Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel

Maldonado, P.; Chase, T.; Reid, A. H.; Shen, X.; Li, R. K.; Carva, K.; Payer, T.; Horn von Hoegen, M.; Sokolowski-Tinten, K.; Wang, X. J.; Oppeneer, P. M.; Dürr, H. A.

doi:10.1103/physrevb.101.100302

Title: Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel

Journal Article · 01 March 2020 · Physical Review. B

DOI: https://doi.org/10.1103/physrevb.101.100302 · OSTI ID:1604496

^[1]; Chase, T. ^[2]; Reid, A. H. ^[3]; Shen, X. ^[3]; Li, R. K. ^[3]; Carva, K. ^[4]; Payer, T. ^[5];

^[5]; Sokolowski-Tinten, K. ^[5]; Wang, X. J. ^[3];

^[1];

^[6]

Uppsala Univ. (Sweden)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). Dept. of Applied Physics
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Charles Univ., Prague (Czech Republic). Faculty of Mathematics and Physics
Univ. of Duisburg-Essen (Germany). Dept. of Physics and Center for Nanointegration Duisburg-Essen (CENIDE)
Uppsala Univ. (Sweden); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Femtosecond laser excitation of solid-state systems creates out-of-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering, we gain a detailed understanding of the complex nonequilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wave-vector-resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy, a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond time scale. We determine the evolving nonequilibrium phonon occupations, which we find to deviate markedly from thermal occupations.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: 2015.0060; 737709; 15–08740Y; AC02-05-CH11231; AC02-76SF00515; 278162697-SFB 1242

OSTI ID:: 1604496

Alternate ID(s):: OSTI ID: 1608315

Journal Information:: Physical Review. B, Vol. 101, Issue 10; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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Title: Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel

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