Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine

Westermann T, Manthe U (2012)
The Journal Of Chemical Physics 137(22): 22A509.

Download
Es wurde kein Volltext hochgeladen. Nur Publikationsnachweis!
Zeitschriftenaufsatz | Veröffentlicht | Englisch
Abstract / Bemerkung
Decoherence effects induced by conical intersecting potential energy surfaces are studied employing the correlation-based von Neumann (CvN) entropy which provides a measure of the complexity of the underlying wavefunction. As a prototypical example, the S-0 -> S-2 excitation in pyrazine is investigated. The 24-dimensional wavepacket dynamics calculations presented utilize the multi-layer extension of the multi-configurational time-dependent Hartree (MCTDH) approach. An efficient numerical scheme is introduced which facilitates CvN entropy constrained wavepacket propagation within the multi-layer MCTDH approach. In unconstrained multi-layer MCTDH calculations, the CvN-entropy is found to provide a valuable analytical tool for studying the decoherence phenomena present. Investigating the CvN entropy after the S-0 -> S-2 excitation as a function of time, a clear separation of time scales is obtained. It can be related to the different dynamical phenomena present: the initial transfer from the upper (S-2) to the lower (S-1) adiabatic electronic states rapidly generates vast amounts of CvN-entropy, while the subsequent motion on the anharmonic lower adiabatic potential energy surface only yields a slow increase of the CvN-entropy. Employing CvN-entropy constrained calculations, the sensitivity of the autocorrelation function, the absorption spectrum, and the diabatic electronic population dynamics to complexity constraints is analyzed in detail. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4733676]
Erscheinungsjahr
Zeitschriftentitel
The Journal Of Chemical Physics
Band
137
Zeitschriftennummer
22
Seite
22A509
ISSN
PUB-ID

Zitieren

Westermann T, Manthe U. Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. The Journal Of Chemical Physics. 2012;137(22):22A509.
Westermann, T., & Manthe, U. (2012). Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. The Journal Of Chemical Physics, 137(22), 22A509. doi:10.1063/1.4733676
Westermann, T., and Manthe, U. (2012). Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. The Journal Of Chemical Physics 137, 22A509.
Westermann, T., & Manthe, U., 2012. Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. The Journal Of Chemical Physics, 137(22), p 22A509.
T. Westermann and U. Manthe, “Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine”, The Journal Of Chemical Physics, vol. 137, 2012, pp. 22A509.
Westermann, T., Manthe, U.: Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. The Journal Of Chemical Physics. 137, 22A509 (2012).
Westermann, Till, and Manthe, Uwe. “Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine”. The Journal Of Chemical Physics 137.22 (2012): 22A509.

5 Zitationen in Europe PMC

Daten bereitgestellt von Europe PubMed Central.

Electron-vibration entanglement in the Born-Oppenheimer description of chemical reactions and spectroscopy.
McKemmish LK, McKenzie RH, Hush NS, Reimers JR., Phys Chem Chem Phys 17(38), 2015
PMID: 26204101
Quantum dynamics of the photostability of pyrazine.
Sala M, Guérin S, Gatti F., Phys Chem Chem Phys 17(44), 2015
PMID: 26381824
Perspective: Nonadiabatic dynamics theory.
Tully JC., J Chem Phys 137(22), 2012
PMID: 23249037

42 References

Daten bereitgestellt von Europe PubMed Central.


AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0
Material in PUB:
Teil dieser Dissertation

Export

Markieren/ Markierung löschen
Markierte Publikationen

Open Data PUB

Web of Science

Dieser Datensatz im Web of Science®

Quellen

PMID: 23249046
PubMed | Europe PMC

Suchen in

Google Scholar