Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor
Abstract
Isotope effects have received increasing attention in materials science and engineering because altering isotopes directly affects phonons, which can affect both thermal properties and optoelectronic properties of conventional semiconductors. However, how isotopic mass affects the optoelectronic properties in 2D semiconductors remains unclear because of measurement uncertainties resulting from sample heterogeneities. Here, we report an anomalous optical bandgap energy red shift of 13 (±7) milli–electron volts as mass of Mo isotopes is increased in laterally structured 100MoS2-92MoS2 monolayers grown by a two-step chemical vapor deposition that mitigates the effects of heterogeneities. This trend, which is opposite to that observed in conventional semiconductors, is explained by many-body perturbation and time-dependent density functional theories that reveal unusually large exciton binding energy renormalizations exceeding the ground-state renormalization energy due to strong coupling between confined excitons and phonons. The isotope effect on the optical bandgap reported here provides perspective on the important role of exciton-phonon coupling in the physical properties of two-dimensional materials.
- Authors:
-
[1];
[2];
[3];
[3];
[3];
[2];
[3];
[3];
[3];
[2];
[3];
[3]
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Wuhan Univ. (China)
- Univ. of Central Florida, Orlando, FL (United States)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 2317786
- Grant/Contract Number:
- AC05-00OR22725; FG02-07ER46354; 62204176
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 8; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Yu, Yiling, Turkowski, Volodymyr, Hachtel, Jordan A., Puretzky, Alexander A., Ievlev, Anton V., Din, Naseem U., Harris, Sumner B., Iyer, Vasudevan, Rouleau, Christopher M., Rahman, Talat S., Geohegan, David B., and Xiao, Kai. Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor. United States: N. p., 2024.
Web. doi:10.1126/sciadv.adj0758.
Yu, Yiling, Turkowski, Volodymyr, Hachtel, Jordan A., Puretzky, Alexander A., Ievlev, Anton V., Din, Naseem U., Harris, Sumner B., Iyer, Vasudevan, Rouleau, Christopher M., Rahman, Talat S., Geohegan, David B., & Xiao, Kai. Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor. United States. https://doi.org/10.1126/sciadv.adj0758
Yu, Yiling, Turkowski, Volodymyr, Hachtel, Jordan A., Puretzky, Alexander A., Ievlev, Anton V., Din, Naseem U., Harris, Sumner B., Iyer, Vasudevan, Rouleau, Christopher M., Rahman, Talat S., Geohegan, David B., and Xiao, Kai. Wed .
"Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor". United States. https://doi.org/10.1126/sciadv.adj0758. https://www.osti.gov/servlets/purl/2317786.
@article{osti_2317786,
title = {Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor},
author = {Yu, Yiling and Turkowski, Volodymyr and Hachtel, Jordan A. and Puretzky, Alexander A. and Ievlev, Anton V. and Din, Naseem U. and Harris, Sumner B. and Iyer, Vasudevan and Rouleau, Christopher M. and Rahman, Talat S. and Geohegan, David B. and Xiao, Kai},
abstractNote = {Isotope effects have received increasing attention in materials science and engineering because altering isotopes directly affects phonons, which can affect both thermal properties and optoelectronic properties of conventional semiconductors. However, how isotopic mass affects the optoelectronic properties in 2D semiconductors remains unclear because of measurement uncertainties resulting from sample heterogeneities. Here, we report an anomalous optical bandgap energy red shift of 13 (±7) milli–electron volts as mass of Mo isotopes is increased in laterally structured 100MoS2-92MoS2 monolayers grown by a two-step chemical vapor deposition that mitigates the effects of heterogeneities. This trend, which is opposite to that observed in conventional semiconductors, is explained by many-body perturbation and time-dependent density functional theories that reveal unusually large exciton binding energy renormalizations exceeding the ground-state renormalization energy due to strong coupling between confined excitons and phonons. The isotope effect on the optical bandgap reported here provides perspective on the important role of exciton-phonon coupling in the physical properties of two-dimensional materials.},
doi = {10.1126/sciadv.adj0758},
journal = {Science Advances},
number = 8,
volume = 10,
place = {United States},
year = {Wed Feb 21 00:00:00 EST 2024},
month = {Wed Feb 21 00:00:00 EST 2024}
}
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