相关论文: Optimal choice of dividing surface for the computa…
Modeling electronic systems is an important application for quantum computers. In the context of materials science, an important open problem is the computational description of chemical reactions on surfaces. In this work, we outline a…
Characterizing thermally activated transitions in high-dimensional rugged energy surfaces is a very challenging task for classical computers. Here, we develop a quantum annealing scheme to solve this problem. First, the task of finding the…
Computing accurate rate constants for catalytic events occurring at the surface of a given material represents a challenging task with multiple potential applications in chemistry. To address this question, we propose an approach based on a…
We analyze the efficiency of different methods for the calculation of reaction rates in the case of two simple analytical benchmark systems. Two classes of methods are considered: the first are based on the free energy calculation along a…
Near-term hardware is constrained by high error rates, small qubit counts, and relatively low output fidelity, making the execution of large, high performance quantum circuits difficult. Circuit partitioning (or circuit cutting) has emerged…
Surfaces serve as highly efficient catalysts for a vast variety of chemical reactions. Typically, such surface reactions involve billions of molecules which diffuse and react over macroscopic areas. Therefore, stochastic fluctuations are…
Rotational transitions in molecular hydrogen collisions are computed. The two most recently developed potential energy surfaces for the H2-H2 system are used from the following works: 1) A.I. Boothroyd, P.G. Martin, W.J. Keogh, M.J.…
The ring polymer molecular dynamics (RPMD) rate theory is an efficient and accurate method for estimating rate coefficients of chemical reactions affected by nuclear quantum effects. The commonly used RPMD treatment of gas-phase bimolecular…
In recent letter [Phys. Rev. Lett {\bf 105}, 150606 (2010)], the surface-mediated diffusion problem is theoretically discussed, and interesting results have been obtained. However, for more general cases, the ansatz of solutions of the…
The quantum circuit model is the most widely used model of quantum computation. It provides both a framework for formulating quantum algorithms and an architecture for the physical construction of quantum computers. However, several other…
We present an exact calculation of the mean first-passage time to a small target on the surface of a 2D or 3D spherical domain, for a molecule performing surface-mediated diffusion. This minimal model of interfacial reactions, which…
Our knowledge about the "cold" Universe often relies on molecular spectra. A general property of such spectra is that the energy level populations are rarely at local thermodynamic equilibrium. Solving the radiative transfer thus requires…
A quantum version of a recent formulation of transition state theory in {\em phase space} is presented. The theory developed provides an algorithm to compute quantum reaction rates and the associated Gamov-Siegert resonances with very high…
An overview of computational methods to describe high-dimensional potential energy surfaces suitable for atomistic simulations is given. Particular emphasis is put on accuracy, computability, transferability and extensibility of the methods…
The accuracy of rate constants calculated using transition state theory depends crucially on the correct identification of a recrossing--free dividing surface. We show here that it is possible to define such optimal dividing surface in…
A computational procedure is developed for determining the conversion probability for reaction-diffusion systems in which a first-order catalytic reaction is performed over active particles. We apply this general method to systems on metric…
Constructing an accurate approximation to nonadiabatic rate theory which is valid for arbitrary values of the electronic coupling has been a long-standing challenge in theoretical chemistry. Ring-polymer instanton theories offer a very…
Quantum mechanical methods have been devised for the elucidation and clarification of reaction paths of chemical processes over decades. While they are typically deployed in routine calculations on systems for which some insights have…
Astrochemical surface reactions are thought to be responsible for the formation of complex organic molecules, which are of potential importance for the origin of life. In a situation, when the chemical composition of dust surfaces is not…
Quantum-chemical simulations are essential for predicting energies of chemical reactions. Accurately solving the many-body Schr\"odinger equation for reagent and product states of most relevant chemical process is, however, unfeasible.…