Ultrafast non-radiative dynamics of atomically thin MoSe2

Ming-Fu Lin, Vidya Kochat, Aravind Krishnamoorthy, Lindsay Bassman Oftelie, Clemens Weninger, Qiang Zheng, Xiang Zhang, Amey Apte, Chandra Sekhar Tiwary, Xiaozhe Shen, Renkai Li, Rajiv Kalia, Pulickel Ajayan, Aiichiro Nakano, Priya Vashishta, Fuyuki Shimojo, Xijie Wang, David M. Fritz and Uwe Bergmann ()
Additional contact information
Ming-Fu Lin: SLAC National Accelerator Laboratory
Vidya Kochat: Rice University
Aravind Krishnamoorthy: Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern California
Lindsay Bassman Oftelie: Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern California
Clemens Weninger: SLAC National Accelerator Laboratory
Qiang Zheng: SLAC National Accelerator Laboratory
Xiang Zhang: Rice University
Amey Apte: Rice University
Chandra Sekhar Tiwary: Rice University
Xiaozhe Shen: SLAC National Accelerator Laboratory
Renkai Li: SLAC National Accelerator Laboratory
Rajiv Kalia: Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern California
Pulickel Ajayan: Rice University
Aiichiro Nakano: Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern California
Priya Vashishta: Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern California
Fuyuki Shimojo: Kumamoto University
Xijie Wang: SLAC National Accelerator Laboratory
David M. Fritz: SLAC National Accelerator Laboratory
Uwe Bergmann: SLAC National Accelerator Laboratory

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract Photo-induced non-radiative energy dissipation is a potential pathway to induce structural-phase transitions in two-dimensional materials. For advancing this field, a quantitative understanding of real-time atomic motion and lattice temperature is required. However, this understanding has been incomplete due to a lack of suitable experimental techniques. Here, we use ultrafast electron diffraction to directly probe the subpicosecond conversion of photoenergy to lattice vibrations in a model bilayered semiconductor, molybdenum diselenide. We find that when creating a high charge carrier density, the energy is efficiently transferred to the lattice within one picosecond. First-principles nonadiabatic quantum molecular dynamics simulations reproduce the observed ultrafast increase in lattice temperature and the corresponding conversion of photoenergy to lattice vibrations. Nonadiabatic quantum simulations further suggest that a softening of vibrational modes in the excited state is involved in efficient and rapid energy transfer between the electronic system and the lattice.

Date: 2017
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DOI: 10.1038/s41467-017-01844-2

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