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Title: Ultrafast non-radiative dynamics of atomically thin MoSe 2

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, MoSe 2. 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 carriermore » 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 MoSe 2 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.« less

Authors:
 [1];  [2];  [3];  [3];  [1];  [4];  [2];  [2];  [2];  [4];  [4];  [3];  [2];  [3];  [3];  [5];  [4];  [6];  [7]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS), Stanford PULSE Inst.
  2. Rice Univ., Houston, TX (United States). Dept. of Materials Science and NanoEngineering
  3. Univ. of Southern California, Los Angeles, CA (United States). Collaboratory for Advanced Computing and Simulations
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Kumamoto Univ. (Japan). Dept. of Physics
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); 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, 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, 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. doi:10.1038/s41467-017-01844-2.
Lin, Ming -Fu, Kochat, Vidya, Krishnamoorthy, Aravind, Bassman, 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. doi: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, 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 = {2017},
month = {10}
}

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Works referenced in this record:

Surface Recombination Limited Lifetimes of Photoexcited Carriers in Few-Layer Transition Metal Dichalcogenide MoS 2
journal, November 2015


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
  • DOI: 10.1021/acsnano.6b01149

Phonon-phonon interactions in photoexcited graphite studied by ultrafast electron diffraction
journal, March 2016


Exciton-exciton annihilation in MoSe 2 monolayers
journal, March 2014


Fast exciton annihilation by capture of electrons or holes by defects via Auger scattering in monolayer metal dichalcogenides
journal, April 2015


Bandgap opening in few-layered monoclinic MoTe2
journal, May 2015

  • Keum, Dong Hoon; Cho, Suyeon; Kim, Jung Ho
  • Nature Physics, Vol. 11, Issue 6
  • DOI: 10.1038/nphys3314

Population inversion and giant bandgap renormalization in atomically thin WS2 layers
journal, June 2015


Strongly enhanced superconductivity in doped monolayer MoS 2 by strain
journal, July 2016


Fundamental limits of exciton-exciton annihilation for light emission in transition metal dichalcogenide monolayers
journal, May 2016


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
  • DOI: 10.1021/nl500595u

Coherent and Incoherent Electron-Phonon Coupling in Graphite Observed with Radio-Frequency Compressed Ultrafast Electron Diffraction
journal, December 2014


Two bounds on the maximum phonon-mediated superconducting transition temperature
journal, September 2006


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
  • DOI: 10.1021/nl5021975

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
  • DOI: 10.1021/nn504760x

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
  • DOI: 10.1038/nature01490

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
  • DOI: 10.1021/acs.jpcc.5b07495

Atomically Thin MoS2 A New Direct-Gap Semiconductor
journal, September 2010


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
  • DOI: 10.1021/nl501612v

Near-unity photoluminescence quantum yield in MoS2
journal, November 2015


Symmetry-dependent phonon renormalization in monolayer MoS 2 transistor
journal, April 2012


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
  • DOI: 10.1063/1.4768218

The Role of Electronic and Phononic Excitation in the Optical Response of Monolayer WS 2 after Ultrafast Excitation
journal, January 2017


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
  • DOI: 10.1021/nl503636c

Superconductivity and Phonon Softening
journal, December 1972


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
  • DOI: 10.1038/nmat4061

Hot electron relaxation and phonon dynamics in graphene
journal, November 2007

  • Butscher, S.; Milde, F.; Hirtschulz, M.
  • Applied Physics Letters, Vol. 91, Issue 20
  • DOI: 10.1063/1.2809413

Electronic acceleration of atomic motions and disordering in bismuth
journal, March 2009

  • Sciaini, Germán; Harb, Maher; Kruglik, Sergei G.
  • Nature, Vol. 458, Issue 7234
  • DOI: 10.1038/nature07788

Screening and many-body effects in two-dimensional crystals: Monolayer MoS 2
journal, June 2016


Atomic-Scale Visualization of Inertial Dynamics
journal, April 2005


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
  • DOI: 10.1038/nnano.2012.193

Strain dependence of band gaps and exciton energies in pure and mixed transition-metal dichalcogenides
journal, October 2016


The crystal structure of MoSe2
journal, November 1963


Observation of Structural Anisotropy and the Onset of Liquidlike Motion During the Nonthermal Melting of InSb
journal, September 2005


A better approximation to the Debye-Waller factor
journal, September 1970


First principles phonon calculations in materials science
journal, November 2015


Low-temperature heat capacities of molybdenum diselenide and ditelluride
journal, July 1975


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
  • DOI: 10.1063/1.3530801

Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction
journal, September 2015


Electronic excitation-induced semiconductor-to-metal transition in monolayer MoTe 2
journal, September 2016


Photoluminescence Enhancement and Structure Repairing of Monolayer MoSe 2 by Hydrohalic Acid Treatment
journal, December 2015


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
  • DOI: 10.1063/1.4926994

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
  • DOI: 10.1039/C4NR02634A

Ultra-low power threshold for laser induced changes in optical properties of 2D molybdenum dichalcogenides
journal, October 2016


Δ self-consistent field method to obtain potential energy surfaces of excited molecules on surfaces
journal, August 2008


Valleytronics in 2D materials
journal, August 2016


Mechanisms for Ultrafast Nonradiative Relaxation in Electronically Excited Eumelanin Constituents
journal, November 2008


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
  • DOI: 10.1063/1.4869342