Stochastic simulation of catalytic surface reactions in the fast diffusion limit

The master equation of a lattice gas reaction tracks the probability of visiting all spatial configurations. The large number of unique spatial configurations on a lattice renders master equation simulations infeasible for even small lattices. In this work, a reduced master equation is derived for the probability distribution of the coverages in the infinite diffusion limit. This derivation justifies the widely used assumption that the adlayer is in equilibrium for the current coverages and temperature when all reactants are highly mobile. Given the reduced master equation, two novel and efficient simulation methods of lattice gas reactions in the infinite diffusion limit are derived. The first method involves solving the reduced master equation directly for small lattices, which is intractable in configuration space. The second method involves reducing the master equation further in the large lattice limit to a set of differential equations that tracks only the species coverages. Solution of the reduced master equation and differential equations requires information that can be obtained through short, diffusion-only kinetic Monte Carlo simulation runs at each coverage. These simulations need to be run only once because the data can be stored and used for simulations with any set of kinetic parameters, gas-phase concentrations, and initial conditions. An idealized CO oxidation reaction mechanism with strong lateral interactions is used as an example system for demonstrating the reduced master equation and deterministic simulation techniques

Wigner distribution functions for complex dynamical systems: a path integral approach

Starting from Feynman's Lagrangian description of quantum mechanics, we propose a method to construct explicitly the propagator for the Wigner distribution function of a single system. For general quadratic Lagrangians, only the classical phase space trajectory is found to contribute to the propagator. Inspired by Feynman's and Vernon's influence functional theory we extend the method to calculate the propagator for the reduced Wigner function of a system of interest coupled to an external system. Explicit expressions are obtained when the external system consists of a set of independent harmonic oscillators. As an example we calculate the propagator for the reduced Wigner function associated with the Caldeira-Legett model

Compressed sensing quantum process tomography for superconducting quantum gates

We apply the method of compressed sensing (CS) quantum process tomography (QPT) to characterize quantum gates based on superconducting Xmon and phase qubits. Using experimental data for a two-qubit controlled-Z gate, we obtain an estimate for the process matrix $\chi$ with reasonably high fidelity compared to full QPT, but using a significantly reduced set of initial states and measurement configurations. We show that the CS method still works when the amount of used data is so small that the standard QPT would have an underdetermined system of equations. We also apply the CS method to the analysis of the three-qubit Toffoli gate with numerically added noise, and similarly show that the method works well for a substantially reduced set of data. For the CS calculations we use two different bases in which the process matrix $\chi$ is approximately sparse, and show that the resulting estimates of the process matrices match each ther with reasonably high fidelity. For both two-qubit and three-qubit gates, we characterize the quantum process by not only its process matrix and fidelity, but also by the corresponding standard deviation, defined via variation of the state fidelity for different initial states.Comment: 16 pages, 11 figure