Journal Article

PUBDB-2016-03264

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Tailored Pump-Probe Transient Spectroscopy With Time-Dependent Density-Functional Theory: Controlling Absorption Spectra

Walkenhorst, J. (Corresponding author) ; De Giovannini, U. ; Castro, A. ; Rubio, A.CFEL*MPG*

2016
Springer Berlin

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Please use a persistent id in citations: doi:10.1140/epjb/e2016-70064-0

Abstract: Recent advances in laser technology allow us to follow electronic motion at its natural time-scale with ultra-fast time resolution, leading the way towards attosecond physics experiments of extreme precision. In this work, we assess the use of tailored pumps in order to enhance (or reduce) some given features of the probe absorption (for example, absorption in the visible range of otherwise transparent samples). This type of manipulation of the system response could be helpful for its full characterization, since it would allow us to visualize transitions that are dark when using unshaped pulses. In order to investigate these possibilities, we perform first a theoretical analysis of the nmon-equilibrium response function in this context, aided by one simple numerical model of the hydrogen atom. Then, we proceed to investigate the feasibility of using time-dependent density-functional theory as a means to implement, theoretically, this absorption-optimization idea, for more complex atoms or molecules. We conclude that the proposed idea could in principle be brought to the laboratory: tailored pump pulses can excite systems into light-absorbing states. However, we also highlight the severe numerical and theoretical difficulties posed by the problem: large-scale non-equilibrium quantum dynamics are cumbersome, even with TDDFT, and the shortcomingsof state-of-the-art TDDFT functionals may still be serious for these out-of-equilibrium situations.

Note: (c) EDP Sciences, Societa Italiana di Fisica, Springer-Verlag. Post referee full text in progress (embargo 1 year from 15.05.2016).

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Experiment(s):

1. No specific instrument

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Database coverage:
; ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; IF < 5 ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection

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