Theoretical study of nonadiabatic hydrogen atom scattering dynamics on metal surfaces using the hierarchical equations of motion method

Abstract

Hydrogen atom scattering on metal surfaces is investigated based on a simplified Newns–Anderson model. Both the nuclear and electronic degrees of freedom are treated quantum mechanically. By partitioning all the surface electronic states as the bath, the hierarchical equations of motion method for the fermionic bath is employed to simulate the scattering dynamics. It is found that, with a reasonable set of parameters, the main features of the recent experimental studies of hydrogen atom scattering on metal surfaces can be reproduced. Vibrational states on the chemisorption state whose energies are close to the incident energy are found to play an important role, and the scattering process is dominated by a single-pass electronic transition forth and back between the diabatic physisorption and chemisorption states. Further study on the effects of the atom-surface coupling strength reveals that, upon increasing the atom-surface coupling strength, the scattering mechanism changes from typical nonadiabatic transitions to dynamics in the electronic friction regime.

Simulating Chemistry on Bosonic Quantum Devices

“…For example, to simulate the dynamics of the spin-boson model, the current qubit-based quantum algorithm developed for the formally exact generalized quantum master equation (GQME) approach − relies on a classical computer to solve the underlying exact memory kernel due to the limited computational resources of current NISQ devices . The hierarchical equations of motion (HEOM) approach is a numerically exact method for open quantum systems, − which decomposes the environment into a few dissipative bosonic modes, , and as a result needs extra qubits for encoding. Bosonic quantum devices provide a natural way to encode the dissipative modes with qumodes to simulate the dynamics of quantum systems coupled to a bosonic environment.…”

A Linearized Semiclassical Dynamics Study of the Multiquantum Vibrational Relaxation of NO Scattering from a Au(111) Surface

“…Specifically, we can extend this model to include orientational dependence and phonon mode dissipation. We can also systematically improve the level of SC theory using the MQC–SC methods developed in our group to selectively quantize nuclear and electronic dofs, while pursuing strategies to benchmark simplified models using exact dynamic methods like the recently developed hierarchy equations of motion (HEOM) approach for the study of metal–molecule interactions. , …”

Artificial-Intelligence-Based Surrogate Solution of Dissipative Quantum Dynamics: Physics-Informed Reconstruction of the Universal Propagator

“…Currently, our focus is on the time-independent case, where the dynamics depend solely on the Hamiltonian. Future investigations may extend to scenarios involving driven quantum systems, where the time evolution is influenced by the interaction with the external fields or by non-Markovian dynamics. ,, In addition, in many nondissipative scenarios, using wave functions alone may suffice. For such physical settings, we expect an excellent performance of our neural propagators (which were applied here to nonpure quantum states).…”