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Ashish Arora

Publications and source records attributed to Ashish Arora.

At least 19 recordsLinked to original sources

Extreme Polarization of the Optical Gap and High-Energy Exciton Landscape in CrSBr

We reveal a strongly anisotropic excitonic landscape in monolayer and bulk-like CrSBr using optical absorption spectroscopy and $GW$-Bethe-Salpeter equation $\textit{ab initio}$ calculations. The direct absorptive determination of the lowest bright optical onsets i.e. $X_0^a$ and $X_0^b$ excitons for the two in-plane polarization eigenaxes yield an in-plane optical gap anisotropy of $470 \pm 15$ meV. This is the highest observed value for any material in the near-infrared-to-visible spectral region to the best of our knowledge. Energetically above, we identify multiple strongly polarized excitons spanning $1.25$ eV to $3.1$ eV selectively aligned along the two orthogonal axes. A resonance $X^-$, located $24$ meV below the $X_0^b$ progressively transfers oscillator strength to $X_b^0$, a behavior consistent with a coupled trion (Fermi-polarion)/exciton pair. Our experiments also provide polarization-resolved broadband dielectric functions of CrSBr. These results establish CrSBr as a strongly polarization-selective excitonic system and highlight its potential for polarization-selective optoelectronics enabled with its large optical-gap anisotropy.

cond-mat.mes-hall

Phonon-modulated Kerr nonlinearity in ultrathin 2H-MoTe2

Controlling nonequilibrium responses in optically driven quantum materials is essential for advancing applications in energy conversion, ultrafast electronics, and quantum computation. Nonlinear optical spectroscopy serves as a powerful tool to investigate ultrafast electron and phonon dynamics in these systems; however, conventional nonlinear approaches often require intense laser pulses (> 10 GW/cm2) and typically encounter a strong background. Here, we introduce a phase-sensitive nonlinear spectroscopic technique that operates at low laser powers (~ 10 kW/cm2, pulse energies ~ 10 pJ) and enables real-time monitoring and active control of coherent phonons in a few-layer (three to five) thick 2H-MoTe2. Upon excitation with ultrashort (~ 10 fs) pump pulses, we achieve displacive excitation of coherent phonons, which periodically modulate the Kerr nonlinearity of the material, leading to cross-phase modulation (XPM) of a delayed probe pulse. This phase modulation induces spectral broadening and oscillations in the center of mass (COM) of the probe spectrum in time, enabling the detection of subtle nonlinear optical responses in a background-free manner. The nonlinear response can be selectively amplified or attenuated by adjusting the strength of the pump pulse, which controls the distribution of photoexcited carriers in the electronic bands. By combining two-color nondegenerate pump-probe measurements and time-dependent density-functional theory (TDDFT) calculations, we directly resolve the coupled nonequilibrium electronic and phonon dynamics. A dual-pump pulse scheme enables precise control of phonon oscillations, allowing selective activation or suppression of specific phonon modes and correspondingly the modulation of the Kerr nonlinearity.

physics.optics

Exciton-Selective Phonon Coupling in a Lead Halide Perovskite

Exciton-phonon interactions govern the optical response of semiconductors, yet disentangling multiple coupling channels in lead halide perovskites remains challenging. We investigate CsPbBr3 microcrystals using photoluminescence, Raman and reflectance spectroscopy at low temperature, revealing the simultaneous presence of high-energy and Rashba excitons, each accompanied by distinct phonon replica series. High-energy exciton replicas are uniquely spaced by approximately 9 meV, whereas Rashba exciton replicas exhibit a characteristic approximately 6 meV spacing, indicating the specificity of the exciton-phonon coupling. Unsupervised machine learning applied to a large low-temperature photoluminescence dataset reveals these replica features are prevalent. With increasing temperature, replica features broaden and merge, evolving into a dominant longitudinal optical phonon coupling regime at room temperature. This work establishes direct spectroscopic evidence for concurrent, exciton-specific phonon coupling within a single material, offering new pathways to engineer light-matter interactions for optoelectronic and phonon-photon-based quantum device applications.

cond-mat.mes-hall

Universal Thickness-Dependent Absorption in Solids at the Nanoscale: Anomalous Enhancement in the Ultrathin Limit

Through systematic experimental and theoretical studies of layer-thickness-dependent absorption in semiconducting MoSe$_2$ and WS$_2$ across the visible to near-infrared spectral range, we demonstrate a universal absorption behavior in solids at nanoscale thicknesses. With increasing thickness, a non-monotonic evolution of absorption integrated over the measured spectral region is revealed which is accompanied by pronounced oscillatory features. This shows a strong deviation from the expected Beer-Lambert law. Below 10 nm, we observe a sharp anomalous increase in absorption, with deviations from Beer's law exceeding 50% in layered semiconductors. Our conclusions hold irrespective of the presence of any optical resonances such as excitons or plasmons within the spectral window. The observed behavior has origins in the electromagnetic interference effects taking place between the two surfaces of the thin crystals. The present work on 2D semiconductors is extendable to all kinds of solids such as conventional semiconductors (e.g. Si, GaAs, GaN, InP), (semi) metals (e.g. Al, Ag, Au, c-HOPG) and 2D magnetic materials (e.g. CrSBr and NiPS$_3$). Our results provide fundamental insights into light-matter interactions in solids at the nanoscale and are vital for optimally designing the new generation of absorption-based flexible optoelectronic devices.

cond-mat.mes-hall

Excited-State Trions in a Quantum Well

We report on the observation of an excited 2s state of a trion in a 4.2 nm wide doped GaAs/Al(0.3)Ga(0.7)As quantum well (QW) using magneto-optical Kerr effect (MOKE) spectroscopy under out-of-plane magnetic fields up to 6 T. This resonance appears slightly below the 2s exciton in energy. Strikingly, the 2s trion is found to be bound only for magnetic fields larger than 1 T. The signature of the 2s trion is absent in the magneto-reflectance spectra, while it is detectable in the MOKE spectra signifying the importance of the powerful technique. Similar to the 1s states, the 2s trion shows an opposite degree of magnetic-field-induced polarization compared to its exciton counterpart, in agreement with our theoretical calculations. This transfer of oscillator strength between the complexes establishes an optical fingerprint of the 2s excited trion.

cond-mat.mes-hall

Engineering 2D material exciton lineshape with graphene/h-BN encapsulation

Control over the optical properties of atomically thin two-dimensional (2D) layers, including those of transition metal dichalcogenides (TMDs), is needed for future optoelectronic applications. Remarkable advances have been achieved through alloying, chemical and electrical doping, and applied strain. However, the integration of TMDs with other 2D materials in van der Waals heterostructures (vdWHs) to tailor novel functionalities remains largely unexplored. Here, the near-field coupling between TMDs and graphene/graphite is used to engineer the exciton lineshape and charge state. Fano-like asymmetric spectral features are produced in WS$_{2}$, MoSe$_{2}$ and WSe$_{2}$ vdWHs combined with graphene, graphite, or jointly with hexagonal boron nitride (h-BN) as supporting or encapsulating layers. Furthermore, trion emission is suppressed in h-BN encapsulated WSe$_{2}$/graphene with a neutral exciton redshift (44 meV) and binding energy reduction (30 meV). The response of these systems to electron-beam and light probes is well-described in terms of 2D optical conductivities of the involved materials. Beyond fundamental insights into the interaction of TMD excitons with structured environments, this study opens an unexplored avenue toward shaping the spectral profile of narrow optical modes for application in nanophotonic devices.

cond-mat.mes-hall

Excitonic Absorption Signatures of Twisted Bilayer WSe$_{2}$ by Electron Energy-Loss Spectroscopy

Moir\'{e} twist angle underpins the interlayer interaction of excitons in twisted van der Waals hetero- and homo-structures. The influence of twist angle on the excitonic absorption of twisted bilayer tungsten diselenide (WSe$_{2}$) has been investigated using electron energy-loss spectroscopy. Atomic-resolution imaging by scanning transmission electron microscopy was used to determine key structural parameters, including the nanoscale measurement of the relative twist angle and stacking order. Detailed spectral analysis revealed a pronounced blueshift in the high-energy excitonic peak C with increasing twist angle, up to 200 meV when compared to the AA$^{\prime}$ stacking. The experimental findings have been discussed relative to first-principle calculations of the dielectric response of the AA$^{\prime}$ stacked bilayer WSe$_{2}$ as compared to monolayer WSe$_{2}$ by employing the \textit{GW} plus Bethe-Salpeter equation (BSE) approaches, resolving the origin of higher energy spectral features from ensembles of excitonic transitions, and thus any discrepancies between previous calculations. Furthermore, the electronic structure of moir\'{e} supercells spanning twist angles of $\sim$9.5-46.5$^{\circ}$ calculated by density functional theory (DFT) were unfolded, showing an uplifting of the conduction band minimum near the $Q$ point and minimal change in the upper valence band concurrently. The combined experiment/theory investigation provides valuable insight into the physical origins of high-energy absorption resonances in twisted bilayers, which enables to track the evolution of interlayer coupling from tuning of the exciton C transitions by absorption spectroscopy.

cond-mat.mes-hall

High-performance broadband Faraday rotation spectroscopy of 2D materials and thin magnetic films

We present a Faraday rotation spectroscopy (FRS) technique for measurements on the micron scale. Spectral acquisition speeds of many orders of magnitude faster than state-of-the-art modulation spectroscopy setups are demonstrated. The experimental method is based on charge-coupled-device detection, avoiding speed-limiting components, such as polarization modulators with lock-in amplifiers. At the same time, FRS spectra are obtained with a sensitivity of 20 $\mu$rad (0.001$^\circ$) over a broad spectral range (525 nm - 800 nm), which is on par with state-of-the-art polarization-modulation techniques. The new measurement technique also automatically cancels unwanted Faraday rotation backgrounds. Using the setup, we perform Faraday rotation spectroscopy of excitons in a hBN-encapsulated atomically thin semiconductor WS$_2$ under magnetic fields of up to 1.4 T at room temperature and liquid helium temperature. We determine the A exciton g-factor of -4.4 $\pm$ 0.3 at room temperature, and -4.2 $\pm$ 0.2 at liquid helium temperature. In addition, we perform FRS and hysteresis loop measurements on a 20 nm thick film of an amorphous magnetic Tb$_{0.2}$Fe$_{0.8}$ alloy.

cond-mat.mes-hall

Substrate influence on transition metal dichalcogenide monolayer exciton absorption linewidth broadening

The excitonic states of transition metal dichacolgenide (TMD) monolayers are heavily influenced by their external dielectric environment based on the substrate used. In this work, various wide bandgap dielectric materials, namely hexagonal boron nitride (\textit{h}-BN) and amorphous silicon nitride (Si$_3$N$_4$), under different configurations as support or encapsulation material for WS$_2$ monolayers are investigated to disentangle the factors contributing to inhomogeneous broadening of exciton absorption lines in TMDs using electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM). In addition, monolayer roughness in each configuration was determined from tilt series of electron diffraction patterns by assessing the broadening of diffraction spots by comparison with simulations. From our experiments, the main factors that play a role in linewidth broadening can be classified in increasing order of importance by: monolayer roughness, surface cleanliness, and substrate-induced charge trapping. Furthermore, because high-energy electrons are used as a probe, electron beam-induced damage on bare TMD monolayer is also revealed to be responsible for irreversible linewidth increases. \textit{h}-BN not only provides clean surfaces of TMD monolayer, and minimal charge disorder, but can also protect the TMD from irradiation damage. This work provides a better understanding of the mechanisms by which \textit{h}-BN remains, to date, the most compatible material for 2D material encapsulation, facilitating the realization of intrinsic material properties to their full potential.

cond-mat.mes-hall

Magnetooptics of layered two-dimensional semiconductors and heterostructures: progress and prospects

Beginning with the 'conventional' two-dimensional (2D) quantum wells (QWs) based on III-V and II-VI semiconductors in the 1970s, to the recent atomically-thin sheets of van der Waals materials such as 2D semiconducting transition metal dichalcogenides (TMDCs) and 2D magnets, the research in 2D materials is continuously evolving and providing new challenges. Magnetooptical spectroscopy has played a significant role in this area of research, both from fundamental physics and technological perspectives. A major challenge in 2D semiconductors such as TMDCs is to understand their spin-valley-resolved physics, and their implications in quantum computation and information research. Since the discovery of valley Zeeman effects, deep insights into the spin-valley physics of TMDCs and their heterostructures has emerged through magnetooptical spectroscopy. In this perspective, we highlight the role of magnetooptics in many milestones such as the discovery of interlayer excitons, phase control between coherently-excited valleys, determination of exciton-reduced masses, Bohr radii and binding energies, physics of the optically-bright and dark excitons, trions, other many-body species such as biexcitons and their phonon replicas in TMDC monolayers. The discussion accompanies open questions, challenges and future prospects in the field including comments on the magnetooptics of van der Waals heterostructures involving TMDCs and 2D magnets.

cond-mat.mes-hall

Efficient MDI Adaptation for n-gram Language Models

This paper presents an efficient algorithm for n-gram language model adaptation under the minimum discrimination information (MDI) principle, where an out-of-domain language model is adapted to satisfy the constraints of marginal probabilities of the in-domain data. The challenge for MDI language model adaptation is its computational complexity. By taking advantage of the backoff structure of n-gram model and the idea of hierarchical training method, originally proposed for maximum entropy (ME) language models, we show that MDI adaptation can be computed in linear-time complexity to the inputs in each iteration. The complexity remains the same as ME models, although MDI is more general than ME. This makes MDI adaptation practical for large corpus and vocabulary. Experimental results confirm the scalability of our algorithm on very large datasets, while MDI adaptation gets slightly worse perplexity but better word error rate results compared to simple linear interpolation.

cs.CL

Dark trions govern the temperature-dependent optical absorption and emission of doped atomically thin semiconductors

We perform absorption and photoluminescence spectroscopy of trions in hBN-encapsulated WSe$_2$, WS$_2$, MoSe$_2$, and MoS$_2$ monolayers, depending on temperature. The different trends for W- and Mo-based materials are excellently reproduced considering a Fermi-Dirac distribution of bright and dark trions. We find a dark trion, $\rm{X_D^-}$ 19 meV $\textit{below}$ the lowest bright trion, $\rm{X}_1^-$ in WSe$_2$ and WS$_2$. In MoSe$_2$, $\rm{X_D^-}$ lies 6 meV $\textit{above}$ $\rm{X}_1^-$, while $\rm{X_D^-}$ and $\rm{X}_1^-$ almost coincide in MoS$_2$. Our results agree with GW-BSE $\textit{ab-initio}$ calculations and quantitatively explain the optical response of doped monolayers with temperature.

cond-mat.mes-hall

The JHU Multi-Microphone Multi-Speaker ASR System for the CHiME-6 Challenge

This paper summarizes the JHU team's efforts in tracks 1 and 2 of the CHiME-6 challenge for distant multi-microphone conversational speech diarization and recognition in everyday home environments. We explore multi-array processing techniques at each stage of the pipeline, such as multi-array guided source separation (GSS) for enhancement and acoustic model training data, posterior fusion for speech activity detection, PLDA score fusion for diarization, and lattice combination for automatic speech recognition (ASR). We also report results with different acoustic model architectures, and integrate other techniques such as online multi-channel weighted prediction error (WPE) dereverberation and variational Bayes-hidden Markov model (VB-HMM) based overlap assignment to deal with reverberation and overlapping speakers, respectively. As a result of these efforts, our ASR systems achieve a word error rate of 40.5% and 67.5% on tracks 1 and 2, respectively, on the evaluation set. This is an improvement of 10.8% and 10.4% absolute, over the challenge baselines for the respective tracks.

eess.AS

CHiME-6 Challenge:Tackling Multispeaker Speech Recognition for Unsegmented Recordings

Following the success of the 1st, 2nd, 3rd, 4th and 5th CHiME challenges we organize the 6th CHiME Speech Separation and Recognition Challenge (CHiME-6). The new challenge revisits the previous CHiME-5 challenge and further considers the problem of distant multi-microphone conversational speech diarization and recognition in everyday home environments. Speech material is the same as the previous CHiME-5 recordings except for accurate array synchronization. The material was elicited using a dinner party scenario with efforts taken to capture data that is representative of natural conversational speech. This paper provides a baseline description of the CHiME-6 challenge for both segmented multispeaker speech recognition (Track 1) and unsegmented multispeaker speech recognition (Track 2). Of note, Track 2 is the first challenge activity in the community to tackle an unsegmented multispeaker speech recognition scenario with a complete set of reproducible open source baselines providing speech enhancement, speaker diarization, and speech recognition modules.

cs.SD

FDFNet : A Secure Cancelable Deep Finger Dorsal Template Generation Network Secured via. Bio-Hashing

Present world has already been consistently exploring the fine edges of online and digital world by imposing multiple challenging problems/scenarios. Similar to physical world, personal identity management is very crucial in-order to provide any secure online system. Last decade has seen a lot of work in this area using biometrics such as face, fingerprint, iris etc. Still there exist several vulnerabilities and one should have to address the problem of compromised biometrics much more seriously, since they cannot be modified easily once compromised. In this work, we have proposed a secure cancelable finger dorsal template generation network (learning domain specific features) secured via. Bio-Hashing. Proposed system effectively protects the original finger dorsal images by withdrawing compromised template and reassigning the new one. A novel Finger-Dorsal Feature Extraction Net (FDFNet) has been proposed for extracting the discriminative features. This network is exclusively trained on trait specific features without using any kind of pre-trained architecture. Later Bio-Hashing, a technique based on assigning a tokenized random number to each user, has been used to hash the features extracted from FDFNet. To test the performance of the proposed architecture, we have tested it over two benchmark public finger knuckle datasets: PolyU FKP and PolyU Contactless FKI. The experimental results shows the effectiveness of the proposed system in terms of security and accuracy.

cs.CV

Zeeman spectroscopy of excitons and hybridization of electronic states in few-layer WSe$_2$, MoSe$_2$ and MoTe$_2$

Monolayers and multilayers of semiconducting transition metal dichalcogenides (TMDCs) offer an ideal platform to explore valley-selective physics with promising applications in valleytronics and information processing. Here we manipulate the energetic degeneracy of the $\mathrm{K}^+$ and $\mathrm{K}^-$ valleys in few-layer TMDCs. We perform high-field magneto-reflectance spectroscopy on WSe$_2$, MoSe$_2$, and MoTe$_2$ crystals of thickness from monolayer to the bulk limit under magnetic fields up to 30 T applied perpendicular to the sample plane. Because of a strong spin-layer locking, the ground state A excitons exhibit a monolayer-like valley Zeeman splitting with a negative $g$-factor, whose magnitude increases monotonically when thinning the crystal down from bulk to a monolayer. Using the $\mathbf{k\cdot p}$ calculation, we demonstrate that the observed evolution of $g$-factors for different materials is well accounted for by hybridization of electronic states in the $\mathrm{K}^+$ and $\mathrm{K}^-$ valleys. The mixing of the valence and conduction band states induced by the interlayer interaction decreases the $g$-factor magnitude with an increasing layer number. The effect is the largest for MoTe$_2$, followed by MoSe$_2$, and smallest for WSe$_2$. Keywords: MoSe$_2$, WSe$_2$, MoTe$_2$, valley Zeeman splitting, transition metal dichalcogenides, excitons, magneto optics.

cond-mat.mes-hall

Phonon Sidebands in Transition Metal Dichalcogenides

Excitons dominate the optical properties of monolayer transition metal dichalcogenides (TMDs). Besides optically accessible bright exciton states, TMDs exhibit also a multitude of optically forbidden dark excitons. Here, we show that efficient exciton-phonon scattering couples bright and dark states and gives rise to an asymmetric excitonic line shape. The observed asymmetry can be traced back to phonon-induced sidebands that are accompanied by a polaron redshift. We present a joint theory-experiment study investigating the microscopic origin of these sidebands in different TMD materials taking into account intra- and intervalley scattering channels opened by optical and acoustic phonons. The gained insights contribute to a better understanding of the optical fingerprint of these technologically promising nanomaterials.

cond-mat.mes-hall

Sparse Coding and Autoencoders

In "Dictionary Learning" one tries to recover incoherent matrices $A^* \in \mathbb{R}^{n \times h}$ (typically overcomplete and whose columns are assumed to be normalized) and sparse vectors $x^* \in \mathbb{R}^h$ with a small support of size $h^p$ for some $0 <p < 1$ while having access to observations $y \in \mathbb{R}^n$ where $y = A^*x^*$. In this work we undertake a rigorous analysis of whether gradient descent on the squared loss of an autoencoder can solve the dictionary learning problem. The "Autoencoder" architecture we consider is a $\mathbb{R}^n \rightarrow \mathbb{R}^n$ mapping with a single ReLU activation layer of size $h$. Under very mild distributional assumptions on $x^*$, we prove that the norm of the expected gradient of the standard squared loss function is asymptotically (in sparse code dimension) negligible for all points in a small neighborhood of $A^*$. This is supported with experimental evidence using synthetic data. We also conduct experiments to suggest that $A^*$ is a local minimum. Along the way we prove that a layer of ReLU gates can be set up to automatically recover the support of the sparse codes. This property holds independent of the loss function. We believe that it could be of independent interest.

cs.LG