Ultrafast non-radiative dynamics of atomically thin MoSe2

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

doi:10.1038/s41467-017-01844-2

Title: Ultrafast non-radiative dynamics of atomically thin MoSe₂

Journal Article · Tue Oct 17 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-01844-2· OSTI ID:1399583

Lin, Ming -Fu ^[1]; Kochat, Vidya ^[2]; Krishnamoorthy, Aravind ^[3]; Bassman Oftelie, Lindsay ^[3]; Weninger, Clemens ^[1]; Zheng, Qiang ^[4]; Zhang, Xiang ^[2]; Apte, Amey ^[2]; Tiwary, Chandra Sekhar ^[2]; Shen, Xiaozhe ^[4]; Li, Renkai ^[4]; Kalia, Rajiv ^[3]; Ajayan, Pulickel ^[2]; Nakano, Aiichiro ^[3]; Vashishta, Priya ^[3]; Shimojo, Fyuki ^[5]; Wang, Xijie ^[4]; Fritz, David M. ^[6]; Bergmann, Uwe ^[7]

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.

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515; SC00014607; AC02-05CH11231; ACI-1548562

OSTI ID:: 1399583

Journal Information:: Nature Communications, Vol. 8, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 36 works

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