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:
-
- Indian Inst. of Science Education and Research, Bhopal (India)
- Indian Inst. of Technology (IIT), Kanpur (India)
- 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}
}
Works referenced in this record:
Surface Recombination Limited Lifetimes of Photoexcited Carriers in Few-Layer Transition Metal Dichalcogenide MoS 2
journal, November 2015
- Wang, Haining; Zhang, Changjian; Rana, Farhan
- Nano Letters, Vol. 15, Issue 12
Observation of Exciton Redshift–Blueshift Crossover in Monolayer WS 2
journal, June 2017
- Sie, E. J.; Steinhoff, A.; Gies, C.
- Nano Letters, Vol. 17, Issue 7
Dielectric Screening of Excitons and Trions in Single-Layer MoS 2
journal, September 2014
- Lin, Yuxuan; Ling, Xi; Yu, Lili
- Nano Letters, Vol. 14, Issue 10
Giant gate-tunable bandgap renormalization and excitonic effects in a 2D semiconductor
journal, July 2019
- Qiu, Zhizhan; Trushin, Maxim; Fang, Hanyan
- Science Advances, Vol. 5, Issue 7
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Renormalization of the quasiparticle band gap in doped two-dimensional materials from many-body calculations
journal, October 2017
- Gao, Shiyuan; Yang, Li
- Physical Review B, Vol. 96, Issue 15
Band renormalization and spin polarization of MoS 2 in graphene/MoS 2 heterostructures
journal, November 2015
- Coy-Diaz, Horacio; Bertran, François; Chen, Chaoyu
- physica status solidi (RRL) - Rapid Research Letters, Vol. 9, Issue 12
Band structure engineering in van der Waals heterostructures via dielectric screening: the GΔW method
journal, March 2017
- Winther, Kirsten T.; Thygesen, Kristian S.
- 2D Materials, Vol. 4, Issue 2
Population inversion and giant bandgap renormalization in atomically thin WS2 layers
journal, June 2015
- Chernikov, Alexey; Ruppert, Claudia; Hill, Heather M.
- Nature Photonics, Vol. 9, Issue 7
Exciton fission in monolayer transition metal dichalcogenide semiconductors
journal, October 2017
- Steinhoff, A.; Florian, M.; Rösner, M.
- Nature Communications, Vol. 8, Issue 1
Influence of Excited Carriers on the Optical and Electronic Properties of MoS 2
journal, June 2014
- Steinhoff, A.; Rösner, M.; Jahnke, F.
- Nano Letters, Vol. 14, Issue 7
Observation of Rapid Exciton–Exciton Annihilation in Monolayer Molybdenum Disulfide
journal, September 2014
- Sun, Dezheng; Rao, Yi; Reider, Georg A.
- Nano Letters, Vol. 14, Issue 10
Absorption of light by excitons and trions in monolayers of metal dichalcogenide : Experiments and theory
journal, May 2014
- Zhang, Changjian; Wang, Haining; Chan, Weimin
- Physical Review B, Vol. 89, Issue 20
Optical Spectrum of : Many-Body Effects and Diversity of Exciton States
journal, November 2013
- Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.
- Physical Review Letters, Vol. 111, Issue 21
Subband-level renormalization and absorptive optical bistability in semiconductor multiple quantum well structures
journal, October 1984
- Schmitt-Rink, S.; Ell, C.; Koch, S. W.
- Solid State Communications, Vol. 52, Issue 2
Electronic excitations: density-functional versus many-body Green’s-function approaches
journal, June 2002
- Onida, Giovanni; Reining, Lucia; Rubio, Angel
- Reviews of Modern Physics, Vol. 74, Issue 2
Atomically Thin A New Direct-Gap Semiconductor
journal, September 2010
- Mak, Kin Fai; Lee, Changgu; Hone, James
- Physical Review Letters, Vol. 105, Issue 13, Article No.136805
Evidence for the Dominance of Carrier-Induced Band Gap Renormalization over Biexciton Formation in Cryogenic Ultrafast Experiments on MoS 2 Monolayers
journal, March 2020
- Wood, Ryan E.; Lloyd, Lawson T.; Mujid, Fauzia
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 7
Coulomb engineering of the bandgap and excitons in two-dimensional materials
journal, May 2017
- Raja, Archana; Chaves, Andrey; Yu, Jaeeun
- Nature Communications, Vol. 8, Issue 1
Bandgap Engineering of Strained Monolayer and Bilayer MoS2
journal, July 2013
- Conley, Hiram J.; Wang, Bin; Ziegler, Jed I.
- Nano Letters, Vol. 13, Issue 8, p. 3626-3630
Effects of confinement and environment on the electronic structure and exciton binding energy of MoS from first principles
journal, December 2012
- Komsa, Hannu-Pekka; Krasheninnikov, Arkady V.
- Physical Review B, Vol. 86, Issue 24
Dimensionality dependence of the band-gap renormalization in two- and three-dimensional electron-hole plasmas in GaAs
journal, January 1987
- Tränkle, G.; Leier, H.; Forchel, A.
- Physical Review Letters, Vol. 58, Issue 4
Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012
- Ramasubramaniam, Ashwin
- Physical Review B, Vol. 86, Issue 11
The Bethe–Salpeter equation: a first-principles approach for calculating surface optical spectra
journal, September 2004
- Palummo, M.; Pulci, O.; Sole, R. Del
- Journal of Physics: Condensed Matter, Vol. 16, Issue 39
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014
- Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
- Nature Materials, Vol. 13, Issue 12
Layer-dependent resonant Raman scattering of a few layer MoS 2 : Raman scattering of a few layer MoS
journal, September 2012
- Chakraborty, Biswanath; Matte, H. S. S. Ramakrishna; Sood, A. K.
- Journal of Raman Spectroscopy, Vol. 44, Issue 1
Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018
- Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
- Reviews of Modern Physics, Vol. 90, Issue 2
Bandgap renormalization at finite carrier densities in semiconductor quantum wells and mesa structures
journal, January 1990
- Reinecke, T. L.; Broido, D. A.; Lach, E.
- Superlattices and Microstructures, Vol. 7, Issue 4
Optical generation of high carrier densities in 2D semiconductor heterobilayers
journal, September 2019
- Wang, Jue; Ardelean, Jenny; Bai, Yusong
- Science Advances, Vol. 5, Issue 9
Anomalous Lattice Vibrations of Single- and Few-Layer MoS 2
journal, March 2010
- Lee, Changgu; Yan, Hugen; Brus, Louis E.
- ACS Nano, Vol. 4, Issue 5
Tightly Bound Excitons in Monolayer
journal, July 2014
- He, Keliang; Kumar, Nardeep; Zhao, Liang
- Physical Review Letters, Vol. 113, Issue 2
Spectroscopic studies of atomic defects and bandgap renormalization in semiconducting monolayer transition metal dichalcogenides
journal, August 2019
- Jeong, Tae Young; Kim, Hakseong; Choi, Sang-Jun
- Nature Communications, Vol. 10, Issue 1
Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment
journal, November 2015
- Kylänpää, Ilkka; Komsa, Hannu-Pekka
- Physical Review B, Vol. 92, Issue 20
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012
- Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
- Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
2D transition metal dichalcogenides
journal, June 2017
- Manzeli, Sajedeh; Ovchinnikov, Dmitry; Pasquier, Diego
- Nature Reviews Materials, Vol. 2, Issue 8
Optically Discriminating Carrier-Induced Quasiparticle Band Gap and Exciton Energy Renormalization in Monolayer
journal, August 2017
- Yao, Kaiyuan; Yan, Aiming; Kahn, Salman
- Physical Review Letters, Vol. 119, Issue 8
Broadband optical properties of monolayer and bulk MoS2
journal, July 2020
- Ermolaev, Georgy A.; Stebunov, Yury V.; Vyshnevyy, Andrey A.
- npj 2D Materials and Applications, Vol. 4, Issue 1
Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS 2
journal, December 2015
- Pogna, Eva A. A.; Marsili, Margherita; De Fazio, Domenico
- ACS Nano, Vol. 10, Issue 1
Dynamical Shift and Broadening of Core Excitons in Semiconductors
journal, November 1982
- Strinati, G.
- Physical Review Letters, Vol. 49, Issue 20
Slow cooling and efficient extraction of C-exciton hot carriers in MoS2 monolayer
journal, January 2017
- Wang, Lei; Wang, Zhuo; Wang, Hai-Yu
- Nature Communications, Vol. 8, Issue 1
Electrical Tuning of Exciton Binding Energies in Monolayer
journal, September 2015
- Chernikov, Alexey; van der Zande, Arend M.; Hill, Heather M.
- Physical Review Letters, Vol. 115, Issue 12
Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
journal, September 2019
- Goryca, M.; Li, J.; Stier, A. V.
- Nature Communications, Vol. 10, Issue 1
Tightly bound trions in monolayer MoS2
journal, December 2012
- Mak, Kin Fai; He, Keliang; Lee, Changgu
- Nature Materials, Vol. 12, Issue 3
Photoinduced Bandgap Renormalization and Exciton Binding Energy Reduction in WS 2
journal, October 2016
- Cunningham, Paul D.; Hanbicki, Aubrey T.; McCreary, Kathleen M.
- ACS Nano, Vol. 11, Issue 12
Layer-controlled CVD growth of large-area two-dimensional MoS 2 films
journal, January 2015
- Jeon, Jaeho; Jang, Sung Kyu; Jeon, Su Min
- Nanoscale, Vol. 7, Issue 5
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer
journal, August 2014
- Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M.
- Physical Review Letters, Vol. 113, Issue 7
Quasiparticle band structures and optical properties of strained monolayer MoS and WS
journal, April 2013
- Shi, Hongliang; Pan, Hui; Zhang, Yong-Wei
- Physical Review B, Vol. 87, Issue 15
Interplay between many body effects and Coulomb screening in the optical bandgap of atomically thin MoS 2
journal, January 2017
- Park, Youngsin; Han, Sang Wook; Chan, Christopher C. S.
- Nanoscale, Vol. 9, Issue 30
Electron-hole excitations and optical spectra from first principles
journal, August 2000
- Rohlfing, Michael; Louie, Steven G.
- Physical Review B, Vol. 62, Issue 8
Giant excitation induced bandgap renormalization in TMDC monolayers
journal, February 2018
- Meckbach, L.; Stroucken, T.; Koch, S. W.
- Applied Physics Letters, Vol. 112, Issue 6
yambo: An ab initio tool for excited state calculations
journal, August 2009
- Marini, Andrea; Hogan, Conor; Grüning, Myrta
- Computer Physics Communications, Vol. 180, Issue 8