Enhancement of Exciton–Phonon Scattering from Monolayer to Bilayer WS2
Abstract
Layered transition metal dichalcogenides exhibit the emergence of a direct bandgap at the monolayer limit along with pronounced excitonic effects. In these materials, interaction with phonons is the dominant mechanism that limits the exciton coherence lifetime. Exciton-phonon interaction also facilitates energy and momentum relaxation, and influences exciton diffusion under most experimental conditions. However, the fundamental changes in the exciton–phonon interaction are not well understood as the material undergoes the transition from a direct to an indirect bandgap semiconductor. Here, we address this question through optical spectroscopy and microscopic theory. In the experiment, we study room-temperature statistics of the exciton line width for a large number of mono- and bilayer WS2 samples. We observe a systematic increase in the room-temperature line width of the bilayer compared to the monolayer of 50 meV, corresponding to an additional scattering rate of ~0.1 fs–1. We further address both phonon emission and absorption processes by examining the temperature dependence of the width of the exciton resonances. Using a theoretical approach based on many-body formalism, we are able to explain the experimental results and establish a microscopic framework for exciton–phonon interactions that can be applied to naturally occurring and artificially prepared multilayer structures.
- Authors:
-
[1];
[2];
[5];
[4];
[6];
- Kavli Energy NanoScience Institute, Berkeley, CA (United States); Stanford Univ., Stanford, CA (United States)
- Technical Univ. of Berlin, Berlin (Germany)
- Chalmers Univ. of Technology, Gothenburg (Sweden)
- Columbia Univ., New York, NY (United States)
- Stanford Univ., Stanford, CA (United States); Columbia Univ., New York, NY (United States)
- Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Univ. of Regensburg, Regensburg (Germany)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1490978
- Grant/Contract Number:
- AC02-76SF00515; SFB 1277; SFB 787; SFB 951; CH 1672/1-1; DGE-1069240; DGE1144155; 696656
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 18; Journal Issue: 10; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; 2D materials; excitons; exciton−phonon interaction; scattering lifetime
Citation Formats
Raja, Archana, Selig, Malte, Berghäuser, Gunnar, Yu, Jaeeun, Hill, Heather M., Rigosi, Albert F., Brus, Louis E., Knorr, Andreas, Heinz, Tony F., Malic, Ermin, and Chernikov, Alexey. Enhancement of Exciton–Phonon Scattering from Monolayer to Bilayer WS2. United States: N. p., 2018.
Web. doi:10.1021/acs.nanolett.8b01793.
Raja, Archana, Selig, Malte, Berghäuser, Gunnar, Yu, Jaeeun, Hill, Heather M., Rigosi, Albert F., Brus, Louis E., Knorr, Andreas, Heinz, Tony F., Malic, Ermin, & Chernikov, Alexey. Enhancement of Exciton–Phonon Scattering from Monolayer to Bilayer WS2. United States. https://doi.org/10.1021/acs.nanolett.8b01793
Raja, Archana, Selig, Malte, Berghäuser, Gunnar, Yu, Jaeeun, Hill, Heather M., Rigosi, Albert F., Brus, Louis E., Knorr, Andreas, Heinz, Tony F., Malic, Ermin, and Chernikov, Alexey. Fri .
"Enhancement of Exciton–Phonon Scattering from Monolayer to Bilayer WS2". United States. https://doi.org/10.1021/acs.nanolett.8b01793. https://www.osti.gov/servlets/purl/1490978.
@article{osti_1490978,
title = {Enhancement of Exciton–Phonon Scattering from Monolayer to Bilayer WS2},
author = {Raja, Archana and Selig, Malte and Berghäuser, Gunnar and Yu, Jaeeun and Hill, Heather M. and Rigosi, Albert F. and Brus, Louis E. and Knorr, Andreas and Heinz, Tony F. and Malic, Ermin and Chernikov, Alexey},
abstractNote = {Layered transition metal dichalcogenides exhibit the emergence of a direct bandgap at the monolayer limit along with pronounced excitonic effects. In these materials, interaction with phonons is the dominant mechanism that limits the exciton coherence lifetime. Exciton-phonon interaction also facilitates energy and momentum relaxation, and influences exciton diffusion under most experimental conditions. However, the fundamental changes in the exciton–phonon interaction are not well understood as the material undergoes the transition from a direct to an indirect bandgap semiconductor. Here, we address this question through optical spectroscopy and microscopic theory. In the experiment, we study room-temperature statistics of the exciton line width for a large number of mono- and bilayer WS2 samples. We observe a systematic increase in the room-temperature line width of the bilayer compared to the monolayer of 50 meV, corresponding to an additional scattering rate of ~0.1 fs–1. We further address both phonon emission and absorption processes by examining the temperature dependence of the width of the exciton resonances. Using a theoretical approach based on many-body formalism, we are able to explain the experimental results and establish a microscopic framework for exciton–phonon interactions that can be applied to naturally occurring and artificially prepared multilayer structures.},
doi = {10.1021/acs.nanolett.8b01793},
journal = {Nano Letters},
number = 10,
volume = 18,
place = {United States},
year = {Fri Aug 10 00:00:00 EDT 2018},
month = {Fri Aug 10 00:00:00 EDT 2018}
}
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