Ultrafast non-radiative dynamics of atomically thin MoSe2
Abstract
Non-radiative energy dissipation in photoexcited materials and resulting atomic dynamics provide a promising pathway to induce structural phase transitions in two-dimensional materials. However, these dynamics have not been explored in detail thus far because of incomplete understanding of interaction between the electronic and atomic degrees of freedom, and a lack of direct experimental methods to quantify real-time atomic motion and lattice temperature. Here, we explore the ultrafast conversion of photoenergy to lattice vibrations in a model bi-layered semiconductor, molybdenum diselenide, MoSe2. Specifically, we characterize sub-picosecond lattice dynamics initiated by the optical excitation of electronic charge carriers in the high electron-hole plasma density regime. Our results focuses on the first ten picosecond dynamics subsequent to photoexcitation before the onset of heat transfer to the substrate, which occurs on a ~100 picosecond time scale. Photoinduced atomic motion is probed by measuring the time dependent Bragg diffraction of a delayed mega-electronvolt femtosecond electron beam. Transient lattice temperatures are characterized through measurement of Bragg peak intensities and calculation of the Debye-Waller factor (DWF). These measurements show a sub-picosecond decay of Bragg diffraction and a correspondingly rapid rise in lattice temperatures. We estimate a high quantum yield for the conversion of excited charge carrier energymore »
- Authors:
-
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS), Stanford PULSE Inst.
- Rice Univ., Houston, TX (United States). Dept. of Materials Science and NanoEngineering
- Univ. of Southern California, Los Angeles, CA (United States). Collaboratory for Advanced Computing and Simulations
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Kumamoto Univ. (Japan). Dept. of Physics
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
- 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); National Science Foundation (NSF)
- OSTI Identifier:
- 1399583
- Grant/Contract Number:
- AC02-76SF00515; SC00014607; AC02-05CH11231; ACI-1548562
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Lin, Ming -Fu, Kochat, Vidya, Krishnamoorthy, Aravind, Bassman Oftelie, Lindsay, Weninger, Clemens, Zheng, Qiang, Zhang, Xiang, Apte, Amey, Tiwary, Chandra Sekhar, Shen, Xiaozhe, Li, Renkai, Kalia, Rajiv, Ajayan, Pulickel, Nakano, Aiichiro, Vashishta, Priya, Shimojo, Fyuki, Wang, Xijie, Fritz, David M., and Bergmann, Uwe. Ultrafast non-radiative dynamics of atomically thin MoSe2. United States: N. p., 2017.
Web. doi:10.1038/s41467-017-01844-2.
Lin, Ming -Fu, Kochat, Vidya, Krishnamoorthy, Aravind, Bassman Oftelie, Lindsay, Weninger, Clemens, Zheng, Qiang, Zhang, Xiang, Apte, Amey, Tiwary, Chandra Sekhar, Shen, Xiaozhe, Li, Renkai, Kalia, Rajiv, Ajayan, Pulickel, Nakano, Aiichiro, Vashishta, Priya, Shimojo, Fyuki, Wang, Xijie, Fritz, David M., & Bergmann, Uwe. Ultrafast non-radiative dynamics of atomically thin MoSe2. United States. https://doi.org/10.1038/s41467-017-01844-2
Lin, Ming -Fu, Kochat, Vidya, Krishnamoorthy, Aravind, Bassman Oftelie, Lindsay, Weninger, Clemens, Zheng, Qiang, Zhang, Xiang, Apte, Amey, Tiwary, Chandra Sekhar, Shen, Xiaozhe, Li, Renkai, Kalia, Rajiv, Ajayan, Pulickel, Nakano, Aiichiro, Vashishta, Priya, Shimojo, Fyuki, Wang, Xijie, Fritz, David M., and Bergmann, Uwe. Tue .
"Ultrafast non-radiative dynamics of atomically thin MoSe2". United States. https://doi.org/10.1038/s41467-017-01844-2. https://www.osti.gov/servlets/purl/1399583.
@article{osti_1399583,
title = {Ultrafast non-radiative dynamics of atomically thin MoSe2},
author = {Lin, Ming -Fu and Kochat, Vidya and Krishnamoorthy, Aravind and Bassman Oftelie, Lindsay and Weninger, Clemens and Zheng, Qiang and Zhang, Xiang and Apte, Amey and Tiwary, Chandra Sekhar and Shen, Xiaozhe and Li, Renkai and Kalia, Rajiv and Ajayan, Pulickel and Nakano, Aiichiro and Vashishta, Priya and Shimojo, Fyuki and Wang, Xijie and Fritz, David M. and Bergmann, Uwe},
abstractNote = {Non-radiative energy dissipation in photoexcited materials and resulting atomic dynamics provide a promising pathway to induce structural phase transitions in two-dimensional materials. However, these dynamics have not been explored in detail thus far because of incomplete understanding of interaction between the electronic and atomic degrees of freedom, and a lack of direct experimental methods to quantify real-time atomic motion and lattice temperature. Here, we explore the ultrafast conversion of photoenergy to lattice vibrations in a model bi-layered semiconductor, molybdenum diselenide, MoSe2. Specifically, we characterize sub-picosecond lattice dynamics initiated by the optical excitation of electronic charge carriers in the high electron-hole plasma density regime. Our results focuses on the first ten picosecond dynamics subsequent to photoexcitation before the onset of heat transfer to the substrate, which occurs on a ~100 picosecond time scale. Photoinduced atomic motion is probed by measuring the time dependent Bragg diffraction of a delayed mega-electronvolt femtosecond electron beam. Transient lattice temperatures are characterized through measurement of Bragg peak intensities and calculation of the Debye-Waller factor (DWF). These measurements show a sub-picosecond decay of Bragg diffraction and a correspondingly rapid rise in lattice temperatures. We estimate a high quantum yield for the conversion of excited charge carrier energy to lattice motion under our experimental conditions, indicative of a strong electron-phonon interaction. First principles nonadiabatic quantum molecular dynamics simulations (NAQMD) on electronically excited MoSe2 bilayers reproduce the observed picosecond-scale increase in lattice temperature and ultrafast conversion of photoenergy to lattice vibrations. Calculation of excited-state phonon dispersion curves suggests that softened vibrational modes in the excited state are involved in efficient and rapid energy transfer between the electronic system and the lattice.},
doi = {10.1038/s41467-017-01844-2},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {Tue Oct 17 00:00:00 EDT 2017},
month = {Tue Oct 17 00:00:00 EDT 2017}
}
Web of Science
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
Strain Engineering for Transition Metal Dichalcogenides Based Field Effect Transistors
journal, April 2016
- Shen, Tingting; Penumatcha, Ashish V.; Appenzeller, Joerg
- ACS Nano, Vol. 10, Issue 4
Phonon-phonon interactions in photoexcited graphite studied by ultrafast electron diffraction
journal, March 2016
- Harb, M.; Enquist, H.; Jurgilaitis, A.
- Physical Review B, Vol. 93, Issue 10
Exciton-exciton annihilation in MoSe monolayers
journal, March 2014
- Kumar, Nardeep; Cui, Qiannan; Ceballos, Frank
- Physical Review B, Vol. 89, Issue 12
Fast exciton annihilation by capture of electrons or holes by defects via Auger scattering in monolayer metal dichalcogenides
journal, April 2015
- Wang, Haining; Strait, Jared H.; Zhang, Changjian
- Physical Review B, Vol. 91, Issue 16
Bandgap opening in few-layered monoclinic MoTe2
journal, May 2015
- Keum, Dong Hoon; Cho, Suyeon; Kim, Jung Ho
- Nature Physics, Vol. 11, Issue 6
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
Strongly enhanced superconductivity in doped monolayer by strain
journal, July 2016
- Zeng, Shuming; Zhao, Yinchang; Li, Geng
- Physical Review B, Vol. 94, Issue 2
Fundamental limits of exciton-exciton annihilation for light emission in transition metal dichalcogenide monolayers
journal, May 2016
- Yu, Yiling; Yu, Yifei; Xu, Chao
- Physical Review B, Vol. 93, Issue 20
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
Coherent and Incoherent Electron-Phonon Coupling in Graphite Observed with Radio-Frequency Compressed Ultrafast Electron Diffraction
journal, December 2014
- Chatelain, Robert P.; Morrison, Vance R.; Klarenaar, Bart L. M.
- Physical Review Letters, Vol. 113, Issue 23
Two bounds on the maximum phonon-mediated superconducting transition temperature
journal, September 2006
- Moussa, Jonathan E.; Cohen, Marvin L.
- Physical Review B, Vol. 74, Issue 9
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
Ultrafast Carrier Thermalization and Cooling Dynamics in Few-Layer MoS 2
journal, October 2014
- Nie, Zhaogang; Long, Run; Sun, Linfeng
- ACS Nano, Vol. 8, Issue 10
Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit
journal, March 2003
- Sokolowski-Tinten, Klaus; Blome, Christian; Blums, Juris
- Nature, Vol. 422, Issue 6929
Thermally Driven (Mo, W)-(S 2 , Se 2 ) Phonon and Photon Energy Relaxation Dynamics
journal, October 2015
- Liu, Yonghui; Wang, Yan; Bo, Maolin
- The Journal of Physical Chemistry C, Vol. 119, Issue 44
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
Hydrogen-on-Demand Using Metallic Alloy Nanoparticles in Water
journal, June 2014
- Shimamura, Kohei; Shimojo, Fuyuki; Kalia, Rajiv K.
- Nano Letters, Vol. 14, Issue 7
Near-unity photoluminescence quantum yield in MoS2
journal, November 2015
- Amani, M.; Lien, D. -H.; Kiriya, D.
- Science, Vol. 350, Issue 6264
Thickness and strain effects on electronic structures of transition metal dichalcogenides: 2H- semiconductors ( Mo, W; S, Se, Te)
journal, January 2012
- Yun, Won Seok; Han, S. W.; Hong, Soon Cheol
- Physical Review B, Vol. 85, Issue 3
Symmetry-dependent phonon renormalization in monolayer MoS transistor
journal, April 2012
- Chakraborty, Biswanath; Bera, Achintya; Muthu, D. V. S.
- Physical Review B, Vol. 85, Issue 16
Field-effect transistors and intrinsic mobility in ultra-thin MoSe2 layers
journal, November 2012
- Larentis, Stefano; Fallahazad, Babak; Tutuc, Emanuel
- Applied Physics Letters, Vol. 101, Issue 22, Article No. 223104
The Role of Electronic and Phononic Excitation in the Optical Response of Monolayer WS 2 after Ultrafast Excitation
journal, January 2017
- Ruppert, Claudia; Chernikov, Alexey; Hill, Heather M.
- Nano Letters, Vol. 17, Issue 2
Ultrafast Dynamics of Defect-Assisted Electron–Hole Recombination in Monolayer MoS 2
journal, December 2014
- Wang, Haining; Zhang, Changjian; Rana, Farhan
- Nano Letters, Vol. 15, Issue 1
Superconductivity and Phonon Softening
journal, December 1972
- Allen, Philip B.; Cohen, Marvin L.
- Physical Review Letters, Vol. 29, Issue 24
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
Hot electron relaxation and phonon dynamics in graphene
journal, November 2007
- Butscher, S.; Milde, F.; Hirtschulz, M.
- Applied Physics Letters, Vol. 91, Issue 20
Electronic acceleration of atomic motions and disordering in bismuth
journal, March 2009
- Sciaini, Germán; Harb, Maher; Kruglik, Sergei G.
- Nature, Vol. 458, Issue 7234
Screening and many-body effects in two-dimensional crystals: Monolayer
journal, June 2016
- Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.
- Physical Review B, Vol. 93, Issue 23
Atomic-Scale Visualization of Inertial Dynamics
journal, April 2005
- Lindenberg, A. M.
- Science, Vol. 308, Issue 5720
Phonons in Ternary Molybdenum Chalcogenide Superconductors
book, January 1982
- Bader, S. D.; Sinha, S. K.; Schweiss, B. P.
- Topics in Current Physics
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
Strain dependence of band gaps and exciton energies in pure and mixed transition-metal dichalcogenides
journal, October 2016
- Defo, Rodrick Kuate; Fang, Shiang; Shirodkar, Sharmila N.
- Physical Review B, Vol. 94, Issue 15
The crystal structure of MoSe2
journal, November 1963
- James, P. B.; Lavik, M. T.
- Acta Crystallographica, Vol. 16, Issue 11, p. 1183-1183
Observation of Structural Anisotropy and the Onset of Liquidlike Motion During the Nonthermal Melting of InSb
journal, September 2005
- Gaffney, K. J.; Lindenberg, A. M.; Larsson, J.
- Physical Review Letters, Vol. 95, Issue 12
A better approximation to the Debye-Waller factor
journal, September 1970
- Hardy, K. A.; Parker, F. T.; Walker, J. C.
- Nuclear Instruments and Methods, Vol. 86, Issue 1
First principles phonon calculations in materials science
journal, November 2015
- Togo, Atsushi; Tanaka, Isao
- Scripta Materialia, Vol. 108
Low-temperature heat capacities of molybdenum diselenide and ditelluride
journal, July 1975
- Kiwia, Harmas L.; Westrum, Edgar F.
- The Journal of Chemical Thermodynamics, Vol. 7, Issue 7
Assessment of the ΔSCF density functional theory approach for electronic excitations in organic dyes
journal, February 2011
- Kowalczyk, Tim; Yost, Shane R.; Voorhis, Troy Van
- The Journal of Chemical Physics, Vol. 134, Issue 5
Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction
journal, September 2015
- Mannebach, Ehren M.; Li, Renkai; Duerloo, Karel-Alexander
- Nano Letters, Vol. 15, Issue 10
Electronic excitation-induced semiconductor-to-metal transition in monolayer
journal, September 2016
- Kolobov, A. V.; Fons, P.; Tominaga, J.
- Physical Review B, Vol. 94, Issue 9
Photoluminescence Enhancement and Structure Repairing of Monolayer MoSe 2 by Hydrohalic Acid Treatment
journal, December 2015
- Han, Hau-Vei; Lu, Ang-Yu; Lu, Li-Syuan
- ACS Nano, Vol. 10, Issue 1
Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory
journal, July 2015
- Weathersby, S. P.; Brown, G.; Centurion, M.
- Review of Scientific Instruments, Vol. 86, Issue 7
Broadband ultrafast nonlinear absorption and nonlinear refraction of layered molybdenum dichalcogenide semiconductors
journal, January 2014
- Wang, Kangpeng; Feng, Yanyan; Chang, Chunxia
- Nanoscale, Vol. 6, Issue 18
Ultra-low power threshold for laser induced changes in optical properties of 2D molybdenum dichalcogenides
journal, October 2016
- Cadiz, Fabian; Robert, Cedric; Wang, Gang
- 2D Materials, Vol. 3, Issue 4
self-consistent field method to obtain potential energy surfaces of excited molecules on surfaces
journal, August 2008
- Gavnholt, Jeppe; Olsen, Thomas; Engelund, Mads
- Physical Review B, Vol. 78, Issue 7
Valleytronics in 2D materials
journal, August 2016
- Schaibley, John R.; Yu, Hongyi; Clark, Genevieve
- Nature Reviews Materials, Vol. 1, Issue 11
Mechanisms for Ultrafast Nonradiative Relaxation in Electronically Excited Eumelanin Constituents
journal, November 2008
- Meng, Sheng; Kaxiras, Efthimios
- Biophysical Journal, Vol. 95, Issue 9
A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations
journal, May 2014
- Shimojo, Fuyuki; Hattori, Shinnosuke; Kalia, Rajiv K.
- The Journal of Chemical Physics, Vol. 140, Issue 18
Low-temperature heat capacities of molybdenum diselenide and ditelluride
journal, July 1975
- Kiwia, Harmas L.; Westrum, Edgar F.
- The Journal of Chemical Thermodynamics, Vol. 7, Issue 7
Thermally Driven (Mo, W)-(S 2 , Se 2 ) Phonon and Photon Energy Relaxation Dynamics
journal, October 2015
- Liu, Yonghui; Wang, Yan; Bo, Maolin
- The Journal of Physical Chemistry C, Vol. 119, Issue 44
Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction
journal, September 2015
- Mannebach, Ehren M.; Li, Renkai; Duerloo, Karel-Alexander
- Nano Letters, Vol. 15, Issue 10
The Role of Electronic and Phononic Excitation in the Optical Response of Monolayer WS 2 after Ultrafast Excitation
journal, January 2017
- Ruppert, Claudia; Chernikov, Alexey; Hill, Heather M.
- Nano Letters, Vol. 17, Issue 2
Photoluminescence Enhancement and Structure Repairing of Monolayer MoSe 2 by Hydrohalic Acid Treatment
journal, December 2015
- Han, Hau-Vei; Lu, Ang-Yu; Lu, Li-Syuan
- ACS Nano, Vol. 10, Issue 1
Strain Engineering for Transition Metal Dichalcogenides Based Field Effect Transistors
journal, April 2016
- Shen, Tingting; Penumatcha, Ashish V.; Appenzeller, Joerg
- ACS Nano, Vol. 10, Issue 4
Hydrogen-on-Demand Using Metallic Alloy Nanoparticles in Water
journal, June 2014
- Shimamura, Kohei; Shimojo, Fuyuki; Kalia, Rajiv K.
- 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
Ultrafast Carrier Thermalization and Cooling Dynamics in Few-Layer MoS 2
journal, October 2014
- Nie, Zhaogang; Long, Run; Sun, Linfeng
- ACS Nano, Vol. 8, Issue 10
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
(Fe,Ni)2P allabogdanite can be an ambient pressure phase in iron meteorites
journal, June 2020
- Litasov, Konstantin D.; Bekker, Tatyana B.; Sagatov, Nursultan E.
- Scientific Reports, Vol. 10, Issue 1
Hot electron relaxation and phonon dynamics in graphene
journal, November 2007
- Butscher, S.; Milde, F.; Hirtschulz, M.
- Applied Physics Letters, Vol. 91, Issue 20
Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory
journal, July 2015
- Weathersby, S. P.; Brown, G.; Centurion, M.
- Review of Scientific Instruments, Vol. 86, Issue 7
Ultra-low power threshold for laser induced changes in optical properties of 2D molybdenum dichalcogenides
journal, October 2016
- Cadiz, Fabian; Robert, Cedric; Wang, Gang
- 2D Materials, Vol. 3, Issue 4
Near-unity photoluminescence quantum yield in MoS2
journal, November 2015
- Amani, M.; Lien, D. -H.; Kiriya, D.
- Science, Vol. 350, Issue 6264
Mechanisms for Ultrafast Nonradiative Relaxation in Electronically Excited Eumelanin Constituents
journal, November 2008
- Meng, Sheng; Kaxiras, Efthimios
- Biophysical Journal, Vol. 95, Issue 9
Field-effect transistors and intrinsic mobility in ultra-thin MoSe2 layers
text, January 2012
- Larentis, S.; Fallahazad, B.; Tutuc, E.
- arXiv
Coherent and incoherent electron-phonon coupling in graphite observed with radio-frequency compressed ultrafast electron diffraction
text, January 2014
- Chatelain, Robert P.; Morrison, Vance R.; Klarenaar, Bart L. M.
- arXiv
Works referencing / citing this record:
Ultrafast carrier and phonon dynamics in few-layer 2H–MoTe 2
journal, September 2019
- Chi, Zhen; Chen, Hailong; Zhao, Qing
- The Journal of Chemical Physics, Vol. 151, Issue 11
Quantum Dynamics at Scale: Ultrafast Control of Emergent Functional Materials
conference, January 2020
- Tiwari, Subodh C.; Krishnamoorthy, Aravind; Rajak, Pankaj
- HPCAsia2020: International Conference on High Performance Computing in Asia-Pacific Region, Proceedings of the International Conference on High Performance Computing in Asia-Pacific Region
Recent Advances in Ultrafast Structural Techniques
journal, April 2019
- Sciaini, Germán
- Applied Sciences, Vol. 9, Issue 7
The lifetime of interlayer breathing modes of few-layer 2H-MoSe 2 membranes
journal, January 2019
- Soubelet, Pedro; Reynoso, Andrés A.; Fainstein, Alejandro
- Nanoscale, Vol. 11, Issue 21
Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface X-ray scattering
journal, March 2019
- Tung, I-Cheng; Krishnamoorthy, Aravind; Sadasivam, Sridhar
- Nature Photonics, Vol. 13, Issue 6
A THz driven split-ring resonator based ultrafast relativistic electron streak camera
journal, August 2019
- Shen, X. L.; Snively, E. C.; Navarro, J. Giner
- AIP Advances, Vol. 9, Issue 8