期刊
NANO LETTERS
卷 21, 期 14, 页码 6171-6178出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01786
关键词
ultrafast electron diffraction; first-principles calculations; layered materials; black phosphorus; electron-phonon coupling
类别
资金
- Max Planck Society
- European Research Council (ERC) under the European Union [ERC-2015-CoG-682843]
- Deutsche Forschungsgemeinschaft (DFG) [182087777 -SFB 951]
- DFG [443988403]
- Swiss National Science Foundation [P2SKP2 184100]
- SinoGerman (CSC-DAAD) Postdoc Scholarship Program [57343410]
- DFG within the Emmy Noether program [RE 3977/1]
- Research Unit of Nanostructured Materials Systems (RUNMS)
- program META.I.AKTOP
By combining experiments and theory, we have identified highly anisotropic electron-phonon scattering processes as the primary driving force of nonequilibrium lattice dynamics in black phosphorus and developed an approach to reproduce experimental features. This method could be extended to other nonequilibrium phenomena involving coupled electron-phonon dynamics.
We combine ultrafast electron diffuse scattering experiments and first-principles calculations of the coupled electron-phonon dynamics to provide a detailed momentum-resolved picture of lattice thermalization in black phosphorus. The measurements reveal the emergence of highly anisotropic nonthermal phonon populations persisting for several picoseconds after exciting the electrons with a light pulse. Ultrafast dynamics simulations based on the time-dependent Boltzmann formalism are supplemented by calculations of the structure factor, defining an approach to reproduce the experimental signatures of nonequilibrium structural dynamics. The combination of experiments and theory enables us to identify highly anisotropic electron-phonon scattering processes as the primary driving force of the nonequilibrium lattice dynamics in black phosphorus. Our approach paves the way toward unravelling and controlling microscopic energy flows in two-dimensional materials and van der Waals heterostructures, and may be extended to other nonequilibrium phenomena involving coupled electron-phonon dynamics such as superconductivity, phase transitions, or polaron physics.
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