10.1021/acs.nanolett.9b01179.s001
Aravind Krishnamoorthy
Aravind
Krishnamoorthy
Ming-Fu Lin
Ming-Fu
Lin
Xiang Zhang
Xiang
Zhang
Clemens Weninger
Clemens
Weninger
Ruru Ma
Ruru
Ma
Alexander Britz
Alexander
Britz
Chandra Sekhar Tiwary
Chandra Sekhar
Tiwary
Vidya Kochat
Vidya
Kochat
Amey Apte
Amey
Apte
Jie Yang
Jie
Yang
Suji Park
Suji
Park
Renkai Li
Renkai
Li
Xiaozhe Shen
Xiaozhe
Shen
Xijie Wang
Xijie
Wang
Rajiv Kalia
Rajiv
Kalia
Aiichiro Nakano
Aiichiro
Nakano
Fuyuki Shimojo
Fuyuki
Shimojo
David Fritz
David
Fritz
Uwe Bergmann
Uwe
Bergmann
Pulickel Ajayan
Pulickel
Ajayan
Priya Vashishta
Priya
Vashishta
Optical Control of Non-Equilibrium Phonon Dynamics
American Chemical Society
2019
dynamic
far-from-equilibrium vibration modes
femtosecond mega-electronvolt electron diffraction experiments
phonon populations
non-radiative energy relaxation pathways
Non-Equilibrium Phonon Dynamics
excitation
understanding
electron diffraction patterns
light-induced
2019-06-24 00:00:00
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Optical_Control_of_Non-Equilibrium_Phonon_Dynamics/8411534
The
light-induced selective population of short-lived far-from-equilibrium
vibration modes is a promising approach for controlling ultrafast
and irreversible structural changes in functional nanomaterials. However,
this requires a detailed understanding of the dynamics and evolution
of these phonon modes and their coupling to the excited-state electronic
structure. Here, we combine femtosecond mega-electronvolt electron
diffraction experiments on a prototypical layered material, MoTe<sub>2</sub>, with non-adiabatic quantum molecular dynamics simulations
and <i>ab initio</i> electronic structure calculations to
show how non-radiative energy relaxation pathways for excited electrons
can be tuned by controlling the optical excitation energy. We show
how the dominant intravalley and intervalley scattering mechanisms
for hot and band-edge electrons leads to markedly different transient
phonon populations evident in electron diffraction patterns. This
understanding of how tuning optical excitations affect phonon populations
and atomic motion is critical for efficiently controlling light-induced
structural transitions of optoelectronic devices.