Related papers: Vibrational response functions for multidimensiona…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
Nonadiabatic corrections in molecules composed of a few atoms are considered. It is demonstrated that a systematic perturbative expansion around the adiabatic solution is possible, with the expansion parameter being the electron-nucleus…
Adiabatic theorem and non-adiabatic corrections have been widely applied in modern quantum technology. Recently, non-adiabatic linear response theory has been developed to probe the many-body correlations in closed systems. In this work, we…
We present a theory of vibrational modulation of two-dimensional coherent Fourier transformed electronic spectra. Based on an expansion of the system's energy gap correlation function in terms of Huang-Rhys factors, we explain the…
An algebraic model taking into account the influence of the molecular rotation on the wave functions of vibrational-rotational states of the diatomic molecule using the formalism of the ladder operators and an expansion in a small parameter…
Although useful to extract excitation energies of states of double-excitation character in time-dependent density functional theory that are missing in the adiabatic approximation, the frequency-dependent kernel derived earlier [J. Chem.…
Real-time simulations of laser-driven electron dynamics contain information about molecular optical properties through all orders in response theory. These properties can be extracted by assuming convergence of the power series expansion of…
In order to model experimental non-resonant Raman optical activity, chemists must compute a host of second-order response tensors, (e.g. the electric-dipole magnetic-dipole polarizability) and their nuclear derivatives along a set of…
The vibrational dynamics of adsorbate molecules in single-molecule junctions depend critically on the geometric structure and electronic interactions between molecule and substrate. Vibrations, excited mechanochemically or by external…
A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…
This contribution reports the study of a set of molecular electronic-structure reorganization representations related to light-induced electronic transitions, modeled in the framework of time-dependent density-functional response theory.…
Electronic friction and Langevin dynamics is a popular mixed quantum-classical method for simulating the nonadiabatic dynamics of molecules interacting with metal surfaces, as it can be computationally more efficient than fully quantum…
Microscopic energy density functionals (EDF) have become a standard tool for nuclear structure calculations, providing an accurate global description of nuclear ground states and collective excitations. For spectroscopic applications this…
The time-development of photoexcitations in molecular aggregates exhibits specific dynamics of electronic states and vibrational wavefunction. We discuss the dynamical formation of entanglement between electronic and vibrational degrees of…
In the current density functional theory of linear and nonlinear time-dependent phenomena, the treatment of exchange and correlation beyond the level of the adiabatic local density approximation is shown to lead to the appearance of…
We present a methodology for simulating multi-dimensional electronic spectra of molecular aggregates with coupling of electronic excitation to a structured environment using the stochastic non-Markovian quantum state diffusion (NMQSD)…
A nonadiabatic scheme for the description of the coupled electron and nuclear motions in the ozone molecule was proposed recently. An initial coherent nonstationary state was prepared as a superposition of the ground state and the excited…
We show that the time dependent single electron, nuclear density matrix of an interacting electronic system coupled to nuclear degrees of freedom can be exactly reproduced by that of an electronic system with arbitrarily specified…
The linear response of non-equilibrium systems with Markovian dynamics satisfies a generalized fluctuation-dissipation relation derived from time symmetry and antisymmetry properties of the fluctuations. The relation involves the sum of two…
The quantum mechanical motion of the atomic nuclei is considered over a single- or a multi-dimensional subspace of electronic states which is separated by a gap from the rest of the electronic spectrum over the relevant range of nuclear…