Nonequilibrium Band Occupation and Optical Response of Gold After Ultrafast XUV Excitation

Overview

Journal Sci Rep

Specialty Science

Date 2022 Mar 19

PMID 35304492

Authors

Pascal D Ndione

Sebastian T Weber

Dirk O Gericke

Baerbel Rethfeld

Affiliations

Soon will be listed here.

Abstract

Free electron lasers offer unique properties to study matter in states far from equilibrium as they combine short pulses with a large range of photon energies. In particular, the possibility to excite core states drives new relaxation pathways that, in turn, also change the properties of the optically and chemically active electrons. Here, we present a theoretical model for the dynamics of the nonequilibrium occupation of the different energy bands in solid gold driven by exciting deep core states. The resulting optical response is in excellent agreement with recent measurements and, combined with our model, provides a quantitative benchmark for the description of electron-phonon coupling in strongly driven gold. Focusing on sub-picosecond time scales, we find essential differences between the dynamics induced by XUV and visible light.

Citing Articles

Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model.

Uehlein M, Weber S, Rethfeld B Nanomaterials (Basel). 2022; 12(10).

PMID: 35630877 PMC: 9145585. DOI: 10.3390/nano12101655.

References

Medvedev N, Milov I . Electron-Phonon Coupling and Nonthermal Effects in Gold Nano-Objects at High Electronic Temperatures. Materials (Basel). 2022; 15(14). PMC: 9322629. DOI: 10.3390/ma15144883. View

Mo M, Chen Z, Li R, Dunning M, Witte B, Baldwin J . Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction. Science. 2018; 360(6396):1451-1455. DOI: 10.1126/science.aar2058. View

Chen Z, Curry C, Zhang R, Treffert F, Stojanovic N, Toleikis S . Ultrafast multi-cycle terahertz measurements of the electrical conductivity in strongly excited solids. Nat Commun. 2021; 12(1):1638. PMC: 7977037. DOI: 10.1038/s41467-021-21756-6. View

Cavalleri A, Rini M, Chong H, Fourmaux S, Glover T, Heimann P . Band-selective measurements of electron dynamics in VO2 using femtosecond near-edge x-ray absorption. Phys Rev Lett. 2005; 95(6):067405. DOI: 10.1103/PhysRevLett.95.067405. View

Kraus D, Ravasio A, Gauthier M, Gericke D, Vorberger J, Frydrych S . Nanosecond formation of diamond and lonsdaleite by shock compression of graphite. Nat Commun. 2016; 7:10970. PMC: 4793081. DOI: 10.1038/ncomms10970. View

Sundaram S, Mazur E . Inducing and probing non-thermal transitions in semiconductors using femtosecond laser pulses. Nat Mater. 2003; 1(4):217-24. DOI: 10.1038/nmat767. View

Chapman D, Gericke D . Analysis of Thomson scattering from nonequilibrium plasmas. Phys Rev Lett. 2011; 107(16):165004. DOI: 10.1103/PhysRevLett.107.165004. View

Hurricane O, Callahan D, Casey D, Celliers P, Cerjan C, Dewald E . Fuel gain exceeding unity in an inertially confined fusion implosion. Nature. 2014; 506(7488):343-8. DOI: 10.1038/nature13008. View

Chen Z, Holst B, Kirkwood S, Sametoglu V, Reid M, Tsui Y . Evolution of ac conductivity in nonequilibrium warm dense gold. Phys Rev Lett. 2013; 110(13):135001. DOI: 10.1103/PhysRevLett.110.135001. View

10.

Ernstorfer R, Harb M, Hebeisen C, Sciaini G, Dartigalongue T, Miller R . The formation of warm dense matter: experimental evidence for electronic bond hardening in gold. Science. 2009; 323(5917):1033-7. DOI: 10.1126/science.1162697. View

11.

Siders C, Cavalleri A, Sokolowski-Tinten K, Toth C, Guo T, Kammler M . Detection of nonthermal melting by ultrafast X-ray diffraction. Science. 1999; 286(5443):1340-2. DOI: 10.1126/science.286.5443.1340. View

12.

Guillot T . Interiors of giant planets inside and outside the solar system. Science. 1999; 286(5437):72-7. DOI: 10.1126/science.286.5437.72. View

13.

Ao T, Ping Y, Widmann K, Price D, Lee E, Tam H . Optical properties in nonequilibrium phase transitions. Phys Rev Lett. 2006; 96(5):055001. DOI: 10.1103/PhysRevLett.96.055001. View

14.

Siwick B, R Dwyer J, Jordan R, Miller R . An atomic-level view of melting using femtosecond electron diffraction. Science. 2003; 302(5649):1382-5. DOI: 10.1126/science.1090052. View

15.

Chen Z, Tsui Y, Mo M, Fedosejevs R, Ozaki T, Recoules V . Electron Kinetics Induced by Ultrafast Photoexcitation of Warm Dense Matter in a 30-nm-Thick Foil. Phys Rev Lett. 2021; 127(9):097403. DOI: 10.1103/PhysRevLett.127.097403. View

16.

Heilpern T, Manjare M, Govorov A, Wiederrecht G, Gray S, Harutyunyan H . Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements. Nat Commun. 2018; 9(1):1853. PMC: 5945638. DOI: 10.1038/s41467-018-04289-3. View

17.

Kritcher A, Swift D, Doppner T, Bachmann B, Benedict L, Collins G . A measurement of the equation of state of carbon envelopes of white dwarfs. Nature. 2020; 584(7819):51-54. DOI: 10.1038/s41586-020-2535-y. View

18.

Medvedev N, Zastrau U, Forster E, Gericke D, Rethfeld B . Short-time electron dynamics in aluminum excited by femtosecond extreme ultraviolet radiation. Phys Rev Lett. 2011; 107(16):165003. DOI: 10.1103/PhysRevLett.107.165003. View

19.

Vorberger J, Gericke D, Bornath T, Schlanges M . Energy relaxation in dense, strongly coupled two-temperature plasmas. Phys Rev E Stat Nonlin Soft Matter Phys. 2010; 81(4 Pt 2):046404. DOI: 10.1103/PhysRevE.81.046404. View

20.

Mahieu B, Jourdain N, Ta Phuoc K, Dorchies F, Goddet J, Lifschitz A . Probing warm dense matter using femtosecond X-ray absorption spectroscopy with a laser-produced betatron source. Nat Commun. 2018; 9(1):3276. PMC: 6095895. DOI: 10.1038/s41467-018-05791-4. View