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Recent advances in high-resolution biomedical imaging focusing on morphological, electrical, and biochemical properties of cells and tissues, scaling from cell clusters down to the molecular level, have improved cancer diagnosis. Multiscale imaging revealed high complexity that requires advanced data processing methods of multifractal analysis. We performed label-free multiscale imaging of surface potential variations in human ovarian and breast cancer cells using Kelvin probe force microscopy (KPFM). An improvement in the differentiation between normal and cancerous cells of for multifractal analysis using adaptive versus median threshold for image binarization was demonstrated. The results reveal the potential of using multifractality as a new biomarker for cancer diagnosis. Furthermore, the surface potential imaging can be used in combination with morphological imaging for cancer diagnosis., Comment: 35 pages, 11 figures

Understanding impacts of phase transition, phase coexistence, and surface magnetism on the longitudinal spin Seebeck effect (LSSE) in a magnetic system is essential to manipulate the spin to charge current conversion efficiency for spincaloritronic applications. We aim to elucidate these effects by performing a comprehensive study of the temperature dependence of LSSE in biphase iron oxide (BPIO = alpha-Fe2O3 + Fe3O4) thin films grown on Si (100) and Al2O3 (111) substrates. A combination of temperature-dependent anomalous Nernst effect (ANE) and electrical resistivity measurements show that the contribution of ANE from the BPIO layer is negligible compared to the intrinsic LSSE in the Si/BPIO/Pt heterostructure even at room temperature. Below the Verwey transition of the Fe3O4 phase, the total signal across BPIO/Pt is dominated by the LSSE. Noticeable changes in the intrinsic LSSE signal for both Si/BPIO/Pt and Al2O3/BPIO/Pt heterostructures around the Verwey transition of the Fe3O4 phase and the antiferromagnetic (AFM) Morin transition of the alpha-Fe2O3 phase are observed. The LSSE signal for Si/BPIO/Pt is found to be almost two times greater than that for Al2O3/BPIO/Pt, an opposite trend is observed for the saturation magnetization though. Magnetic force microscopy reveals the higher density of surface magnetic moments of the Si/BPIO film compared to the Al2O3/BPIO film, which underscores a dominant role of interfacial magnetism on the LSSE signal and thereby explains the larger LSSE for Si/BPIO/Pt., Comment: Accepted in ACS Applied Materials and Interfaces

The optical and electronic properties of 2D semiconductors are intrinsically linked via the strong interactions between optically excited bound species and free carriers. Here we use near-field scanning microwave microscopy (SMM) to image spatial variations in photoconductivity in MoS$_2$--WS$_2$ lateral multijunction heterostructures using photon energy-resolved narrowband illumination. We find that the onset of photoconductivity in individual domains corresponds to the optical absorption onset, confirming that the tightly bound excitons in transition metal dichalcogenides can nonetheless dissociate into free carriers. These photogenerated carriers are most likely n-type and are seen to persist for up to days, and informed by finite element modeling we reveal that they can increase the carrier density by up to 200 times. This persistent photoconductivity appears to be dominated by contributions from the multilayer MoS$_2$ domains, and we attribute the flake-wide response in part to charge transfer across the heterointerface. Spatial correlation of our SMM imaging with photoluminescence (PL) mapping confirms the strong link between PL peak emission photon energy, PL intensity, and the local accumulated charge. This work reveals the spatially and temporally complex optoelectronic response of these systems and cautions that properties measured during or after illumination may not reflect the true dark state of these materials but rather a metastable charged state., Comment: 27 pages, 5 figures

Two-dimensional (2D) materials and heterostructures have recently gained wide attention due to potential applications in optoelectronic devices. However, the optical properties of the heterojunction have not been properly characterized due to the limited spatial resolution, requiring nano-optical characterization beyond the diffraction limit. Here, we investigate the lateral monolayer MoS2-WS2 heterostructure using tip-enhanced photoluminescence (TEPL) spectroscopy on a non-metallic substrate with picoscale tip-sample distance control. By placing a plasmonic Au-coated Ag tip at the heterojunction, we observed more than three orders of magnitude photoluminescence (PL) enhancement due to the classical near-field mechanism and charge transfer across the junction. The picoscale precision of the distance-dependent TEPL measurements allowed for investigating the classical and quantum tunneling regimes above and below the ~320 pm tip-sample distance, respectively. Quantum plasmonic effects usually limit the maximum signal enhancement due to the near-field depletion at the tip. We demonstrate a more complex behavior at the 2D lateral heterojunction, where hot electron tunneling leads to the quenching of the PL of MoS2, while simultaneously increasing the PL of WS2. Our simulations show agreement with the experiments, revealing the range of parameters and enhancement factors corresponding to various regimes. The controllable photoresponse of the lateral junction can be used in novel nanodevices.

Lateral two-dimensional (2D) transitional metal dichalcogenide (TMD) heterostructures have recently attracted a wide attention as promising materials for optoelectronic nanodevices. Due to the nanoscale width of lateral heterojunctions, the study of their optical properties is challenging and requires using subwavelength optical characterization techniques. We investigated the photoresponse of a lateral 2D WSe2/MoSe2 heterostructure using tip-enhanced photoluminescence (TEPL) with nanoscale spatial resolution and with picoscale tip-sample distance dependence. We demonstrate the observation of quantum plasmonic effects in 2D heterostructures on a non-metallic substrate, and we report the nano-optical measurements of the lateral 2D TMD heterojunction width of ~ 150 nm and the charge tunneling distance of ~ 20 pm. Controlling the plasmonic tip location allows for both nano-optical imaging and plasmon-induced hot electron injection into the heterostructure. By adjusting the tip-sample distance, we demonstrated the controllability of the hot-electron injection via the competition of two quantum plasmonic photoluminescence (PL) enhancement and quenching mechanisms. The directional charge transport in the depletion region leads to the increased hot electron injection, enhancing the MoSe2 PL signal. The properties of the directional hot-electron injection in the quantum plasmonic regime make the lateral 2D MoSe2/WSe2 heterostructures promising for quantum nanodevices with tunable photoresponse.

Near-field optical microscopy can be used as a viable route to understand the nanoscale material properties below the diffraction limit. On the other hand, atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDs) are the materials of recent interest to study the spatial confinement of charge carriers, photon, and phonons. Heterostructures based on Mo or W based monolayer TMDs form type-II band alignment, and hence the optically excited carriers can be easily separated for applications pertaining to photonics and electronics. Mapping these spatially confined carriers or photons in a heterostructure with nanoscale resolution as well as their recombination behavior at the interfaces are necessary for the effective use of these materials in future high performance optoelectronics. We performed tip-enhanced photoluminescence (TEPL) imaging to increase the spatial resolution on multi-junction monolayer MoSe2-WSe2 lateral heterostructures grown by chemical vapor deposition (CVD) method. The near-field nano-PL emission map was used to distinguish the presence of distinct crystalline boundaries and the heterogeneities across the interfaces. This method significantly improves the nanoscale resolution of 2D materials, especially for understanding the PL emission properties at the vicinity of hetero-interfaces.

Two-dimensional monolayer transition metal dichalcogenides (TMDs) have unique optical and electronic properties for applications pertaining to field effect transistors, light emitting diodes, photodetectors, and solar cells. Vertical interfacing of WS2 and MoS2 layered materials in combination with other families of 2D materials were previously reported. On the other hand, lateral heterostructures are particularly promising for the spatial confinement of charged carriers, excitons and phonons within an atomically-thin layer. In the lateral geometry, the quality of the interface in terms of the crystallinity and optical properties is of paramount importance. Using plasmonic near-field tip-enhanced technology, we investigated the detailed nanoscale photoluminescence (nano-PL) characteristics of the hetero-interface in a monolayer WS2-MoS2 lateral heterostructure. Focusing the laser excitation spot at the apex of a plasmonic tip improved the PL spatial resolution by an order of magnitude compared to the conventional far-field PL. Nano-PL spatial line profiles were found to be more pronounced and enhanced at the interfaces. By analyzing the spectral signals of the heterojunctions, we obtained a better understanding of these direct band gap layered semiconductors, which may help to design next-generation smart optoelectronic devices.

Band gap tuning in two-dimensional transitional metal dichalcogenides (TMDs) is crucial in fabricating new optoelectronic devices. High resolution photoluminescence (PL) microscopy is needed for accurate band gap characterization. We performed tip-enhanced photoluminescence (TEPL) measurements of monolayer MoSe2 with nanoscale spatial resolution, providing an improved characterization of the band gap correlated with the topography compared with the conventional far field spectroscopy. We also observed PL shifts at the edges and investigated the spatial dependence of the TEPL enhancement factors., Comment: 8 pages, 3 figures. Figure 2 update

We report a study of long-range MoS2-substrate interaction using resonant Raman imaging. We observed a strong thickness-dependent peak shift of a Raman-forbidden mode that can be used as a new method of determining the thickness of multilayered MoS2 flakes. In addition, dependence of the Raman scattering intensity on thickness is explained by the interference enhancement theory. Finally, the resonant Raman spectra on different substrates are analysed.

Raman spectroscopy has been widely applied to the chemical analysis of food quality and, in particular, of chocolate. We perform Raman analysis of bloom formation in white and dark chocolates. We show evidence of sugar and fat bloom and investigate spectroscopic signatures of polymorphic changes in different phases.

Single molecule detection, sequencing and conformational mapping of aptamers are important for improving medical and biosensing technologies and for better understanding of biological processes at the molecular level. We obtain vibrational signals of single aptamers immobilized on gold substrates using tip-enhanced Raman spectroscopy (TERS). We compare topographic and optical signals and investigate the fluctuations of the position-dependent TERS spectra. TERS mapping provides information about the chemical composition and conformation of aptamers, and paves the way to future single-molecule label-free sequencing.

Two-dimensional (2D) materials beyond graphene such as transition metal dichalcogenides (TMDs) have unique mechanical, optical and electronic properties with promising applications in flexible devices, catalysis and sensing. Optical imaging of TMDs using photoluminescence and Raman spectroscopy can reveal the effects of structure, strain, doping, defects, edge states, grain boundaries and surface functionalization. However, Raman signals are inherently weak and so far have been limited in spatial resolution in TMDs to a few hundred nanometres which is much larger than the intrinsic scale of these effects. Here we overcome the diffraction limit by using resonant tip-enhanced Raman scattering (TERS) of few-layer MoS2, and obtain nanoscale optical images with ~ 20 nm spatial resolution. This becomes possible due to electric field enhancement in an optimized subnanometre-gap resonant tip-substrate configuration. We investigate the limits of signal enhancement by varying the tip-sample gap with sub-Angstrom precision and observe a quantum quenching behavior, as well as a Schottky-Ohmic transition, for subnanometre gaps, which enable surface mapping based on this new contrast mechanism. This quantum regime of plasmonic gap-mode enhancement with a few nanometre thick MoS2 junction may be used for designing new quantum optoelectronic devices and sensors.

Amplified ultrashort laser pulses are useful in many fields of science and engineering. Pushing the frontiers of ultrashort pulse generation will lead to new applications in biomedical imaging, communications and sensing. We propose a new, quantum approach to ultrashort pulse generation using transient quantum coherence which predicts order of magnitude stronger pulses generated with lower input energy than in the steady-state regime, reducing the practical heating limitations. This femtosecond quantum-coherent analog of nanosecond Q-switching is not limited by the pulse duration constraints of the latter, and, in principle, may be used for a variety of lasers including x-ray and plasmon nanolasers. We apply this approach to generation of giant plasmon pulses and achieve quantum control of plasmon relaxation dynamics by varying the drive pulse delay, amplitude and duration. We provide insights into the control mechanisms, and discuss future implementations and applications of this new source of ultrashort nanooptical fields.

Spasers have been theoretically predicted and experimentally observed and promise to deliver new exciting nanophotonic and biomedical applications. Here we theoretically investigate ultrafast dynamical properties of spasers with external plasmonic feedback. We consider a spaser both as a nanoscale source and detector of plasmons which could be used to design novel nano-imaging and sensing techniques. We show that, as with conventional lasers, spasers are sensitive to external feedback. However, unlike the lasers, spasers have faster relaxation dynamics which could be used to develop new ultrasensitive near field imaging techniques. We investigate the dependence of spaser relaxation oscillations on feedback parameters and show that quantum coherence can be used to increase the sensitivity to feedback.

We theoretically investigate exciton relaxation dynamics in molecular aggregates based on model photosynthetic complexes under various conditions of incoherent excitation. We show that noise-induced quantum coherence is generated between spatially-separated exciton states which belong to the same or different energy transfer pathways, coupled via real and virtual transfer processes. Such quantum coherence effects may be used to improve light-harvesting efficiency and to reveal quantum phenomena in biology., Comment: needs major revision

We performed food residue analysis of cook-stones from experimental and prehistoric earth ovens using a handheld Raman spectrometry. Progress in modern optical technology provides a facile means of rapid non-destructive identification of residue artifacts from archaeological sites. For this study spectral signatures were obtained on sotol (Dasylirion spp.) experimentally baked in an earth oven as well as sotol residue on an experimentally used processing tool. Inulin was the major residue component. The portable handheld Raman spectrometer also detected traces of inulin on boiling stones used to boil commercially obtained inulin. The Raman spectra of inulin and sotol may be useful as signatures of wild plant residues in archaeology. Spectroscopic analysis of millennia-old cook-stones from prehistoric archaeological sites in Fort Hood, TX revealed the presence of residues whose further identification requires improvement of current optical methods., Comment: 18 pages, 5 figures, 1 table

Coherent anti-Stokes Raman scattering (CARS) and, in particular, femtosecond adaptive spectroscopic techniques (FAST CARS) have been successfully used for molecular spectroscopy and microscopic imaging. Recent progress in ultrafast nanooptics provides flexibility in generation and control of optical near fields, and holds promise to extend CARS techniques to the nanoscale. In this theoretical study, we demonstrate ultrafast subwavelentgh control of coherent Raman spectra of molecules in the vicinity of a plasmonic nanostructure excited by ultrashort laser pulses. The simulated nanostructure design provides localized excitation sources for CARS by focusing incident laser pulses into subwavelength hot spots via two self-similar nanolens antennas connected by a waveguide. Hot-spot-selective dual-tip-enhanced CARS (2TECARS) nanospectra of DNA nucleobases are obtained by simulating optimized pump, Stokes and probe near fields using tips, laser polarization- and pulse-shaping. This technique may be used to explore ultrafast energy and electron transfer dynamics in real space with nanometre resolution and to develop novel approaches to DNA sequencing., Comment: 11 pages, 6 figures

We investigate surface plasmon amplification in a silver nanoparticle coupled to an externally driven three-level gain medium, and show that quantum coherence significantly enhances the generation of surface plasmons. Surface plasmon amplification by stimulated emission of radiation is achieved in the absence of population inversion on the spasing transition, which reduces the pump requirements. The coherent drive allows us to control the dynamics, and holds promise for quantum control of nanoplasmonic devices., Comment: 5 pages, 4 figures