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Adarsh, K. V.

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

8 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Multiple Carrier Generation at an Exceptionally Low Energy Threshold

Multiple carrier generation (MCG), a process wherein two or more carriers are generated from a single high-energy absorbed photon, holds immense promise for quantum sensing, metrology, low-threshold lasers, and photovoltaics. Despite its potential, MCG has faced obstacles such as low efficiency and a high threshold photon energy at least twice the band gap (2?Eg) of the semiconductor, limiting its application only to a class of materials with low Eg. Here, we present a new approach that overcomes this limitation by leveraging carrier-donor scattering to excite secondary electrons from donor states strategically positioned below the conduction band. Our method relies on strong Coulomb interaction, reduced dielectric screening, slow hot carrier cooling, and strictly follows the energy conservation rules. We experimentally demonstrated this idea in a model system of monolayer (1L) MoS2 by exploiting electron-donating chalcogen vacancy states. We observed an exceptionally low MCG threshold of ~1.12?Eg for the first time in 1L MoS2. Remarkably, the quantum yield can be further increased to >3 by increasing the photon energy to 1.65?Eg, representing a substantial advancement over existing methods. Our findings extend the horizon of MCG into next-generation high-performance optoelectronic devices with an on-demand operating spectral range spanning from infrared to ultraviolet.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS↗
DOE OSTI2024

High-Temperature Observation of Intralayer, Interlayer, and Rydberg Excitons in Bulk Van Der Waals Alloy Single Crystals

Transition metal dichalcogenides 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 Mo0.5 W0.5 S2 and Mo0.5 W0.5 Se2 single crystals through temperature-dependent reflectance spectroscopy and first-principles calculations. We observed Rydberg excitons and interlayer excitons in both the single crystals. Notably, we provide the first experimental evidence of highly energetic A' and B' excitons in Mo0.5 W0.5 S2 at room temperature. The strong carrier-phonon scattering significantly broadens the A', B', and interlayer excitons at room temperature in bulk Mo0.5 W0.5 S2 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.

excitons↗
DOE OSTI2024

Superfluorescence from Electron-Hole Plasma at Moderate Temperatures of 175 K

Superfluorescence, a cooperative coherent spontaneous emission, is of great importance to the understanding of many-body correlation in optical processes. Even though superfluorescence has been demonstrated in many diverse systems, it is hard to observe in electron-hole plasma (EHP) due to its rapid dephasing and hence needs strong magnetic fields or complex microcavities. Herein, we report the first experimental observation of superfluorescence from EHP up to a moderate temperature of 175 K without external stimuli in a coupled metal halide perovskite quantum dots film. The EHP exhibits macroscopic quantum coherence through spontaneous synchronization. The coherence of the excited state decays by superfluorescence, which is redshifted 40 meV from the spontaneous emission with a ~1700 times faster decay rate and exhibits quadratic fluence dependence. Notably, the excited state population's delayed growth and abrupt decay, which are strongly influenced by the pump fluence and the Burnham-Chiao ringing, are the characteristics of the superfluorescence. Our findings will open up a new frontier for cooperative emission and light beam-based technologies.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS↗
DOE OSTI2022

Giant spin-selective bandgap renormalization in CsPbBr 3 colloidal nanocrystals

The spin-dependence of the strongly correlated phenomena and many-body interactions play an important role in quantum information science. In particular, it is quite interesting but unclear how the spin degree of freedom ramifies the bandgap renormalization, one of the fundamental many-body phenomena. We report the first room-temperature observation of giant spin-selective bandgap renormalization (SS-BGR) in CsPbBr 3 colloidal nanocrystals using time-resolved circularly polarized femtosecond pump-probe spectroscopy. The SS-BGR results from many-body interactions among carriers with the same spin that renormalize their joint density of states by 57+/- 1 meV, visualized here as photoinduced absorption (PIA) below band-edge transition energy when the pump and probe are co-polarized. The hallmark result of spectrally resolved SS-BGR is in stark contrast to the usually submerged signal in II-VI and III-V semiconductors and is 3 orders of magnitude larger than that observed in Ge/SiGe quantum wells, highlighting the unique and beneficial band structure of the metal-halide semiconductors. We propose that the PIA, due to SS-BGR, can be used to describe the spin-polarization and spin-relaxation dynamics. The experimental and theoretical findings open up new possibilities for optical manipulation of spin degrees of freedom and their many-body interactions in metal-halide perovskite nanocrystals for potential room-temperature applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2

Coulomb interactions in atomically thin transition metal dichalcogenides can be dynamically engineered by exploiting the dielectric environment to control the optical and electronic properties. Here we demonstrate an optically tunable giant band-gap renormalization (BGR) ~1200 and 850 meV from the edge of the conduction band and complete suppression of the exciton absorption in large-area single-layer (1L) and three-layer (3L) MoS2, respectively. The observed giant BGR is two orders of magnitude larger than that in the conventional semiconductors, and it persists for tens of ps. Strikingly, our results demonstrate photoinduced transparency at the electronic band gap using an intense optical field at room temperature. Exciton bleach recovery in 1L and 3L show a contrasting fluence-dependent response, demonstrating the layer-dependent optical tuning of exciton lifetime in a way that would be both reversible and real time. We find that the optical band gap (exciton resonance peak) shows a transient redshift followed by an anomalous blueshift from the lowest energy point as a function of the photo-generated carrier density. The observed exciton energy shift is analogous to atom-atom interactions, and it varies as a Lennard-Jones like potential as a function of the interexciton separation.

2D semiconductors↗
DOE OSTI2020

Polaron and Spin Dynamics in Organic–Inorganic Lead Halide Perovskite Nanocrystals

Long-lived carrier population and spin-based behavior in lead halide perovskite nanocrystals (NCs) are very interesting for implementing photovoltaic devices with efficiencies exceeding the Shockley–Queisser limit and quantum information processing, respectively. However, a comprehensive understanding of polaron-mediated charge carrier interactions and an accurate description of the spin-polarized states for spintronics are still lacking. Herein, the carrier and spin interactions are studied under controlled conditions in FAPbI 3 and Cs 0.01 FA 0.99 Pb(Br 0.11 I 0.89 ) 3 NCs through ultrafast transient absorption (TA) spectroscopy. At early timescales, TA spectrum shows an asymmetric derivative feature originating from the hot carrier-induced spectral redshift in FAPbI 3 NCs (55 ± 3 meV) and Cs0.01FA0.99Pb(Br0.11I0.89)3 NCs (54 ± 2 meV) at the bandedges that stabilizes to 9 ± 1 and 11 ± 2 meV, respectively, at 1 ps due to the polaron formation. The kinetic analysis indicates that the polaron populations in FAPbI3 and Cs 0.01 FA 0.99 Pb(Br 0.11 I 0.89 ) 3 NCs decay with an average lifetime of 657 ± 34 and 532 ± 28 ps, respectively. The circular polarization-resolved TA reveals that polaron formation can control spin relaxation in NCs, thus providing a powerful tool to explore the development of their prospective applications in spintronics.

36 MATERIALS SCIENCE↗