectral edges at red wavelengths. Meanwhile, high-order modes at blue/green wavelengths are suppressed via engineering the substrate-induced diffraction channels and the absorption of amorphous Si. This design produces possibly the most saturated and brightest reds with ~80% reflectance, exceeding the red vertex in sRGB and even the cadmium red pigment. Its nature of being sensitive to polarization and illumination angle could be potentially used for information encryption, and this proposed paradigm could be generalized to other Schrödinger's color pixels.

Transient events in thin films and interfaces have been studied using the technique of time resolved pump-probe nanosecond Brewster angle microscopy. For p-polarized light there is a minimum reflectivity at the Brewster angle. When the interface is viewed with light that is both incident and reflected at the Brewster angle the resulting image is dark. Subsequent small changes is refractive index will then cause an increase in the reflectivity in affected regions providing high contrast images of an altered interface with a dark background level. This is the basis of Brewster angle microscopy. In the present work two synchronized nanosecond pulsed lasers were used in the pump-probe configuration in order to induce changes at an air-liquid interface and to monitor the resulting morphology changes over a range of time delays from nanosecond to milliseconds after laser-excitation. This method can be used to observe morphological changes in phase altering thin-films and molecular monolayers. Further it can be used to obtain information about transient photochemistry even in optically thin materials and nano-films. In the current work the method is used to monitor laser induced processes in phase separating binary liquid mixtures as well as in monolayers of photo-responsive amphiphilic molecules derived from spiropyran on water. The two systems are quite different but provide valuable comparisons.