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Enam Chowdhury

Publications and source records attributed to Enam Chowdhury.

15 recordsLinked to original sources

Nonlinear Photocurrent Spectroscopy and Polarization-Tunable Shift Current in the Layered Semiconductor $\mathrm{CuScP_2S_6}$

The class of layered metal thiophosphates and selenophosphates are emerging as promising candidates for non-linear photonic and optoelectronic applications. Here we report one-photon absorption (1PA) and two-photon absorption (2PA) induced photocurrents in $CuScP_2S_6$, establishing it as an optoelectronically-active non-centrosymmetric semiconductor. Spectrally-resolved 1PA and 2PA photoresponsivity paired with photoluminescence and differential reflectance measurements reveal a band gap of 2.35 eV, several higher energy interband transitions, and sub-band gap multiphoton excitonic transitions. Vertical graphite/$CuScP_2S_6$/graphite devices exhibit zero-bias photocurrent with a polarity controlled by both photon energy and optical polarization orientation within the ab-plane. This sign-dependence combined with a characteristic power-law transition from linear to square-root scaling are consistent with a shift-current origin to this bulk photovoltaic effect (BPVE). These findings establish $CuScP_2S_6$ as a multi-functional platform for polarization-sensitive non-linear optoelectronics.

cond-mat.mtrl-sci

From pore collapse to crystal growth: ultrafast laser-induced stishovite formation in nanoporous silica

The crystallization of amorphous solids under ultrafast laser irradiation represents a paradigm of non-equilibrium phase transitions, where the interplay between electromagnetic energy localization and atomic-scale dynamics remains largely uncharted. By using a multiscale framework that couples finite-difference time-domain simulations of nonlinear femtosecond laser pulse propagation with molecular dynamics of the atomic response, we demonstrate that field enhancement around the pores of nanoporous amorphous silica confines laser energy and drives rapid pore collapse. In nanoporous silica, the enhanced local electromagnetic field leads to stronger energy absorption compared with smaller-pore and homogeneous systems. This heterogeneous energy localization provides preferential nucleation sites within the dense glass network, leading to ultrafast formation of stishovite on a sub-nanosecond timescale, faster than in homogeneous silica. This accelerated crystallization can outpace pressure relaxation making the transition to a high-pressure phase possible. These results are confirmed by experimental observations of femtosecond-laser-induced crystallization in confined geometries, and show that electromagnetic hotspots in nanoporous glass structures can be tailored to control solid-state transformations.

cond-mat.mtrl-sci

Pulse-Duration Scaling of Ultrafast Laser-Induced Damage Threshold in Hybrid Gratings

High damage threshold gratings are in demand worldwide as critical components for next generation ultrahigh intensity lasers. Here we investigate the pulse-duration dependence of ultrafast laser-induced damage thresholds (LIDT) in hybrid multilayer dielectric gratings, touted to combine superior performance properties of both metallic and multilayer dielectric (MLD) gratings, using a dynamic finite-difference time-domain model incorporated with linear and non-linear absorption models. Simulations agree with reported experimental LIDT values for three representative designs and predict scaling exponents which vary with pulse durations ranging from 10 to 500 fs. The results reveal strong dependence on both material bandgap and grating field distribution, providing guidance for designing high LIDT gratings.

physics.optics

Cryogenically Enhanced Laser-Induced Amorphous Phase Transitions in Crystalline Silicon

Amorphization of silicon is crucial to applications in photonics, microelectronics and solar cell technologies. Ultrafast lasers have been used to generate amorphous silicon from crystalline silicon using rapid nonthermal melting and solidification in room temperature. As material temperature can affect cooling rates significantly, adding temperature control in ultrafast laser modification of silicon may allow a new degree of freedom in ultrafast laser modification. In this work, we investigate the role of cryogenic temperature in governing ultrafast damage pathways via single-shot femtosecond laser irradiation of silicon from room temperature down to 24K at 1030nm. Across this temperature range, we observe a pronounced enhancement of amorphization at lower temperatures, revealed through optical microscopy, Raman spectroscopy, and Kelvin probe force microscopy (KPFM). Raman analysis identifies this ring as an amorphous surface layer, while complementary AFM and SEM imaging show temperature-dependent changes in surface morphology, including localized melt redistribution and refrozen material. To elucidate the physical origins of this behavior, we implement a carrier dependent two-temperature model (nTTM). The simulations reproduce the experimentally observed trends and indicate that reduced phonon population, modified absorption pathways, and altered lattice relaxation dynamics at cryogenic temperatures collectively promote amorphous freezing over recrystallization. This study represents the first detailed examination of silicon under ultrafast irradiation below the liquid-nitrogen regime and reveals temperature-governed mechanisms relevant for advanced silicon microstructuring.

cond-mat.mtrl-sci

Highly Efficient Second/Third Harmonic Generation in van der Waals Layered Material AgScP2S6 with Anisotropic Polarization and Temperature Dependence

Single-crystal X-ray diffraction and nonlinear optical measurements, especially second- and third-harmonic generation (SHG/THG) are comprehensively investigated for the van der Waals layered material AgScP2S6 with a non-centrosymmetric P31c (159) space group. Linear optical constants are extracted using spectroscopic ellipsometry and applied in fitting the harmonic generation behavior. Polarization-resolved SHG and THG measurements exhibit pronounced anisotropy, with emission patterns well-described by theoretical models derived from the khi(2) and khi(3) tensor elements. The material demonstrates exceptionally high nonlinear susceptibilities, with khi(2) ~ 10^(-8) m/V and khi(3) ~ 10^(-17) m^2/V^2 which is a few orders of magnitude greater than comparable 2D materials reported in the literature. Temperature-dependent SHG and THG measurements from 300 K to 25 K reveal exponential decay in harmonic signal intensities, attributed to reduced carrier mobility, with no evidence of structural phase transitions, consistent with results from single crystal diffraction and heat capacity measurements. Polarization-resolved SHG and THG measurements also reveal distinct orientation and ellipticity trends, highlighting the anisotropic nonlinear tensor contributions and contrasting polarization selection rules in the material. These results establish AgScP2S6 as a high-performance, thermally stable, and highly anisotropic nonlinear candidate material suitable for compact photonic applications such as ultrafast optical modulators, polarization-sensitive detectors, and wavelength-tunable light sources.

cond-mat.mtrl-sci

Mimicking the earth core conditions with ultrafast laser materials interaction

Ultrafast lasers create extreme, non-equilibrium thermodynamic conditions that can transiently reach pressures and temperatures comparable to interior core of the earth. Here we show that femtosecond excitation of amorphous silica-hafnia multilayer dielectrics drives the formation of high-pressure crystalline phases of silica including stishovite, seifertite, and the pyrite-type high density structure, within confined subsurface regions.Using TEM, SAED, and 4D-STEM, we directly map nanoscale phase evolution and identify crystalline motifs embedded inside laser generated blisters.Complementary molecular dynamics simualtions reveal the thermodynamic pathway underlying these transformations, where rapid electronic pressure initiates densification and octahedral coordination, followed by temperature driven crystallization and displacive transitions during ultrafast quenching. The resulting polymorphs reflects a dual-stage pathway inaccessible under equilibrium processing. Our results establish femtosecond laser excitation as a viable route to synthesize and stabilize ultrahigh-density high pressure silica phases under ambient conditions, without a diamond anvil cell, with implications for laser-damage mechanisms, high-energy-density materials, and planetary physics.

cond-mat.mtrl-sci

Single shot multi-time frame imaging of plasmas with a frequency tagged GHz pulse train

Studying plasma dynamics is crucial for understanding processes like inertial confinement fusion, material damage, and shockwave formation from intense laser or current interactions. While pump-probe methods are standard for capturing these dynamics, single-shot experiments using high-power, low-repetition-rate systems with custom targets are challenging. We present a novel imaging technique using a synchronized GHz-rate spectrally tagged probe laser to capture multiple time-resolved snapshots from a single pump event.

physics.plasm-ph

Ferroelectric Epsilon-WO3 Nanoparticles and Its Bipolaron Driven Opto-electronic Properties at Room Temperature

A unique polymorph of binary tungsten trioxide, the epsilon phase of WO3, has non-centrosymmetric ferroelectric structure, typically stable below -43 degree C in bulk. We have stabilized the epsilon-WO3 at room temperature (RT) and nanostructured powders via flame spray pyrolysis synthesis. These nanopowders are drop cast into uniform thin films to enable RT measurement of ferroelectric and optoelectronic properties. We report ferroelectric hysteresis, nanoscale domains, and dipole switching measured via Piezo-response force microscopy (PFM). The epsilon-WO3 films also display optical second harmonic generation (SHG) and anticlockwise ferroelectric butterfly capacitance versus voltage hysteresis, further demonstrating the ferroelectric nature of epsilon-WO3. Remarkably, epsilon-WO3 shows ferroelectric polarization responses to optical stimuli and form bipolaron at RT, a spin-zero quasiparticle previously found only in cryogenic temperatures. The bipolaron formation and its interaction with electro-optical stimuli results in a single layer solid-state blue coloration, a ferrochromic effect. A mechanism of the ferrochromic effect is discussed. In summary, epsilon-WO3 appears to be a ferroelectric with the simplest structure, forming bosonic spin-zero bipolaron at RT, and it's dipoles respond to opto-electrical signals; therefore, this material holds significant promise for transforming the field of optoelectronics.

cond-mat.mtrl-sci

Continuous relativistic high-harmonic generation from a kHz liquid-sheet plasma mirror

We report on continuous high-harmonic generation at 1 kHz repetition rate from a liquid-sheet plasma mirror driven by relativistic-intensity near-single-cycle light transients. Through precise control of both the surface plasma density gradient and the driving light waveform, we can produce highly stable and reproducible extreme ultraviolet spectral quasi-continua, corresponding to the generation of stable kHz-trains of isolated attosecond pulses in the time domain. This confirms the exciting potential of liquid sheet targets as one of the building blocks of future high-power attosecond lasers.

physics.plasm-ph

High average power ultrafast laser technologies for driving future advanced accelerators

Large scale laser facilities are needed to advance the energy frontier in high energy physics and accelerator physics. Laser plasma accelerators are core to advanced accelerator concepts aimed at reaching TeV electron electron colliders. In these facilities, intense laser pulses drive plasmas and are used to accelerate electrons to high energies in remarkably short distances. A laser plasma accelerator could in principle reach high energies with an accelerating length that is 1000 times shorter than in conventional RF based accelerators. Notionally, laser driven particle beam energies could scale beyond state of the art conventional accelerators. LPAs have produced multi GeV electron beams in about 20 cm with relative energy spread of about 2 percent, supported by highly developed laser technology. This validates key elements of the US DOE strategy for such accelerators to enable future colliders but extending best results to date to a TeV collider will require lasers with higher average power. While the per pulse energies envisioned for laser driven colliders are achievable with current lasers, low laser repetition rates limit potential collider luminosity. Applications will require rates of kHz to tens of kHz at Joules of energy and high efficiency, and a collider would require about 100 such stages, a leap from current Hz class LPAs. This represents a challenging 1000 fold increase in laser repetition rates beyond current state of the art. This whitepaper describes current research and outlook for candidate laser systems as well as the accompanying broadband and high damage threshold optics needed for driving future advanced accelerators.

physics.acc-ph

Generation of even and odd high harmonics in resonant metasurfaces using single and multiple ultra-intense laser pulses

High harmonic generation (HHG) opens a window on the fundamental science of strong-field light-mater interaction and serves as a key building block for attosecond optics and metrology. Resonantly enhanced HHG from hot spots in nanostructures is an attractive route to overcoming the well-known limitations of gases and bulk solids. We demonstrate a nanoscale platform for highly efficient HHG driven by strong mid-infrared laser pulses: an ultra-thin resonant gallium phosphide (GaP) metasurface. The wide bandgap and the lack of inversion symmetry of the GaP crystal enable the generation of even and odd harmonics covering a wide range of photon energies between 1.3 and 3 eV with minimal reabsorption. The resonantly enhanced conversion efficiency facilitates single-shot measurements that avoid material damage and pave the way to controllable transition between perturbative and non-perturbative regimes of light-matter interactions at the nanoscale.

physics.optics

Tunable tunnel barriers in a semiconductor via ionization of individual atoms

We report scanning tunneling microscopy studies of individual adatoms deposited on an InSb(110) surface. The adatoms can be reproducibly dropped off from the STM tip by voltage pulses, and impact tunneling into the surface by up to ~100x. The spatial extent and magnitude of the tunneling effect are widely tunable by imaging conditions such as bias voltage, set current and photoillumination. We attribute the effect to occupation of a (+/0) charge transition level, and switching of the associated adatom-induced band bending. The effect in STM topographic images is well reproduced by transport modeling of filling and emptying rates as a function of the tip position. STM atomic contrast and tunneling spectra are in good agreement with density functional theory calculations for In adatoms. The adatom ionization effect can extend to distances greater than 50 nm away, which we attribute to the low concentration and low binding energy of the residual donors in the undoped InSb crystal. These studies demonstrate how individual atoms can be used to sensitively control current flow in nanoscale devices.

cond-mat.mes-hall

Single-Shot Multi-Stage Damage and Ablation of Silicon by Femtosecond Mid-infrared Laser Pulses

Although ultrafast laser materials processing has advanced at a breakneck pace over the last two decades, most applications have been developed with laser pulses at near-IR or visible wavelengths. Recent progress in mid-infrared (MIR) femtosecond laser source development may create novel capabilities for material processing. This is because, at high intensities required for such processing, wavelength tuning to longer wavelengths opens the pathway to a special regime of laser-solid interactions. Under these conditions, due to the $λ^2$ scaling, the ponderomotive energy of laser-driven electrons may significantly exceed photon energy, band gap and electron affinity and can dominantly drive absorption, resulting in a paradigm shift in the traditional concepts of ultrafast laser-solid interactions. Irreversible high-intensity ultrafast MIR laser-solid interactions are of primary interest in this connection, but they have not been systematically studied so far. To address this fundamental gap, we performed a detailed experimental investigation of high-intensity ultrafast modifications of silicon by single femtosecond MIR pulses ($λ$ = 2.7 - 4.2 $μ$m). Ultrafast melting, interaction with silicon-oxide surface layer, and ablation of the oxide and crystal surfaces were ex-situ characterized by scanning electron, atomic-force, and transmission electron microscopy combined with focused ion-beam milling, electron diffractometry, and $μ$-Raman spectroscopy. Laser induced damage and ablation (LIDA) thresholds were measured as functions of laser wavelength. The traditional theoretical models did not reproduce the wavelength scaling of the damage thresholds. To address the disagreement, we discuss possible novel pathways of energy deposition driven by the ponderomotive energy and field effects characteristic of the MIR wavelength regime.

cond-mat.mtrl-sci

Nonlinear manifestations of photon acceleration in time-dependent metasurfaces: tunable broadband harmonics generation

Time-dependent nonlinear media, such as rapidly generated plasmas produced via laser ionization of gases, can increase the energy of individual laser photons and generate tunable high-order harmonic pulses. This phenomenon, known as photon acceleration, has traditionally required extreme-intensity laser pulses and macroscopic propagation lengths. Here, we report on a novel nonlinear material$-$an ultrathin semiconductor metasurface$-$that exhibits efficient photon acceleration at low intensities. We observe a signature nonlinear manifestation of photon acceleration: third-harmonic generation of near-infrared photons with tunable frequencies reaching up to $\approx3.1ω$. A simple time-dependent coupled-mode theory, found to be in good agreement with experimental results, is utilized to predict a new path towards nonlinear radiation sources that combine resonant upconversion with broadband operation.

physics.optics

Relativistic laser driven electron accelerator using micro-channel plasma targets

We present an experimental demonstration of the efficient acceleration of electrons beyond 60 MeV using micro-channel plasma targets. We employed a high-contrast, 2.5 J, 32 fs short pulse laser interacting with a 5 μm inner diameter, 300 μm long micro-channel plasma target. The micro-channel was aligned to be collinear with the incident laser pulse, confining the majority of the laser energy within the channel. The measured electron spectrum showed a large increase of the cut-off energy and slope temperature when compared to that from a 2 μm flat Copper target, with the cutoff energy enhanced by over 2.6 times and the total energy in electrons >5 MeV enhanced by over 10 times. Three-dimensional particle-in-cell simulations confirm efficient direct laser acceleration enabled by the novel structure as the dominant acceleration mechanism for the high energy electrons. The simulations further reveal the guiding effect of the channel that successfully explains preferential acceleration on the laser/channel axis observed in experiments. Finally, systematic simulations provide scalings for the energy and charge of the electron pulses. Our results show that the micro-channel plasma target is a promising electron source for applications such as ion acceleration, Bremsstrahlung X-ray radiation, and THZ generation.

physics.plasm-ph