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  Nonadiabatic and Time-Resolved Photoelectron Spectroscopy for Molecular Systems

Flick, J., Appel, H., & Rubio, A. (2014). Nonadiabatic and Time-Resolved Photoelectron Spectroscopy for Molecular Systems. Journal of Chemical Theory and Computation, 10(4), 1665-1676. doi:10.1021/ct4010933.

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Item Permalink: https://hdl.handle.net/11858/00-001M-0000-0019-1A9C-8 Version Permalink: https://hdl.handle.net/21.11116/0000-0005-407D-7
Genre: Journal Article

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Flick, Johannes1, Author           
Appel, Heiko1, Author           
Rubio, Angel1, 2, Author           
Affiliations:
1Theory, Fritz Haber Institute, Max Planck Society, ou_634547              
2Nano-Bio Spectroscopy Group and ETSF Scientific Development Centre, Departamento de F, ou_persistent22              

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 Abstract: We quantify the nonadiabatic contributions to the vibronic sidebands of equilibrium and explicitly time-resolved nonequilibrium photoelectron spectra for a vibronic model system of trans-polyacetylene. Using exact diagonalization, we directly evaluate the sum-over-states expressions for the linear-response photocurrent. We show that spurious peaks appear in the Born–Oppenheimer approximation for the vibronic spectral function, which are not present in the exact spectral function of the system. The effect can be traced back to the factorized nature of the Born–Oppenheimer initial and final photoemission states and also persists when either only initial or final states are replaced by correlated vibronic states. Only when correlated initial and final vibronic states are taken into account are the spurious spectral weights of the Born–Oppenheimer approximation suppressed. In the nonequilibrium case, we illustrate for an initial Franck–Condon excitation and an explicit pump–pulse excitation how the vibronic wavepacket motion of the system can be traced in the time-resolved photoelectron spectra as a function of the pump–probe delay.

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Language(s): eng - English
 Dates: 2013-12-092014-03-242014-04-08
 Publication Status: Issued
 Pages: 12
 Publishing info: -
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 Rev. Type: Peer
 Identifiers: DOI: 10.1021/ct4010933
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Project name : DYNAMO - Dynamical processes in open quantum systems: pushing the frontiers of theoretical spectroscopy
Grant ID : 267374
Funding program : Funding Programme 7 (FP7)
Funding organization : European Commission (EC)

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Title: Journal of Chemical Theory and Computation
  Other : J. Chem. Theory Comput.
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 10 (4) Sequence Number: - Start / End Page: 1665 - 1676 Identifier: Other: 1549-9618
CoNE: https://pure.mpg.de/cone/journals/resource/111088195283832