article
Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine
published
yes
Till
Westermann
author 24758931
Uwe
Manthe
author 109657
10018
department
17982
department
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]
AIP Publishing2012
eng
The Journal Of Chemical Physics
0021-9606
23249046
00031249140001010.1063/1.4733676
1372222A509
https://pub.uni-bielefeld.de/record/2637434
<div style="text-indent:-25px; padding-left:25px;padding-bottom:0px;">Westermann, T., & Manthe, U. (2012). Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. <em>The Journal Of Chemical Physics</em>, <em>137</em>(22), 22A509. doi:10.1063/1.4733676</div>
T. Westermann and U. Manthe, “Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine”, <em>The Journal Of Chemical Physics</em>, vol. 137, 2012, pp. 22A509.
Westermann, T., & Manthe, U., 2012. Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. <em>The Journal Of Chemical Physics</em>, 137(22), p 22A509.
<div style="text-indent:-25px; padding-left:25px;padding-bottom:0px;">Westermann, T. & Manthe, U. (2012). Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. <em>The Journal Of Chemical Physics</em>, <em>137</em>(22), 22A509. AIP Publishing. doi:10.1063/1.4733676.</div>
<div style="text-indent:-25px; padding-left:25px;padding-bottom:0px;">Westermann, Till, and Manthe, Uwe. 2012. “Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine”. <em>The Journal Of Chemical Physics</em> 137 (22): 22A509.</div>
T. Westermann and U. Manthe, Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine, The Journal Of Chemical Physics <strong>137</strong>, (2012).
Westermann T, Manthe U. Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. <em>The Journal Of Chemical Physics</em>. 2012;137(22):22A509.
Westermann, T.; Manthe, U. (2012): Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine <em>The Journal Of Chemical Physics</em>,137:(22): 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).
T. Westermann, and U. Manthe, “Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine”, <em>The Journal Of Chemical Physics</em>, <strong>2012</strong>, <em>137</em>, 22A509.
Westermann T, Manthe U (2012) <br /><em>The Journal Of Chemical Physics</em> 137(22): 22A509.
Westermann T, Manthe U (2012) <br />Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine.<br />The Journal Of Chemical Physics 137(22): 22A509.
Westermann, T., & Manthe, U. (2012). Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine. <em>The Journal Of Chemical Physics</em>, <em>137</em>(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. <em>The Journal Of Chemical Physics</em> 137, 22A509.
Westermann, Till, and Manthe, Uwe. “Decoherence induced by conical intersections: Complexity constrained quantum dynamics of photoexcited pyrazine”. <em>The Journal Of Chemical Physics</em> 137.22 (2012): 22A509.
25533072013-02-04T08:02:23Z2018-07-24T13:01:17Z