相关论文: Coupled Wavepackets for Non-Adiabatic Molecular Dy…
A method for performing variable-width (thawed) Gaussian wavepacket (GWP) variational dynamics on machine-learned potentials is presented. Instead of fitting the potential energy surface (PES), the anharmonic correction to the global…
The choice of the electronic representation in on-the-fly quantum dynamics is crucial. The adiabatic representation is appealing since adiabatic states are readily available from quantum chemistry packages. The nuclear wavepackets are then…
We present a new formulation of the correlated electron-ion dynamics (CEID) scheme, which systematically improves Ehrenfest dynamics by including quantum fluctuations around the mean-field atomic trajectories. We show that the method can…
In this work, we employ trajectory-based simulations to predict the electronic coherences created by nonadiabatic dynamics near conical intersections. The mapping approach to surface hopping (MASH) is compared with standard fewest-switches…
The dynamics of vibrational wave packets excited in K$_2$ dimers attached to superfluid helium nanodroplets is investigated by means of femtosecond pump-probe spectroscopy. The employed resonant three-photon-ionization scheme is studied in…
We use the effective Hamiltonian that we recently fitted against the first 306 experimentally observed vibronic transitions of NO2 [J. Chem. Phys. 119, 5923 (2003)] to investigate the time domain nonadiabatic dynamics of this molecule on…
Nonadiabatic molecular dynamics (NAMD) is widely used to describe hot electron relaxation and nonradiative recombination processes, but high computational costs limit its application to large supercells. Here, we implement a nonadiabatic…
The ultimate semiclassical wave packet propagation technique is a complex, time-dependent WBK method known as generalized Gaussian wave packet dynamics (GGWPD). It requires overcoming many technical difficulties in order to be carried out…
Non-adiabatic dynamics at molecule-metal interfaces govern diverse and technologically important phenomena, from heterogeneous catalysis to dye-sensitized solar energy conversion and charge transport across molecular junctions. Realistic…
A non-Markovian master equation for a molecule interacting with a heat bath is obtained using the cumulant expansion method. The equation is applied to the problem of molecular wave packet relaxtional dynamics. An exact solution is derived…
The development of emerging technologies in quantum optics demands accurate models that faithfully capture genuine quantum effects. Mature semiclassical approaches reach their limits when confronted with quantized electromagnetic fields,…
We present a general concept to accelerate non-relativistic charged particles. Our concept employs an adiabatically-tapered dielectric-lined waveguide which supports accelerating phase velocities for synchronous acceleration. We propose an…
An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely-spaced electronic states. We propose a mixed quantum-classical scheme…
We develop a semi-classical method to simulate the motion of atoms in a dissipative optical lattice. Our method treats the internal states of the atom quantum mechanically, including all nonadiabatic couplings, while position and momentum…
The static and dynamical properties of a one-dimensional quantum system described by a non-Hermitian Hamiltonian of the so-called Hatano-Nelson type; a tight-binding model with asymmetric (or non-reciprocal) hopping, are studied. The static…
The increasing need to simulate the dynamics of photoexcited molecular and nanosystems in the sub-picosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the…
Non-adiabatic chemical reactions involving continuous circularly polarized light (cw CPL) have not attracted as much attention as dynamics in unpolarized/linearly polarized light. However, including circularly (in contrast to linearly)…
Many advanced quantum techniques feature non-Gaussian dynamics, and the ability to manipulate the system in that domain is the next-stage in many experiments. One example of meaningful non-Gaussian dynamics is that of a double-well…
We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…
A generalization of the stochastic wave function method to quantum master equations which are not in Lindblad form is developed. The proposed stochastic unravelling is based on a description of the reduced system in a doubled Hilbert space…