Stochastic Methods and Computer Techniques in Quantum Dynamics

Alladi Ramakrishnan, Nagarajan Ranganathan

Ronnie Kosloff Uriel Shafir

An efficient algorithm to simulate dynamics of open quantum system is presented. The method describes the dynamics by unraveling stochastic wave functions converging to a density operator description. The stochastic techniques are based on the quantum collision model. Modeling systems dynamics by wave functions and modeling the interaction with the environment with a collision sequence reduces the complexity scale significantly. The algorithm developed, can be implemented on quantum computers. We introduce stochastic methods that exploit statistical characters of the model, as Markovianity, Brownian motion and binary distribution. The central limit theorem is employed to study the convergence of distributions of stochastic dynamics of pure quantum states represented by wave vectors. By averaging a sample of functions in the distribution we prove and demonstrate the convergence of the dynamics to the mixed quantum state described by a density operator.

Uriel Shafir, Ronnie Kosloff

An efficient algorithm to simulate dynamics of open quantum system is presented. The method describes the dynamics by unraveling stochastic wave functions converging to a density operator description. The stochastic techniques are based on the quantum collision model. Modeling systems dynamics with wave functions and modeling the interaction with the environment with a collision sequence reduces the scale of the complexity significantly. The algorithm developed can be implemented on quantum computers. We introduce stochastic methods that exploit statistical characteristics of the model such as Markovianity, Brownian motion, and binary distribution. The central limit theorem is employed to study the convergence of distributions of stochastic dynamics of pure quantum states represented by wave vectors. By averaging a sample of functions in the distribution we prove and demonstrate the convergence of the dynamics to the mixed quantum state described by a density operator.

Michel Caffarel

Annabelle Canestraight

This thesis develops stochastic many-body methodologies for the electronic structure description of chemically relevant systems with strong electron correlation and nonequilibrium dynamics. Many phenomena of interest in chemistry and materials science, including excited-state processes, charge transfer at catalytic interfaces, and plasmon-mediated photocatalysis, require an accurate treatment of interacting electrons beyond mean-field theory. However, direct solutions of the many-body Schrodinger equation remain computationally intractable for realistic systems due to the exponential growth of the configurational Hilbert space with system size. This challenge motivates the development of reduced representations and embedding strategies capable of retaining essential correlation effects at lower computational cost. The work presented here focuses on stochastic matrix compression and downfolding techniques for many-body electronic structure theory. In particular, new stochastic compression approaches are introduced for the efficient representation of many-body Hamiltonians and correlated wavefunctions within reduced active subspaces. These methods extend stochastic electronic structure techniques beyond their traditional applications in many-body perturbation theory and provide a framework for treating correlated subsystems embedded within large chemical environments. Applications of these approaches are demonstrated across several classes of problems. First, stochastic downfolding methodologies are developed for the computation of charged excitations and Dyson orbitals relevant to catalytic interfaces and molecular spectroscopy. These techniques enable the treatment of large orbital spaces while maintaining accurate descriptions of electron correlation in the active region. Second, stochastic compression methods are applied to the computation of total energies in large solvated and reactive systems, where conventional correlated approaches become prohibitively expensive. Finally, the thesis explores nonequilibrium electronic dynamics at driven catalytic interfaces, including plasmon-assisted charge transfer processes. In this context, time-dependent many-body simulations reveal that transient driving fields can dynamically modify molecular spectral structure, opening additional resonant pathways for hot-carrier injection that are absent in equilibrium descriptions. Taken together, the methods developed in this thesis provide new strategies for reducing the computational complexity of correlated electronic structure calculations while preserving the essential physics of many-body interactions. These results broaden the applicability of stochastic and embedding-based approaches to large-scale equilibrium and nonequilibrium problems in chemistry, condensed matter physics, and materials science.

Sergio A Albeverio, Ph. Blanchard, D. Testard