Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41467-017-01844-2
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Funding
- Computational Materials Sciences Program - U.S. Department of Energy, Office of Science, and Basic Energy Sciences [DE-SC00014607]
- DOE BES SUF Division Accelerator & Detector RD program
- LCLS Facility
- National Science Foundation [ACI-1548562]
- SLAC [DE-AC02-05-CH11231, DE-AC02-76SF00515]
- Grants-in-Aid for Scientific Research [16K05478] Funding Source: KAKEN
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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.
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