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

Abstract

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.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [3]; ORCiD logo [3];  [2]; ORCiD logo [1]
  1. Indian Inst. of Science Education and Research, Bhopal (India)
  2. Indian Inst. of Technology (IIT), Kanpur (India)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1832860
Report Number(s):
NREL/JA-5900-79661
Journal ID: ISSN 2469-9950; MainId:35882;UUID:21da61b0-b668-478b-8290-8d8bc429c53a;MainAdminID:63268; TRN: US2216795
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 104; Journal Issue: 20; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 2D semiconductors; solar-photochemistry

Citation Formats

Bera, Santu K., Shrivastava, Meghanns, Bramhachari, Khamari, Zhang, Hanyu, Poonia, Ajay K., Mandal, Dipendranath, Miller, Elisa M., Beard, Matthew C., Agarwal, Amit, and Adarsh, K. V. Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2. United States: N. p., 2021. Web. doi:10.1103/physrevb.104.l201404.
Bera, Santu K., Shrivastava, Meghanns, Bramhachari, Khamari, Zhang, Hanyu, Poonia, Ajay K., Mandal, Dipendranath, Miller, Elisa M., Beard, Matthew C., Agarwal, Amit, & Adarsh, K. V. Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2. United States. https://doi.org/10.1103/physrevb.104.l201404
Bera, Santu K., Shrivastava, Meghanns, Bramhachari, Khamari, Zhang, Hanyu, Poonia, Ajay K., Mandal, Dipendranath, Miller, Elisa M., Beard, Matthew C., Agarwal, Amit, and Adarsh, K. V. Thu . "Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2". United States. https://doi.org/10.1103/physrevb.104.l201404. https://www.osti.gov/servlets/purl/1832860.
@article{osti_1832860,
title = {Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2},
author = {Bera, Santu K. and Shrivastava, Meghanns and Bramhachari, Khamari and Zhang, Hanyu and Poonia, Ajay K. and Mandal, Dipendranath and Miller, Elisa M. and Beard, Matthew C. and Agarwal, Amit and Adarsh, K. V.},
abstractNote = {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.},
doi = {10.1103/physrevb.104.l201404},
journal = {Physical Review B},
number = 20,
volume = 104,
place = {United States},
year = {2021},
month = {11}
}

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