Coupling electron-nuclear

Switching electronic population to different final states with high efficiency via SPODS is a fundamental resonant strong-field effect as the only requirement is the use of intense ultrashort laser pulses exhibiting temporally varying optical phases, such as phase jumps [67, 68, 70, 71] or chirps [44, 72]. Only recently, these concepts were transferred to molecules, where the coupled electron-nuclear dynamics have to be considered in addition [73,74]. 

In conclusion, the concept of SPODS as discussed on atomic systems in the preceding sections is readily extended to the control of coupled electron-nuclear... 

Figure 41. Model system for the investigation of coupled electron-nuclear dynamics in a control field. Three ions and an electron are arranged in one dimension, where only the middle ion (coordinate R) and the electron (coordinate x) are allowed to move.

Figure 42. Contour plot displaying the model potential for a coupled electronic-nuclear motion. Contours are drawn in increments of 1 eV ranging from 1 eV to 10 eV as a function of the electronic (x) and nuclear coordinate (R).

A practical CASSCF approach to coupled electron-nuclear dynamics... 

Keywords Ehrenfest method CASSCF Coupled electron-nuclear dynamics Charge migration Charge transfer... 

We apply our second-order Ehrenfest method to study the coupled electron-nuclear dynamics of benzene upon... 

Mendive-Tapia D, Vacher M, Bearpark MJ, Robb MA (2013) Coupled electron-nuclear dynamics charge migration and charge transfer initiated near a conical intersection. J Chem Phys 139(4) 044110... 

Coherent Control in the Sub-femtosecond Domain Theory for Coupled Electron Nuclear Motion... 

In response theory, the basis functions %v(f) e usually chosen to be time independent for strong fields or coupled electron-nuclear dynamics, time-dependent basis functions can sometimes be more appropriate. 

Jones, G. A., Acocella, A., Zerbetto, R (2008). On-the-fly, electric-field-driven, coupled electron-nuclear dynamics. The Journal of Physical Chemistry A, 112(40), 9650-9656. doi 10.1021/ Jp805360v. 

Therefore, we present here our semiclassical Field-Induced Surface Hopping (FISH) method [59] for the simulation and control of the laser-driven coupled electron-nuclear dynamics in complex molecular systems including all degrees of freedom. It is based on the combination of quantum electronic state population dynamics with classical nuclear dynamics carried out on the fly . The idea of the method is to propagate independent trajectories in the manifold of adiabatic electronic states and allow them to switch between the states under the influence of the laser field. The switching probabilities are calculated fully quantum mechanically. The application of our FISH method will be illustrated in Sect. 17.6 on the example of optimal dynamic discrimination (ODD) of two almost identical flavin molecules. 

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