Related papers: Why do mixed quantum-classical methods describe sh…
We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…
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 geometric phase (GP) is a fundamental quantum effect arising from conical intersections (CIs), with profound consequences for vibronic energy levels. Standard imaginary-time path integral molecular dynamics (PIMD) based on the…
While the treatment of conical intersections in molecular dynamics generally requires nonadiabatic approaches, the Born-Oppenheimer adiabatic approximation is still adopted as a valid alternative in certain circumstances. In the context of…
Quantum technologies based on adiabatic techniques can be highly effective, but often at the cost of being very slow. Here we introduce a set of experimentally realistic, non-adiabatic protocols for spatial state preparation, which yield…
Examples of geometric phases abound in many areas of physics. They offer both fundamental insights into many physical phenomena and lead to interesting practical implementations. One of them, as indicated recently, might be an inherently…
We explore the simulation of conical intersections (CIs) on quantum devices, setting the groundwork for potential applications in nonadiabatic quantum dynamics within molecular systems. The intersecting potential energy surfaces of…
We develop a linear vibronic coupling (LVC) model for polyenes described by the extended Hubbard-Peierls Hamiltonian. This model is applied to trans-hexatriene to benchmark quantum-classical dynamics methods against fully quantum…
Geometric quantum computation is the idea that geometric phases can be used to implement quantum gates, i.e., the basic elements of the Boolean network that forms a quantum computer. Although originally thought to be limited to adiabatic…
A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…
Geometric phases accompanying adiabatic quantum evolutions can be used to construct robust quantum control for quantum information processing due to their noise-resilient feature. A significant development along this line is to construct…
Ehrenfest dynamics is a useful approximation for ab initio mixed quantum-classical molecular dynamics that can treat electronically nonadiabatic effects. Although a severe approximation to the exact solution of the molecular time-dependent…
Nonadiabatic geometric quantum computation (NGQC) and nonadiabatic holonomic quantum computation (NHQC) have been proposed to reduce the run time of geometric quantum gates. However, in terms of robustness against experimental control…
Incorporating nuclear quantum effects into nonadiabatic dynamics remains a significant challenge. Herein we introduce new nonadiabatic dynamics approaches based on the recently developed constrained nuclear-electronic orbital (CNEO) theory.…
The geometric phase effect arises from the dependence on the nuclear coordinates in the electronic Hamiltonian, leading to sign changes of the electronic wave functions upon traversal of certain paths in nuclear configuration space. The…
Nonadiabatic quantum interferences emerge whenever nuclear wavefunctions in different electronic states meet and interact in a nonadiabatic region. In this work, we analyze how nonadiabatic quantum interferences translate in the context of…
Ab initio modeling of conical intersection dynamics is crucial for various photochemical, photophysical, and biological processes. However, adiabatic electronic states obtained from electronic structure computations involve random phases,…
We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…
We extend correlated sampling from classical auxiliary-field quantum Monte Carlo to the quantum-classical (QC-AFQMC) framework, enabling accurate nuclear force computations crucial for geometry optimization and reaction dynamics. Stochastic…
Accelerating quantum dynamical simulations with quantum computing has received considerable attention but remains a significant challenge. In variational quantum algorithms for quantum dynamics, designing an expressive and shallow-depth…