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Title: Photocarrier‐Induced Active Control of Second‐Order Optical Nonlinearity in Monolayer MoS 2

Abstract

Abstract Atomically thin transition metal dichalcogenides (TMDs) in their excited states can serve as exceptionally small building blocks for active optical platforms. In this scheme, optical excitation provides a practical approach to control light‐TMD interactions via the photocarrier generation, in an ultrafast manner. Here, it is demonstrated that via a controlled generation of photocarriers the second‐harmonic generation (SHG) from a monolayer MoS 2 crystal can be substantially modulated up to ≈55% within a timeframe of ≈250 fs, a set of performance characteristics that showcases the promise of low‐dimensional materials for all‐optical nonlinear data processing. The combined experimental and theoretical study suggests that the large SHG modulation stems from the correlation between the second‐order dielectric susceptibility χ (2) and the density of photoexcited carriers in MoS 2 . Indeed, the depopulation of the conduction band electrons, at the vicinity of the high‐symmetry K/K′ points of MoS 2 , suppresses the contribution of interband electronic transitions in the effective χ (2) of the monolayer crystal, enabling the all‐optical modulation of the SHG signal. The strong dependence of the second‐order optical response on the density of photocarriers reveals the promise of time‐resolved nonlinear characterization as an alternative route to monitoring carrier dynamics inmore » excited states of TMDs.« less

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [3];  [2]; ORCiD logo [5]
  1. School of Electrical and Computer Engineering Georgia Institute of Technology Atlanta GA 30332‐0250 USA
  2. Department of Chemistry Emory University Atlanta GA 30322 USA
  3. Department of Materials Science and Engineering Texas A&,M University College Station TX 77843 USA
  4. School of Electrical and Computer Engineering Georgia Institute of Technology Atlanta GA 30332‐0250 USA, Toyota Research Institute of North America Ann Arbor MI 48105 USA
  5. School of Electrical and Computer Engineering Georgia Institute of Technology Atlanta GA 30332‐0250 USA, School of Materials Science and Engineering Georgia Institute of Technology Atlanta GA 30332 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1582685
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Name: Small Journal Volume: 16 Journal Issue: 5; Journal ID: ISSN 1613-6810
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Taghinejad, Mohammad, Xu, Zihao, Wang, Hua, Taghinejad, Hossein, Lee, Kyu‐Tae, Rodrigues, Sean P., Adibi, Ali, Qian, Xiaofeng, Lian, Tianquan, and Cai, Wenshan. Photocarrier‐Induced Active Control of Second‐Order Optical Nonlinearity in Monolayer MoS 2. Germany: N. p., 2020. Web. doi:10.1002/smll.201906347.
Taghinejad, Mohammad, Xu, Zihao, Wang, Hua, Taghinejad, Hossein, Lee, Kyu‐Tae, Rodrigues, Sean P., Adibi, Ali, Qian, Xiaofeng, Lian, Tianquan, & Cai, Wenshan. Photocarrier‐Induced Active Control of Second‐Order Optical Nonlinearity in Monolayer MoS 2. Germany. https://doi.org/10.1002/smll.201906347
Taghinejad, Mohammad, Xu, Zihao, Wang, Hua, Taghinejad, Hossein, Lee, Kyu‐Tae, Rodrigues, Sean P., Adibi, Ali, Qian, Xiaofeng, Lian, Tianquan, and Cai, Wenshan. Tue . "Photocarrier‐Induced Active Control of Second‐Order Optical Nonlinearity in Monolayer MoS 2". Germany. https://doi.org/10.1002/smll.201906347.
@article{osti_1582685,
title = {Photocarrier‐Induced Active Control of Second‐Order Optical Nonlinearity in Monolayer MoS 2},
author = {Taghinejad, Mohammad and Xu, Zihao and Wang, Hua and Taghinejad, Hossein and Lee, Kyu‐Tae and Rodrigues, Sean P. and Adibi, Ali and Qian, Xiaofeng and Lian, Tianquan and Cai, Wenshan},
abstractNote = {Abstract Atomically thin transition metal dichalcogenides (TMDs) in their excited states can serve as exceptionally small building blocks for active optical platforms. In this scheme, optical excitation provides a practical approach to control light‐TMD interactions via the photocarrier generation, in an ultrafast manner. Here, it is demonstrated that via a controlled generation of photocarriers the second‐harmonic generation (SHG) from a monolayer MoS 2 crystal can be substantially modulated up to ≈55% within a timeframe of ≈250 fs, a set of performance characteristics that showcases the promise of low‐dimensional materials for all‐optical nonlinear data processing. The combined experimental and theoretical study suggests that the large SHG modulation stems from the correlation between the second‐order dielectric susceptibility χ (2) and the density of photoexcited carriers in MoS 2 . Indeed, the depopulation of the conduction band electrons, at the vicinity of the high‐symmetry K/K′ points of MoS 2 , suppresses the contribution of interband electronic transitions in the effective χ (2) of the monolayer crystal, enabling the all‐optical modulation of the SHG signal. The strong dependence of the second‐order optical response on the density of photocarriers reveals the promise of time‐resolved nonlinear characterization as an alternative route to monitoring carrier dynamics in excited states of TMDs.},
doi = {10.1002/smll.201906347},
journal = {Small},
number = 5,
volume = 16,
place = {Germany},
year = {Tue Jan 14 00:00:00 EST 2020},
month = {Tue Jan 14 00:00:00 EST 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/smll.201906347

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