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000866227 0247_ $$2doi$$a10.1103/PhysRevB.100.174301
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000866227 1001_ $$0P:(DE-HGF)0$$aRothenbach, N.$$b0$$eFirst author
000866227 245__ $$aMicroscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure
000866227 260__ $$aWoodbury, NY$$bInst.$$c2019
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000866227 520__ $$aThe element specificity of soft x-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]n as a model system, we perform ultraviolet pump/soft x-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or nonlocal relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L3 absorption edge and relax within 1 ps by electron-phonon coupling, soft x-ray analysis identifies a change at the oxygen K absorption edge of the MgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, nonthermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L3 edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with nonequilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these nonlocal, nonequilibrium dynamics.
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000866227 7001_ $$0P:(DE-HGF)0$$aGruner, M. E.$$b1
000866227 7001_ $$0P:(DE-HGF)0$$aOllefs, K.$$b2
000866227 7001_ $$0P:(DE-Juel1)162347$$aSchmitz-Antoniak, C.$$b3
000866227 7001_ $$0P:(DE-HGF)0$$aSalamon, S.$$b4
000866227 7001_ $$0P:(DE-HGF)0$$aZhou, P.$$b5
000866227 7001_ $$0P:(DE-HGF)0$$aLi, R.$$b6
000866227 7001_ $$0P:(DE-HGF)0$$aMo, M.$$b7
000866227 7001_ $$0P:(DE-HGF)0$$aPark, S.$$b8
000866227 7001_ $$0P:(DE-HGF)0$$aShen, X.$$b9
000866227 7001_ $$0P:(DE-HGF)0$$aWeathersby, S.$$b10
000866227 7001_ $$0P:(DE-HGF)0$$aYang, J.$$b11
000866227 7001_ $$0P:(DE-HGF)0$$aWang, X. J.$$b12
000866227 7001_ $$0P:(DE-HGF)0$$aPentcheva, R.$$b13
000866227 7001_ $$0P:(DE-HGF)0$$aWende, H.$$b14
000866227 7001_ $$0P:(DE-HGF)0$$aBovensiepen, U.$$b15$$eCorresponding author
000866227 7001_ $$0P:(DE-HGF)0$$aSokolowski-Tinten, K.$$b16
000866227 7001_ $$0P:(DE-HGF)0$$aEschenlohr, A.$$b17
000866227 773__ $$0PERI:(DE-600)2844160-6$$a10.1103/PhysRevB.100.174301$$gVol. 100, no. 17, p. 174301$$n17$$p174301$$tPhysical review / B$$v100$$x0163-1829$$y2019
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