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 »
- Authors:
-
- School of Electrical and Computer Engineering Georgia Institute of Technology Atlanta GA 30332‐0250 USA
- Department of Chemistry Emory University Atlanta GA 30322 USA
- Department of Materials Science and Engineering Texas A&,M University College Station TX 77843 USA
- 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
- 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}
}
https://doi.org/10.1002/smll.201906347
Web of Science
Works referenced in this record:
Multimodal Nonlinear Optical Imaging of MoS 2 and MoS 2 -Based van der Waals Heterostructures
journal, February 2016
- Li, Dawei; Xiong, Wei; Jiang, Lijia
- ACS Nano, Vol. 10, Issue 3
Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014
- Xu, Xiaodong; Yao, Wang; Xiao, Di
- Nature Physics, Vol. 10, Issue 5
Dispersion of bound electron nonlinear refraction in solids
journal, June 1991
- Sheik-Bahae, M.; Hutchings, D. C.; Hagan, D. J.
- IEEE Journal of Quantum Electronics, Vol. 27, Issue 6
Exciton dynamics in atomically thin MoS : Interexcitonic interaction and broadening kinetics
journal, August 2013
- Sim, Sangwan; Park, Jusang; Song, Jeong-Gyu
- Physical Review B, Vol. 88, Issue 7
Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces
journal, May 2017
- Shcherbakov, Maxim R.; Liu, Sheng; Zubyuk, Varvara V.
- Nature Communications, Vol. 8, Issue 1
Resonant Light-Induced Heating in Hybrid Cavity-Coupled 2D Transition-Metal Dichalcogenides
journal, March 2016
- Taghinejad, Hossein; Taghinejad, Mohammad; Tarasov, Alexey
- ACS Photonics, Vol. 3, Issue 4
Dispersion and band-gap scaling of the electronic Kerr effect in solids associated with two-photon absorption
journal, July 1990
- Sheik-Bahae, M.; Hagan, D. J.; Van Stryland, E. W.
- Physical Review Letters, Vol. 65, Issue 1
Charge-Induced Second-Harmonic Generation in Bilayer WSe 2
journal, July 2015
- Yu, Huakang; Talukdar, Deep; Xu, Weigao
- Nano Letters, Vol. 15, Issue 8
Enhanced Nonlinear Refractive Index in -Near-Zero Materials
journal, June 2016
- Caspani, L.; Kaipurath, R. P. M.; Clerici, M.
- Physical Review Letters, Vol. 116, Issue 23
Ultrafast Electron Dynamics and Optical Nonlinearities in Metal Nanoparticles
journal, March 2001
- Voisin, Christophe; Del Fatti, Natalia; Christofilos, Dimitris
- The Journal of Physical Chemistry B, Vol. 105, Issue 12
Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region
journal, April 2016
- Alam, M. Z.; De Leon, I.; Boyd, R. W.
- Science, Vol. 352, Issue 6287
A Nickel–Gold Bilayer Catalyst Engineering Technique for Self-Assembled Growth of Highly Ordered Silicon Nanotubes (SiNT)
journal, February 2013
- Taghinejad, M.; Taghinejad, H.; Abdolahad, M.
- Nano Letters, Vol. 13, Issue 3
All-optical control of light on a silicon chip
journal, October 2004
- Almeida, Vilson R.; Barrios, Carlos A.; Panepucci, Roberto R.
- Nature, Vol. 431, Issue 7012
Transient Second-Order Nonlinear Media: Breaking the Spatial Symmetry in the Time Domain via Hot-Electron Transfer
journal, January 2020
- Taghinejad, Mohammad; Xu, Zihao; Lee, Kyu-Tae
- Physical Review Letters, Vol. 124, Issue 1
2D Materials for Optical Modulation: Challenges and Opportunities
journal, February 2017
- Yu, Shaoliang; Wu, Xiaoqin; Wang, Yipei
- Advanced Materials, Vol. 29, Issue 14
All-optical materials design of chiral edge modes in transition-metal dichalcogenides
journal, October 2016
- Claassen, Martin; Jia, Chunjing; Moritz, Brian
- Nature Communications, Vol. 7, Issue 1
Hot-Electron-Assisted Femtosecond All-Optical Modulation in Plasmonics
journal, January 2018
- Taghinejad, Mohammad; Taghinejad, Hossein; Xu, Zihao
- Advanced Materials, Vol. 30, Issue 9
All-optical switching in a liquid crystalline waveguide
journal, January 2005
- Fratalocchi, Andrea; Assanto, Gaetano
- Applied Physics Letters, Vol. 86, Issue 5
Ultrafast optical switching of infrared plasmon polaritons in high-mobility graphene
journal, March 2016
- Ni, G. X.; Wang, L.; Goldflam, M. D.
- Nature Photonics, Vol. 10, Issue 4
Facile fabrication of wafer-scale MoS 2 neat films with enhanced third-order nonlinear optical performance
journal, January 2015
- Zhang, Xiaoyan; Zhang, Saifeng; Chang, Chunxia
- Nanoscale, Vol. 7, Issue 7
Energy band-gap dependence of two-photon absorption
journal, January 1985
- Van Stryland, Eric W.; Woodall, M. A.; Vanherzeele, H.
- Optics Letters, Vol. 10, Issue 10
Ultrafast Control of Phase and Polarization of Light Expedited by Hot-Electron Transfer
journal, August 2018
- Taghinejad, Mohammad; Taghinejad, Hossein; Xu, Zihao
- Nano Letters, Vol. 18, Issue 9
Inductive Tuning of Fano-Resonant Metasurfaces Using Plasmonic Response of Graphene in the Mid-Infrared
journal, February 2013
- Mousavi, S. Hossein; Kholmanov, Iskandar; Alici, Kamil B.
- Nano Letters, Vol. 13, Issue 3
Observation of intense second harmonic generation from MoS atomic crystals
journal, May 2013
- Malard, Leandro M.; Alencar, Thonimar V.; Barboza, Ana Paula M.
- Physical Review B, Vol. 87, Issue 20
All-Optical Control of Light in Micro- and Nanophotonics
journal, April 2019
- Taghinejad, Mohammad; Cai, Wenshan
- ACS Photonics, Vol. 6, Issue 5
Exciton Dynamics in Suspended Monolayer and Few-Layer MoS 2 2D Crystals
journal, January 2013
- Shi, Hongyan; Yan, Rusen; Bertolazzi, Simone
- ACS Nano, Vol. 7, Issue 2
Ultrafast All-Optical Graphene Modulator
journal, January 2014
- Li, Wei; Chen, Bigeng; Meng, Chao
- Nano Letters, Vol. 14, Issue 2
Dispersion of phonon-assisted nonresonant third-order nonlinearities
journal, November 2003
- Dinu, M.
- IEEE Journal of Quantum Electronics, Vol. 39, Issue 11
Lateral and vertical heterostructures in two-dimensional transition-metal dichalcogenides [Invited]
journal, January 2019
- Taghinejad, Hossein; Eftekhar, Ali A.; Adibi, Ali
- Optical Materials Express, Vol. 9, Issue 4
Active nanoplasmonic metamaterials
journal, June 2012
- Hess, O.; Pendry, J. B.; Maier, S. A.
- Nature Materials, Vol. 11, Issue 7
Large optical nonlinearity of ITO nanorods for sub-picosecond all-optical modulation of the full-visible spectrum
journal, September 2016
- Guo, Peijun; Schaller, Richard D.; Ocola, Leonidas E.
- Nature Communications, Vol. 7, Issue 1
Giant Enhancement of the Optical Second-Harmonic Emission of Monolayers by Laser Excitation at Exciton Resonances
journal, March 2015
- Wang, G.; Marie, X.; Gerber, I.
- Physical Review Letters, Vol. 114, Issue 9
Ultrafast nonlinear all-optical processes in silicon-on-insulator waveguides
journal, June 2007
- Dekker, R.; Usechak, N.; Först, M.
- Journal of Physics D: Applied Physics, Vol. 40, Issue 14
Sub-femtojoule all-optical switching using a photonic-crystal nanocavity
journal, May 2010
- Nozaki, Kengo; Tanabe, Takasumi; Shinya, Akihiko
- Nature Photonics, Vol. 4, Issue 7
2D transition metal dichalcogenides
journal, June 2017
- Manzeli, Sajedeh; Ovchinnikov, Dmitry; Pasquier, Diego
- Nature Reviews Materials, Vol. 2, Issue 8
Tunable nonlinear refractive index of two-dimensional MoS_2, WS_2, and MoSe_2 nanosheet dispersions [Invited]
journal, January 2015
- Wang, Gaozhong; Zhang, Saifeng; Zhang, Xiaoyan
- Photonics Research, Vol. 3, Issue 2
All-optical high-speed signal processing with silicon–organic hybrid slot waveguides
journal, March 2009
- Koos, C.; Vorreau, P.; Vallaitis, T.
- Nature Photonics, Vol. 3, Issue 4
Nonlinear optical effects in epsilon-near-zero media
journal, June 2019
- Reshef, Orad; De Leon, Israel; Alam, M. Zahirul
- Nature Reviews Materials, Vol. 4, Issue 8
Defect-Mediated Alloying of Monolayer Transition-Metal Dichalcogenides
journal, November 2018
- Taghinejad, Hossein; Rehn, Daniel A.; Muccianti, Christine
- ACS Nano, Vol. 12, Issue 12
Optical modulators with 2D layered materials
journal, March 2016
- Sun, Zhipei; Martinez, Amos; Wang, Feng
- Nature Photonics, Vol. 10, Issue 4
Ultrafast switching of tunable infrared plasmons in indium tin oxide nanorod arrays with large absolute amplitude
journal, February 2016
- Guo, Peijun; Schaller, Richard D.; Ketterson, John B.
- Nature Photonics, Vol. 10, Issue 4
Carrier-induced change in refractive index of InP, GaAs and InGaAsP
journal, January 1990
- Bennett, B. R.; Soref, R. A.; Del Alamo, J. A.
- IEEE Journal of Quantum Electronics, Vol. 26, Issue 1
Nonequilibrium electron dynamics in noble metals
journal, June 2000
- Del Fatti, N.; Voisin, C.; Achermann, M.
- Physical Review B, Vol. 61, Issue 24
Inducing and probing non-thermal transitions in semiconductors using femtosecond laser pulses
journal, December 2002
- Sundaram, S. K.; Mazur, E.
- Nature Materials, Vol. 1, Issue 4
Valleytronics in 2D materials
journal, August 2016
- Schaibley, John R.; Yu, Hongyi; Clark, Genevieve
- Nature Reviews Materials, Vol. 1, Issue 11
Strain relaxation via formation of cracks in compositionally modulated two-dimensional semiconductor alloys
journal, April 2018
- Taghinejad, Hossein; Eftekhar, Ali A.; Campbell, Philip M.
- npj 2D Materials and Applications, Vol. 2, Issue 1
Transient SHG Imaging on Ultrafast Carrier Dynamics of MoS 2 Nanosheets
journal, February 2018
- Jang, Houk; Dhakal, Krishna P.; Joo, Kyung-Il
- Advanced Materials, Vol. 30, Issue 14
Atomic-Layer Graphene as a Saturable Absorber for Ultrafast Pulsed Lasers
journal, October 2009
- Bao, Qiaoliang; Zhang, Han; Wang, Yu
- Advanced Functional Materials, Vol. 19, Issue 19