Related papers: Nonadiabatic ab initio molecular dynamics includin…
We propose to measure the importance of spin-orbit couplings (SOCs) in the nonadiabatic molecular quantum dynamics rigorously with quantum fidelity. To make the criterion practical, quantum fidelity is estimated efficiently with the…
We have experimentally and theoretically investigated the mixed-field orientation of rotational-state-selected OCS molecules and we achieve strong degrees of alignment and orientation. The applied moderately intense nanosecond laser pulses…
While, the sulfur dioxide molecule has been extensively studied over the last decades, its photoexcitation dynamics is still unclear, due to its complexity, combining conical intersections and spin-orbit coupling between a manifold of…
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…
We study effects of nonadiabatic couplings in a model of a diatomic molecule in the context of attosecond transient absorption spectroscopy. By using a model system consisting of four diabatic electronic states and with a variable strength…
Nonadiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy…
Spin-orbit, charge-transfer intersystem crossing (SOCT-ISC) allows for the efficient production of triplet excited states in donor-acceptor (DA) dyads without the involvement of heavy atoms, for use in a myriad of technologies. This process…
We present a theoretical study of the impact of an electrostatic field combined with non-resonant linearly polarized laser pulses on the rotational dynamics of linear molecules. Within the rigid rotor approximation, we solve the…
Excited-state molecular dynamics (ESMD) simulations near conical intersections (CIs) pose significant challenges when using machine learning potentials (MLPs). Although MLPs have gained recognition for their integration into mixed…
We demonstrate the emergence of the non-Abelian geometric potentials and thus the three-dimensional (3D) spin-orbit coupling (SOC) for ultracold atoms without using the laser beams. This is achieved by subjecting an atom to a periodic…
In a Stark decelerator, polar molecules are slowed down and focussed by an inhomogeneous electric field which switches between two configurations. For the decelerator to work, it is essential that the molecules follow the changing electric…
We study the growth dynamics of ordered structures of strongly interacting polar molecules in optical lattices. Using dipole blockade of microwave excitations, we map the system onto an interacting spin-1/2 model possessing ground states…
Energy transfer during molecular collisions on metal surfaces plays a pivotal role in a host of critical interfacial processes. Despite significant efforts, our understanding of relevant energy transfer mechanisms, even in an…
Recently, the technique of counterdiabatic driving, which provides an effective strategy for accelerating adiabatic quantum evolution, has been widely applied in the preparation of many-body quantum states. In this work, we propose a…
For future use in modeling photoexcited dynamics and intersystem crossing, we calculate spin-adiabatic states and their analytical nuclear gradients within CIS the- ory. These energies and forces should be immediately useful for surface…
We experimentally demonstrated strong adiabatic mixed-field orientation of carbonyl sulfide molecules (OCS) in their absolute ground state of $\text{N}_{\text{up}}/\text{N}_{\text{tot}}=0.882$. OCS was oriented in combined non-resonant…
We build on the concept of eigenvector continuation to develop an efficient multi-state method for the rigorous and smooth interpolation of a small training set of many-body wavefunctions through chemical space at mean-field cost. The…
Nonadiabatic molecular dynamics is an effective method for modeling nonradiative decay in electronically excited molecules. Its accuracy depends strongly on the quality of the potential energy surfaces, and its affordability for long…
Transforming rovibronic Hamiltonians of molecular systems from the $\Lambda S$ (Hund's case a) basis to the adiabatic $\Omega$ representation is widely used to "remove" spin-orbit coupling (SOC) and enable single-state treatments of spectra…
The importance of triplet states in the photorelaxation dynamics of SO2 is studied by mixed quantum-classical dynamics simulations. Using the Surface Hopping including ARbitrary Couplings (Sharc) method, intersystem crossing processes…