arXiv subjects

K. V. Adarsh

Publications and source records attributed to K. V. Adarsh.

At least 19 recordsLinked to original sources

arXiv2026

Ferroelastic exciton splitting in hybrid perovskite nanowalls

Hybrid metal-halide perovskites are soft semiconductors in which electronic excitations are strongly influenced by lattice distortions and structural phase transitions. An important open question is whether ferroelastic symmetry breaking merely broadens optical resonances or instead modifies excitonic states through exciton-lattice coupling. Here, we address this question using highly aligned MAPbI3 nanowalls fabricated by glancing-angle deposition, enabling symmetry-selective coupling between ferroelastic texture, structural anisotropy, and a well-defined optical axis. Combining temperature-dependent photoluminescence, X-ray diffraction and polarization-resolved ultrafast transient absorption spectroscopy, we observe a polarization-selective excitonic splitting in the orthorhombic phase at 5 K, characterized by orthogonal optical selection rules and a 45 meV energy separation. Near 160 K, where orthorhombic and tetragonal phases coexist, a lower-energy lattice-coupled excitation emerges 58 meV below the centre of the anisotropically split excitonic structure, consistent with coupling between excitonic and lattice-dressed states. At higher temperatures, these excitations progressively acquire lattice-dressed character accompanied by reduced optical anisotropy. A symmetry-guided effective Hamiltonian captures the evolution from anisotropically split excitons to coupled excitonic and lattice-dressed states across the structural transition. Our results show that ferroelastic texture and phase coexistence can modify exciton-lattice coupling, providing a route to symmetry-selective optical responses in soft polar semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

High-temperature observation of intralayer, interlayer, and Rydberg excitons in bulk van der Waals alloy single crystals

Transition metal dichalcogenides (TMDs) exhibit remarkable optical properties due to the diverse number of strongly bound excitons, which can be fine-tuned by alloying. Despite a flurry of research activity in characterizing these excitons, a comprehensive and profound understanding of their behavior with temperature is lacking. Here, we report the rich spectrum of excitonic features within bulk van der Waals alloy Mo$_{0.5}$W$_{0.5}$S$_2$ and Mo$_{0.5}$W$_{0.5}$Se$_2$ single crystals through temperature-dependent reflectance spectroscopy and first-principle calculations. We observed Rydberg excitons and interlayer excitons in both the single crystals. Notably, we provide the first experimental evidence of highly energetic A$^\prime$ and B$^\prime$ excitons in Mo$_{0.5}$W$_{0.5}$S$_2$ at room temperature. The strong carrier-phonon scattering significantly broadens the A$^\prime$, B$^\prime$ and interlayer excitons at room temperature in bulk Mo$_{0.5}$W$_{0.5}$S$_2$ single crystal compared to its selenide. Our findings, supported by density functional theory and Bethe-Salpeter equation calculations, signify the crucial role of carrier-phonon interactions. These results open pathways for next-generation optoelectronic devices and quantum technologies operating at high temperature.

cond-mat.mtrl-sci↗

arXiv2023

Enhancing the ultrafast third order nonlinear optical response by charge transfer in VSe2-reduced graphene oxide hybrid

Nonlinear optical phenomena play a critical role in understanding microscopic light-matter interactions and have far-reaching applications across various fields, such as biosensing, quantum information, optical switching, and all-optical data processing. Most of these applications require materials with high third-order absorptive and refractive optical nonlinearities. However, most materials show weak nonlinear optical responses due to their perturbative nature and often need to be improved for practical applications. Here, we demonstrate that the charge donor-acceptor hybrid of VSe2-reduced graphene oxide (rGO) hybrid exhibits enhanced ultrafast third-order absorptive and refractive nonlinearities compared to the pristine systems, at least by one order of magnitude. Through density functional theory and Bader charge analysis, we elucidate the strong electronic coupling in the VSe2-rGO hybrid, involving the transfer of electrons from VSe2 to rGO. Steady-state and time-resolved photoluminescence (PL) measurements confirm the electronic coupling and charge transfer. Furthermore, we fabricate an ultrafast optical limiter device with better performance parameters, such as an onset threshold of 2.5 mJ cm-2 and differential transmittance of 0.42.

physics.optics↗

arXiv2023

Ultrafast Third-Order Nonlinear Optical Response of Charge Coupled Gold Nanoparticle-Ge24Se76 Heterostructure

The donor-acceptor interaction of a charge-coupled heterostructure encompassing a metal and an amorphous semiconductor subjected to a laser field has many potential applications in the realm of nonlinear optics. In this work, we fabricate an electron donor gold nanoparticle (AuNP) and acceptor amorphous Ge24Se76 heterostructure on a quartz substrate using a sequential thermal evaporation technique. In this charge-coupled heterostructure, we demonstrate the ultrafast third-order nonlinear absorptive and refractive response and their sign reversal compared to pristine Ge24Se76. Enhanced optical nonlinearity in these heterostructures of varying plasmonic wavelengths is due to charge transfer, verified by the Raman spectroscopy. Further, the ultrafast transient absorption measurements support the thesis of charge transfer in the AuNP/Ge24Se76 heterostructure. These findings open up exciting opportunities for developing novel device technologies with far-reaching applications in nonlinear optics.

cond-mat.mtrl-sci↗

arXiv2023

Room temperature electron-hole liquid phase in monolayer MoSi$_2$Z$_4$ (Z = pinctogen)

Photo-excited electrons and holes in insulators, above a critical density and below a critical temperature, can condense to form an electron-hole liquid (EHL) phase. However, observing the EHL phase at room temperature is extremely challenging. Here, we introduce the monolayer MoSi$_2$Z$_4$ (Z= N, As, P) series of compounds as a promising platform for observing the EHL phase at room temperature. The higher impact of the Coulomb interactions in two dimensions helps these monolayers support the EHL phase with an increased EHL binding energy and transition temperature, along with strongly bound excitons. Our findings motivate further exploration of the MoSi$_2$Z$_4$ monolayers for realizing the EHL phase at high temperatures to harness collective phenomena for optoelectronic applications.

cond-mat.mes-hall↗

arXiv2022

Strongly bound excitons in monolayer MoSi$_2$Z$_4$ (Z = pnictogen)

Reduced dielectric screening in two-dimensional materials enables bound excitons, which modifies their optical absorption and optoelectronic response even at room temperature. Here, we demonstrate the existence of excitons in the bandgap of the monolayer family of the newly discovered synthetic MoSi$_2$Z$_4$ (Z = N, P, and As) series of materials. All three monolayers support several bright and strongly bound excitons with binding energies varying from 1 eV to 1.35 eV for the lowest energy exciton resonances. On increasing the pump fluence, the exciton binding energies get renormalized, leading to a redshift-blueshift crossover. Our study shows that the MoSi$_2$Z$_4$ series of monolayers offer an exciting test-bed for exploring the physics of strongly bound excitons and their non-equilibrium dynamics.

cond-mat.mes-hall↗

arXiv2022

Nonlinear Optical Limiting with Hybrid Nanostructures of NiCo2O4 and Multiwall Carbon Nanotubes

Nonlinear optical (NLO) response in terms of reverse saturable absorption (RSA) has been exploited extensively for optical limiting. Here, we experimentally demonstrate that flower-like hybrid nanostructures of NiCo2O4 and Multiwall Carbon Nanotubes (NCO@MWCNT) exhibit a strong non-linearity in their absorption, specifically an excited state absorption (ESA) induced RSA, when exposed to nanosecond laser pulses. We obtain strong nonlinear absorption coefficient (\b{eta}) and nonlinear refractive index (n2) in hybrid NCO@MWCNT, the values that are 2-times and 2-orders of magnitude higher, respectively compared to NCO or MWCNT alone. This offers straightforward application in optical limiting with optical limiting (FOL) and optical onset (FON) threshold ca. 2-10 times lower than benchmark NLO materials, e.g., graphene, family of 2-D transition metal dichalcogenides (TMDC) materials and recently established NCO. Notably, for femtosecond pumping, NLO response of NCO@MWCNT is dominated by saturable absorption (SA) with a week contribution from two photon absorption (TPA), arising respectively from MWCNT and NCO. A remarkable sign reversal along with a larger amplitude is obtained for n2 thanks to the charge transfer from MWCNT to NCO.

physics.optics↗

arXiv2021

Unveiling and engineering of third order optical nonlinearities in NiCo$_2$O$_4$ nanoflowers

In this paper, we demonstrate NiCo$_2$O$_4$ (NCO) as an efficient new nonlinear optical material with straightforward potential applications in optical limiting devices. We obtain nonlinear absorption coefficient ($β$) and nonlinear refractive index ($n_2$) in parallel by performing Z-scan technique, in both open and closed aperture configurations, respectively. To understand the mechanism responsible for third order optical nonlinearity in NCO, we excited the sample with contrasting laser pulse durations, 7 ns and 120 fs, at two different off-resonant wavelengths. For ns excitation, nonlinearity is mediated by excited state absorption (ESA) and free-carrier absorption, that gives rise to large \b{eta}ESA and positive $n_2$. On the other hand, when excited with fs laser, two-photon absorption (TPA) takes place and bound carriers induce strong negative $n_2$. The values obtained for $β$ and $n_2$ in NCO are found to be higher among the family of well-known conventional transition metal oxides, therefore are promising for optics and other photonics applications.

physics.optics↗

arXiv2021

Pulse-duration dependence of saturable and reverse saturable absorption in ZnCo2O4 microflowers

We employed open-aperture Z-scan technique to unveil the third-order optical nonlinearity in ZnCo2O4 (ZCO) microflowers. Our results indicate that intersystem crossing (ISC) lifetime can be used as simple tool to demonstrate remarkably contrasting optical nonlinearity in ZCO. Ultrafast transient absorption measurements reveal that ISC from singlet to triplet state takes place in 5 ps. For femtosecond laser pulses, when the pulse duration is shorter than ISC lifetime, saturable absorption (SA) takes place for all intensities. On the contrary, when the pulse duration is longer than ISC for nanosecond excitation, we observe transition from SA to reverse SA (RSA) at higher intensities via excited-state absorption. We envisage that benefiting from SA and RSA, ZCO emerges as potential candidate for mode locking and optical limiting devices.

physics.optics↗

arXiv2020

Intriguing electronic and optical prospects of FCC bimetallic two-dimensional heterostructures: epsilon near-zero behaviour in UV-vis range

Higher superconducting critical temperature and large-area epsilon-near-zero interfaces are two long-standing goals of Condensed Matter Physics and Optics. Motivated by the recent advancements of experimental interests on metallic nanostructures, we have theoretically investigated some selected bimetallic FCC combinations starting from large-area interface to embedded and doped two-dimensional (2D) nanostructures. Using different first-principles techniques, encompassing density functional theory (DFT), time-dependent DFT (TDDFT), phonon and DFT-coupled quantum transport, we propose the prospects of some selective bimetallic nanostructures like Au/Ag and Pt/Pd to exhibit exotic electronic phenomena. For 2D doped and embedded nanostructures of these systems, non-trivial band-structure and Fermi-surface topology may be emblematic to the presence of instabilities like charge density waves. We specifically highlight the optical attributes extracted from the TDDFT calculations for these systems, where interfacial morphology induced band-localization leads to near-zero behavior of both real and imaginary parts of the dynamical dielectric response is observed in the ultra-violet to visible (UV-vis) optical range. Low-energy intra-band plasmonic oscillations present for individual metallic surfaces are completely suppressed for embedded and doped nanostructures. Phonon-dispersion of the model systems indicates the presence of soft phonons and dynamical instabilities. Quantum transport calculations on simplest possible device made out of these bimetallic systems reveals generation of highly transmitting pockets over the cross-sectional area for some selected device geometry. We envisage that, if observed experimentally, such systems may lead to many fascinating physics and applications in many diverse fields ranging from condensed matter physics to optics or even more.

cond-mat.supr-con↗

arXiv2020

Near resonant nanosecond laser driven nonlinear optical response in As50S50 thin films

Nanosecond near resonant excitation in As50S50 thin films leads to strong nonlinear optical response, i.e. nonlinear absorption coefficient up to 4 x 106 cm/GW and nonlinear refractive index of 8.5 cm2/GW, both of which is the strongest ever reported in amorphous semiconductors. We propose a five-level energy model to explain such effect which indicates that nonlinear process is reverse saturable absorption in nature, mediated by excited state absorption from triplet-triplet transition. On the other hand, observation of negative nonlinear refractive index reveals the occurrence of self-defocusing effect. Finally, benefitting from the strong nonlinear response, we demonstrate a promising application of As50S50 thin films as an optical limiter for optoelectronic sensors.

physics.optics↗

arXiv2018

Quantification of nonlinear absorption in ternary As-Sb-Se chalcogenide glasses

In this article, we studied intensity dependent third order nonlinear optical response in ternary As40Sb7Se53 and As40Sb10Se50 chalcogenide glasses by employing nanosecond Z-scan technique. At low intensity, we observed saturable absorption in As40Sb7Se53 which makes a remarkable transition to reverse saturable absorption at higher intensities. On the other hand, when the Sb concentration increased in As40Sb10Se50, saturable absorption disappears and the sample exhibits only two-photon absorption. Experimental results further indicate that the strong two-photon absorption in our samples can be exploited to fabricate high performance solid state optical limiting devices for next generation all-optical network.

physics.optics↗

arXiv2018

Intricate modulation of interlayer coupling at GO/MoSe2 interface: application in time-dependent optics and device transport

In GO/MoSe2 semiconductor heterostructure, we have demonstrated a subtle control on the doping dynamics by modulating interlayer coupling through the combination of strain-reducing relative rotation of the constituting layers and variation of ligand type and concentration. By first-principles calculations incorporating spin-orbital coupling, we have investigated the impact of variable interlayer coupling in introducing non-collinear magnetic behaviour in the heterostructure. The outcome of varying carrier type and their respective concentrations are investigated by static as well as time dependent density functional calculations, which indicates presence of optical anisotropy and time-dependent optical phenomena like exciton quenching and band-gap renormalization. Performance of such heterostructures as channel material in devices with top and edge metal contacts is analyzed. Our self-consistent quantum transport calculations have evinced that the nature of interface-induced variation in doping is extrapolated for devices only in the case of top contacts. The edge contact, although exhibits a better transmission, are inefficient for sensing the ligand-induced doping modulation introduced via vertical inter-layer charge transfer.

cond-mat.mtrl-sci↗

arXiv2018

Kinetics of photo-dissolution within Ag/As2S3 heterostructure

Chalcogenide glass-silver heterostructures are candidates for photoresist and diffractive optical applications. To optimize their processing, we report the kinetics of Ag photo-dissolution in As2S3 matrix using in-situ optical transmission/reflection measurements and real time atomic force microscopy (AFM) imaging under optical illumination. The results indicate that photodissolution occurs in three stages with the extent and kinetics of each stage depending strongly on Ag film thickness. By contrast, the photo-dissolution is found to be independent of As2S3 matrix thickness. The extent of three stages also depends strongly on the laser dose and can be reduced to two stages at higher laser fluence. A comparative study of two oppositely stacked sample configurations: As2S3/Ag/glass and Ag/As2S3/glass show that the heterostructures respond differently to light illumination. For the former, Ag dissolves completely into As2S3 matrix at a faster rate than for the latter case. The origin of this difference is established by energy dispersive X-ray spectroscopy and AFM measurements.

cond-mat.mtrl-sci↗

arXiv2018

Ultrafast light-induced softening of chalcogenide thin films above the rigidity percolation transition

Little is known about the role of network rigidity in light-induced structural rearrangements in network glasses due to a lack of supporting experiments and theories. In this report, we demonstrate for the first time the ultrafast structural rearrangements manifested as induced absorption (IA) over a broad spectral range in a-GexAs35-xSe65 thin films above the mean-field rigidity percolation transition, quantified by the mean coordination number = 2.40. The IA spectrum arising from self-trapped excitons, induced structural rearrangements by softening the glass network that strikingly reveal two relaxation mechanisms which differ by one order of magnitude. The fast kinetics of electron-lattice interaction occurs within 1 ps, exhibits a weak dependence on rigidity and dominates in the sub-bandgap region. In a stark contrast, the slow kinetics are associated with the structural changes in the bandgap region and depends strongly on network rigidity. Our results further demonstrate that amplitude of IA scales a linear relationship with excitation fluence which provides a unique way to induce structural rearrangements in over-coordinated network to exploit it for practical purposes. Our results modify the conventional concept of rigidity dependence of light-induced effects in network glasses, when excited with an ultrafast laser.

cond-mat.mtrl-sci↗

arXiv2018

Designing hybrid graphene oxide- gold nanoparticles for nonlinear optical response: Experiment and theory

Nonlinear optical absorption of light by materials are weak due to its perturbative nature, although a strong nonlinear response is of crucial importance to applications in optical limiting and switching. Here we demonstrate experimentally and theoretically an extremely efficient scheme of excited state absorption by charge transfer between donor and acceptor materials as the new method to enhance the nonlinear absorption by orders of magnitude. With this idea, we have demonstrated strong excited state absorption (ESA) in reduced graphene oxide that otherwise shows increased transparency at high fluence and enhancement of ESA by one orders of magnitude in graphene oxide by attaching gold nanoparticles (AuNP) in the tandem configuration that acts as an efficient charge transfer pair when excited at the plasmonic wavelength. To explain the unprecedented enhancement, we have developed a five-level rate equation model based on the charge transfer between the two materials and numerically simulated the results. To understand the correlation of interfacial charge-transfer with the concentration and type of the functional ligands attached to the graphene oxide sheet, we have investigated the AuNP-graphene oxide interface with various possible ligand configurations from first-principles calculations. By using the strong ESA of our hybrid materials, we have fabricated liquid cell-based high-performance optical limiters with important device parameters better than that of the benchmark optical limiters.

cond-mat.mes-hall↗

arXiv2017

Enhancement of Two photon absorption with Ni doping in the dilute magnetic Semiconductor ZnO Crystalline Nanorods

In this letter, we have investigated the third-order optical nonlinearities of high-quality Ni doped ZnO nanorods crystallized in wurtzite lattice, prepared by the wet chemical method. In our experiments, we found that the two photon absorption coefficient beta increases by as much as 14 times i.e. 7.6 err 0.4 to 112 err 6 cm per GW, when the Ni doping is increased from 0 to 10 percent. The substantial enhancement in beta is discussed in terms of the bandgap scaling and Ni doping. Furthermore, we also show that the optical bandgap measured by UVVis and photo luminescence spectroscopic, continuously red shift with increasing Ni doping concentration. We envision that the strong nonlinear optical properties together with their dilute magnetic effects, they form an important class of materials for potential applications in magneto-optical and integrated optical chips.

cond-mat.mtrl-sci↗

arXiv2015

Nanosecond light induced, thermally tunable transient dual absorption bands in a-Ge5As30Se65 thin film

In this article, we report the first observation of nanosecond laser induced transient dual absorption bands, one in the bandgap (TA1) and another in the sub-bandgap (TA2) regions of a-Ge5As30Se65 thin films. Strikingly, these bands are thermally tunable and exhibit a unique contrasting characteristic: the magnitude of TA1 decreases while that of TA2 increases with increasing temperature. Further, the decay kinetics of these bands is strongly influenced by the temperature, which signifies a strong temperature-dependent exciton recombination mechanism. The induced absorption shows quadratic and the decay time constant shows linear dependence on the laser beam fluence.

cond-mat.mtrl-sci↗