相关论文: Ab-initio simulation of excited-state potential en…
Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…
Obtaining accurate ground and low-lying excited states of electronic systems is crucial in a multitude of important applications. One ab initio method for solving the Schr\"odinger equation that scales favorably for large systems is…
We present a discussion of recent progress in excited-state-specific quantum chemistry and quantum Monte Carlo alongside a demonstration of how a combination of methods from these two fields can offer reliably accurate excited state…
A faithful description of chemical processes requires exploring extended regions of the molecular potential energy surface (PES), which remains challenging for strongly correlated systems. Transferable deep-learning variational Monte Carlo…
The essence of atomic structure theory, quantum chemistry, and computational materials science is solving the multi-electron stationary Schr\"odinger equation. The Quantum Monte Carlo-based neural network wave function method has surpassed…
We present a variational Monte Carlo algorithm for estimating the lowest excited states of a quantum system which is a natural generalization of the estimation of ground states. The method has no free parameters and requires no explicit…
Quantum Monte Carlo (QMC) is a stochastic method which has been particularly successful for ground-state electronic structure calculations but mostly unexplored for the computation of excited-state energies. Here, we show that, within a…
Reflecting the increasing interest in quantum computing, the variational quantum eigensolver (VQE) has attracted much attentions as a possible application of near-term quantum computers. Although the VQE has often been applied to quantum…
The potential energy surface (PES) is crucial for interpreting a variety of chemical reaction processes. However, predicting accurate PESs with high-level electronic structure methods is a challenging task due to the high computational…
We employ quantum Monte Carlo to obtain chemically accurate vertical and adiabatic excitation energies, and equilibrium excited-state structures for the small, yet challenging, formaldehyde and thioformaldehyde molecules. A key ingredient…
Due to their diverse nature, the faithful description of excited states within electronic structure theory methods remains one of the grand challenges of modern theoretical chemistry. Quantum Monte Carlo (QMC) methods have been applied very…
Understanding the properties of excited states of complex molecules is crucial for many chemical and physical processes. Calculating these properties is often significantly more resource-intensive than calculating their ground state…
Excited states of molecules lie in the heart of photochemistry and chemical reactions. The recent development in quantum computational chemistry leads to inventions of a variety of algorithms that calculate the excited states of molecules…
Electronically excited states of molecules are at the heart of photochemistry, photophysics, as well as photobiology and also play a role in material science. Their theoretical description requires highly accurate quantum chemical…
Quantum Monte Carlo methods are first-principle approaches that approximately solve the Schr\"odinger equation stochastically. As compared to traditional quantum chemistry methods, they offer important advantages such as the ability to…
We introduce several improvements to the penalty-based variational quantum Monte Carlo (VMC) algorithm for computing electronic excited states of Entwistle $\textit{et al.}$ [M. T. Entwistle $\textit{et al.}$, Nat. Commun. $\textbf{14}$,…
We show that the recently developed phaseless auxiliary-field quantum Monte Carlo (AFQMC) method can be used to study excited states, providing an alternative to standard quantum chemistry methods. The phaseless AFQMC approach, whose…
We introduce the multistate iterative qubit coupled cluster (MS-iQCC) method, a quantum-inspired algorithm that runs efficiently on classical hardware and is designed to predict both ground and excited electronic states of molecules.…
This paper explores the utility of the quantum phase estimation (QPE) in calculating high-energy excited states characterized by promotions of electrons occupying inner energy shells. These states have been intensively studied over the last…
We present a new approach to calculate excited states with the full configuration interaction quantum Monte Carlo (FCIQMC) method. The approach uses a Gram-Schmidt procedure, instantaneously applied to the stochastically evolving…