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A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional theory (TDDFT) around a suitable reference density. We show that the inclusion of the second order term renders the method a self-consistent scheme and improves the calculated optical spectra of molecules by a proper treatment of the coupled response. In the application to ion-fullerene collisions, the inclusion of self-consistency is found to be crucial for a correct description of the charge transfer between projectile and target. For a model of the photoreceptor in retinal proteins, nonadiabatic molecular dynamics simulations are performed and reveal problems of TDDFT in the prediction of intra-molecular charge transfer excitations.
We review different computational methods for the calculation of photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses using time-dependent density-functional theory (TDDFT) that are suitable for the desc
We demonstrate that a conditional wavefunction theory enables a unified and efficient treatment of the equilibrium structure and nonadiabatic dynamics of correlated electron-ion systems. The conditional decomposition of the many-body wavefunction for
Hyperconjugation is a basic conception of chemistry. Its straightforward effect is exhibited by the spatial delocalization characteristics of the electron density distributions or wavefunctions. Such effects on the electron wavefunctions of the highe
We present a detailed analysis of several time-dependent DFT (TD-DFT) methods, including conventional hybrid functionals and two types of non-empirically tuned range-separated functionals, for predicting a diverse set of electronic excitations in DNA
We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we construct a cl