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AgAu2.pdf (705.29 kB)
Stochastic Thermodynamics Analysis of Ultrafast AgAu Nanoshell Dynamics in the Nonlinear Response Regime
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submitted on 22.08.2020 and posted on 24.08.2020by Guilherme Ferbonink, Thenner S. Rodrigues, Pedro Camargo, Rodrigo Albuquerque, RENE NOME
The understanding of relaxation dynamics of
metallic nanoshells is important for a range of nanotechnological applications.
In this work, we present a combined experimental-theoretical study of the
relaxation dynamics of AgAu nanoshells. This was investigated using ultrafast
pump-probe experiments resonant with the surface plasmon of the nanoshells, as
well as via atomistic molecular dynamics simulations of relaxation and
temperature-jump (DT-jump) processes. Both
techniques were then discussed and complemented using a non-equilibrium
statistical mechanical model. Data collected at low energies were consistent
with our previously reported work and allowed the characterization of intrinsic
electron-phonon coupling times (EPCT) and of the overall relaxation dynamics in
terms of a two-temperature model. Data at intermediate and higher energies, in
turn, showed a nonlinear dependence of EPCT as a function of the pump power, faster
relaxation being observed at higher pump energies. In the limit of small DT-jumps, relaxation
based on a two-temperature model is recovered, whereas in the limit of large DT-jumps, the
relaxation becomes faster with increasing temperature change. The results
reported here give insight on the ultrafast dynamics of AgAu nanoshells and
might also be applied to other metallic systems, paving the way to the better
understanding of relaxation dynamics of nanoparticles in general.