arXiv subjects

Aditya D. Mohite

Publications and source records attributed to Aditya D. Mohite.

At least 19 recordsLinked to original sources

arXiv2026

Quantum Dot Moiré from Crossed MoS2 Nanoribbons

Twisted atomically thin layers have attracted much attention for Moiré potential and correlated quantum phenomena. However, existing Moiré superlattices have largely been limited to extensive wavefunction without lateral confinement. Here we introduce a new platform where 1D nanoribbons of 2D MoS2 grown by vapor deposition can be easily superposed at various angles from stacking and transferring, to form Moiré quantum dots at their intersections with unique exciton physics. Angle-dependent Moiré intersections show enhanced exciton emission at commensurate angle 22 deg, which demonstrates faster relaxation at the cryogenic temperature. A size-dependent study further exhibits a reduced exciton energy and soften out-of-plane interlayer coupling for smaller Moiré areas. Our results reveal exciton physics turnability via precise overlapping of 1D nanoribbons.

cond-mat.mtrl-sci↗

arXiv2025

Symmetry-Controlled Ultrastrong Phonon-Photon Coupling in a Terahertz Cavity

Optical cavities provide a powerful means to engineer light-matter hybrid states by coupling confined electromagnetic fields with matter excitations. Achieving in situ control of the coupling strength is essential for investigating how such hybridization evolves with the coupling strength. In this work, we use a symmetry-changing structural phase transition in lead halide perovskites to reversibly tune the phonon-photon coupling strength, leveraging the fact that their phonon frequencies and oscillator strengths are dictated by lattice symmetry. Terahertz time-domain spectroscopy of MAPbI3 embedded in nanoslot cavities reveals three polariton branches above the critical temperature Tc = 162.5 K, and the emergence of an additional branch below Tc, activated by a new phonon mode in the low-temperature phase. The full dispersion is accurately reproduced using a multimode Hopfield model, confirming that all normalized coupling strengths remain in the ultrastrong coupling regime. These results demonstrate symmetry-controlled tuning of ultrastrong coupling via phonon engineering in optical cavities.

quant-ph↗

arXiv2025

Multimode Phonon-Polaritons in Lead-Halide Perovskites in the Ultrastrong Coupling Regime

Phonons play a central role in fundamental solid-state phenomena, including superconductivity, Raman scattering, and symmetry-breaking phases. Harnessing phonons to control these effects and enable quantum technologies is therefore of great interest. However, most existing phonon control strategies rely on external driving fields or anharmonic interactions, limiting their applicability. Here, we realize multimode ultrastrong light--matter coupling and theoretically show the modulation of phonon emission. This regime is realized by coupling two optical phonon modes in lead halide perovskites to a nanoslot array functioning as a single-mode cavity. The small mode volume of the nanoslots enables high coupling strengths in the phonon-polariton system. We show theoretically that the nanoslot resonator mediates an effective interaction between phonon modes, leading to superthermal phonon bunching in thermal equilibrium between distinct modes. Our findings are well described by a multimode Hopfield model. This work establishes a pathway for engineering phononic properties for light-harvesting and light-emitting technologies.

quant-ph↗

arXiv2025

Unconventional Temperature Dependence of Exciton Diamagnetism in 2D Ruddlesden-Popper Lead Halide Perovskites

Layered hybrid perovskites containing larger organic cations have demonstrated superior environmental stability, but the presence of these insulating spacers also strengthens the exciton binding energy, which contributes to reduced carrier separation. The consequences of increased binding energy on device efficiency are still not fully documented, and binding energy measurements are often conducted at cryogenic temperatures where linewidths are decreased and a series of hydrogen-like bound states can be identified, but not under ambient conditions where devices are expected to operate. In contrast to the quenching observed in 3D perovskites such as methylammonium lead iodide, where exciton binding energies are thought to decrease at higher temperatures, we present evidence for a smaller excitonic radius at higher temperatures in the $n=5$ member of butylammonium-spaced methylammonium lead iodide, (BA)$_2$(MA)$_{n-1}$Pb$_n$I$_{3n+1}$. We measured the temperature-dependent diamagnetic shift coefficient in magnetic fields up to 40\,T, which is one-third as large at room temperature as those at cryogenic temperatures. In both the ideal 2D and 3D hydrogen models, this trend would indicate that the exciton binding energy more than triples at room temperature.

cond-mat.mtrl-sci↗

arXiv2025

Two-dimensional perovskites with maximum symmetry enable exciton diffusion length exceeding 2 micrometers

Realizing semiconductors with high symmetry of their crystallographic structures has been a virtue of inorganic materials and has resulted in novel physical behaviors. In contrast, hybrid (organic and inorganic) crystals such as two-dimensional metal halide perovskites exhibit much lower crystal symmetry due to in-plane or out of plane octahedral distortions. Despite their amazing ability for photoinduced light emission at room temperature, the Achilles' heel of this attractive class of 2D materials for optoelectronics remains the poor control and lack of performance for charge carrier transport. Inspired by the tremendous charge carrier properties of the 3D cubic perovskite phase of FAPbI3 and combining the use of the appropriate cage cation, the spacer molecule and the temperature and rate of crystallization, we report a new series of FA-based layered two-dimensional perovskites that exhibits the highest theoretically predicted symmetry with a tetragonal P4/mmm space group, resulting in no octahedral distortion in both in-plane and out-of-plane directions. These 2D perovskites present the shortest interlayer distances (4 angstrom), which results in systematically lower bandgaps (1.7 to 1.8 eV). Finally, the absence of octahedral distortions, results in an exciton diffusion length of 2.5 μm, and a diffusivity of 4.4 cm2s-1, both of which are an order of magnitude larger compared to previously reported 2D perovskites and on par with monolayer transition metal dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2025

Overcoming the surface paradox: Buried perovskite quantum dots in wide-bandgap perovskite thin films

Colloidal perovskite quantum dots (PQDs) are an exciting platform for on-demand quantum, and classical optoelectronic and photonic devices. However, their potential success is limited by the extreme sensitivity and low stability arising from their weak intrinsic lattice bond energy and complex surface chemistry. Here we report a novel platform of buried perovskite quantum dots (b-PQDs) in a three-dimensional perovskite thin-film, fabricated using one-step, flash annealing, which overcomes surface related instabilities in colloidal perovskite dots. The b-PQDs demonstrate ultrabright and stable single-dot emission, with resolution-limited linewidths below 130 μeV, photon-antibunching (g^2(0)=0.1), no blinking, suppressed spectral diffusion, and high photon count rates of 10^4/s, consistent with unity quantum yield. The ultrasharp linewidth resolves exciton fine-structures (dark and triplet excitons) and their dynamics under a magnetic field. Additionally, b-PQDs can be electrically driven to emit single photons with 1 meV linewidth and photon-antibunching (g^2(0)=0.4). These results pave the way for on-chip, low-cost single-photon sources for next generation quantum optical communication and sensing.

physics.optics↗

arXiv2024

Keldysh tuning of photoluminescence in a lead halide perovskite crystal

In 1964, Keldysh laid the groundwork for strong-field physics in atomic, molecular, and solid-state systems by delineating a ubiquitous transition from multiphoton absorption to quantum electron tunneling under intense AC driving forces. While both processes in semiconductors can generate carriers and result in photon emission through electron-hole recombination, the low quantum yields in most materials have hindered direct observation of the Keldysh crossover. Leveraging the large quantum yields of photoluminescence in lead halide perovskites, we show that we can not only induce bright light emission from extreme sub-bandgap light excitation but also distinguish between photon-induced and electric-field-induced processes. Our results are rationalized by the Landau-Dykhne formalism, providing insights into the non-equilibrium dynamics of strong-field light-matter interactions. These findings open new avenues for light upconversion and sub-bandgap photon detection, highlighting the potential of lead halide perovskites in advanced optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2023

Architecture Optimization Dramatically Improves Reverse Bias Stability in Perovskite Solar Cells: A Role of Polymer Hole Transport Layers

We report that device architecture engineering has a substantial impact on the reverse bias instability that has been reported as a critical issue in commercializing perovskite solar cells. We demonstrate breakdown voltages exceeding -15 V in typical pin structured perovskite solar cells via two steps: i) using polymer hole transporting materials; ii) using a more electrochemically stable gold electrode. While device degradation can be exacerbated by higher reverse bias and prolonged exposure, our as-fabricated perovskite solar cells completely recover their performance even after stressing at -7 V for 9 hours both in the dark and under partial illumination. Following these observations, we systematically discuss and compare the reverse bias driven degradation pathways in perovskite solar cells with different device architectures. Our model highlights the role of electrochemical reaction rates and species in dictating the reverse bias stability of perovskite solar cells.

physics.chem-ph↗

arXiv2022

Deterministic synthesis of phase pure 2D perovskites via progressive transformation of layer thickness

Two-dimensional (2D) halide perovskites have emerged as semiconductor platforms for realizing efficient and durable optoelectronic devices. However, the reproducible synthesis of 2D perovskite crystals with desired layer thickness (or n value) greater than 2, has been an enduring challenge due to the lack of kinetic control (temperature, time, stoichiometry) for each layer thickness. Here, we demonstrate a novel method term as the kinetically controlled space confinement (KCSC) for the deterministic growth of phase pure Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) 2D perovskites. The phase-pure growth was achieved by progressively increasing the temperature (fixed time) or the crystallization time (fixed temperature), which allowed for an acute control of the crystallization kinetics. We also observe a systematic transformation from a lower n-value to n=3, 4, 5, 6 in 2D perovskites. In-situ photoluminescence spectroscopy and imaging suggest that the progressive transformation from lower to higher n-value occurs via intercalation of excess precursor ions. These experiments enabled the development of a machine learning assisted multi-parameter phase diagram, which predicts the growth of 2D phase with a specific n-value.

cond-mat.mtrl-sci↗

arXiv2022

Direct visualization of ultrafast lattice ordering triggered by an electron-hole plasma in 2D perovskites

Direct visualization of ultrafast coupling between charge carriers and lattice degrees of freedom in photo-excited semiconductors has remained a long-standing challenge and is critical for understanding the light-induced physical behavior of materials under extreme non-equilibrium conditions. Here, by monitoring the evolution of the wave-vector resolved ultrafast electron diffraction intensity following above-bandgap photo-excitation, we obtain a direct visual of the structural dynamics in monocrystalline 2D perovskites. Analysis reveals a surprising, light-induced ultrafast lattice ordering resulting from a strong interaction between hot-carriers and the perovskite lattice, which induces an in-plane octahedra rotation, towards a more symmetric phase. Correlated ultrafast spectroscopy performed at the same carrier density as ultrafast electron diffraction reveals that the creation of a hot and dense electron-hole plasma triggers lattice ordering at short timescales by modulating the crystal cohesive energy. Finally, we show that the interaction between the carrier gas and the lattice can be altered by tailoring the rigidity of the 2D perovskite by choosing the appropriate organic spacer layer.

cond-mat.mtrl-sci↗

arXiv2022

Cavity-Enhanced Raman Scattering from 2D Hybrid Perovskites

Two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs) are promising candidates for optoelectronic applications due to their efficient light emission properties, and strong dielectric confinement effects. Raman spectroscopy is a versatile, non-contact and often non-destructive technique, widely used to characterize crystalline materials. However, the inherently weak phonon scattering, strong background, and complex nature of the Raman signals from HOIPs present challenges in obtaining reliable signals. Further, the fragile nature of the 2D HOIP crystals results in rapid degradation upon exposure to heat, light and moisture, which presents further difficulty in enhancing Raman scattered photon signals. Herein, we report a novel approach to enhance the weak Raman scattering signals in Ruddlesden-Popper (RP) phase HOIPs by introducing an open-cavity comprising HOIP crystals on a gold substrate. We observe 15x enhancement of the Raman signals due to the Purcell effect inside the high-index HOIP crystals. Our simple approach can be extended to enhance the study of phonon scattering in other HOIP and van der Waals layered crystals.

cond-mat.mtrl-sci↗

arXiv2021

Self-Hybridized Polaritonic Emission from Layered Perovskites

Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (> 100 nm) crystals and near-unity absorption in thin (< 20 nm) crystals. We observe resonances with quality factors > 250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D-HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry.

physics.optics↗

arXiv2020

Determination of Dielectric Functions and Exciton Oscillator Strength of Two-Dimensional Hybrid Perovskites

Two-dimensional (2D) hybrid organic inorganic perovskite (HOIP) semiconductors have attracted widespread attention as a platform of next generation optoelectronic devices benefiting from their naturally occurring and tunable multiple quantum-well like (QW) structures, which enable a wide range of physical properties. Determining the intrinsic optical/electronic properties of 2D HOIPs is extremely important for further utility in photonic and optoelectronics devices. Here, we obtain the optical dielectric functions, complex refractive indices, and complex optical conductivities of both Ruddlesden-Popper (RP) and Dion-Jacobsen (DJ) phases of 2D HOIPs as a function of the perovskite QW thickness via spectroscopic ellipsometry over a broad energy range of 0.73 - 3.34 eV. We identify a series of feature peaks in the dielectric functions, and explain the evolution of ground state exciton peak with unit cell thickness and changing excitonic confinement. We observe extraordinary values of optical extinction and electric loss tangents at the primary excitonic resonances and provide their detailed comparison with other known excitonic materials. Our study is expected to lay foundation for understanding optical properties of pure phase 2D HOIPs, which will be helpful for the accurate modelling of their photonics and optoelectronic devices.

physics.app-ph↗

arXiv2019

Opto-valleytronic imaging of atomically thin semiconductors

Transition metal dichalcogenide semiconductors represent elementary components of layered heterostructures for emergent technologies beyond conventional opto-electronics. In their monolayer form they host electrons with quantized circular motion and associated valley polarization and valley coherence as key elements of opto-valleytronic functionality. Here, we introduce two-dimensional polarimetry as means of direct imaging of the valley pseudospin degree of freedom in monolayer transition metal dichalcogenides. Using MoS$_2$ as a representative material with valley-selective optical transitions, we establish quantitative image analysis for polarimetric maps of extended crystals, and identify valley polarization and valley coherence as sensitive probes of crystalline disorder. Moreover, we find site-dependent thermal and non-thermal regimes of valley-polarized excitons in perpendicular magnetic fields. Finally, we demonstrate the potential of wide-field polarimetry for rapid inspection of opto-valleytronic devices based on atomically thin semiconductors and heterostructures.

cond-mat.mes-hall↗

arXiv2019

Signatures of defect-localized charged excitons in the photoluminescence of monolayer molybdenum disulfide

We study spatial photoluminescence characteristics of neutral and charged excitons across extended monolayer MoS$_2$ synthesized by chemical vapor deposition. Using two-dimensional hyperspectral photoluminescence mapping at cryogenic temperatures we identify regions with increased emission from charged excitons associated with both spin-orbit split valence subbands. Such regions are attributed to unintentional doping at defect sites with excess charge that bind neutral excitons to form defect-pinned trions. Our findings imply comparable timescales for the formation, relaxation, and radiative decay of $B$ trions, and add defect-localized $A$ and $B$ trions to the realm of photoexcited quasiparticles in layered semiconductors.

cond-mat.mes-hall↗

arXiv2019

Free-standing bialkali photocathodes using atomically thin substrates

We report successful deposition of high quantum efficiency (QE) bialkali antimonide K2CsSb photocathodes on graphene films. The results pave a pathway towards an ultimate goal of encapsulating technologically-relevant photocathodes for accelerator technology with an atomically-thin protecting layer to enhance lifetime while minimizing QE losses. A QE of 17 % at ~3.1 eV (405 nm) is the highest value reported so far on graphene substrates and is comparable to that obtained on stainless steel and nickel reference substrates. The spectral responses of the photocathodes on graphene exhibit signature features of K2CsSb including the characteristic absorption at ~2.5 eV. Materials characterization based on X-ray fluorescence (XRF) and X-ray diffraction (XRD) reveals that the composition and crystal quality of these photocathodes deposited on graphene is comparable to those deposited on a reference substrate. Quantitative agreement between optical calculations and QE measurements for the K2CsSb on free suspended graphene and a graphene coated metal substrate further confirms the high quality interface between the photocathodes and graphene. Finally, a correlation between the QE and graphene quality as characterized by Raman spectroscopy suggests that a lower density of atomistic defects in the graphene films leads to higher QE of the deposited K2CsSb photocathodes.

cond-mat.mtrl-sci↗

arXiv2018

Polariton hyperspectral imaging of two-dimensional semiconductor crystals

Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form quasiparticles known as polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with cavity-assisted hyperspectral imaging. Using extended WS$_2$ monolayers, we establish the regime of strong coupling with a scanning microcavity to map out polariton properties and correlate their spatial features with intrinsic and extrinsic effects. We find a high level of homogeneity, and show that polariton splitting variations are correlated with intrinsic exciton properties such as oscillator strength and linewidth. Moreover, we observe a deviation from thermal equilibrium in the resonant polariton population, which we ascribe to non-perturbative polariton-phonon coupling. Our measurements reveal a promisingly consistent polariton landscape, and highlight the importance of phonons for future polaritonic devices.

physics.optics↗

arXiv2018

A Physics-based Analytical Model for Perovskite Solar Cells

Perovskites are promising next-generation absorber materials for low-cost and high-efficiency solar cells. Although perovskite cells are configured similar to the classical solar cells, their operation is unique and requires development of a new physical model for characterization, optimization of the cells, and prediction of the panel performance. In this paper, we develop such a physics-based analytical model to describe the operation of different types of perovskite solar cells, explicitly accounting non-uniform generation, carrier selective transport layers, and voltage-dependent carrier collection. The model would allow experimentalists to characterize key parameters of existing cells, understand performance bottlenecks, and predict performance of perovskite-based solar panel - the obvious next step to the evolution of perovskite solar cell technology.

cond-mat.mes-hall↗