相关论文: A Promising Intersection of Excited-State-Specific…

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 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…

The accurate quantum chemical calculation of excited states is a challenging task, often requiring computationally demanding methods. When entire ground and excited potential energy surfaces (PESs) are desired, e.g., to predict the…

We perform excited-state variational Monte Carlo and diffusion Monte Carlo calculations using a simple and efficient wave function ansatz. This ansatz follows the recent variation-after-response formalism, accurately approximating a…

We systematically investigate the calculation of excited states in quantum chemistry using auxiliary field quantum Monte Carlo (AFQMC). Symmetry allows targeting of the lowest triplet excited states in AFQMC based on restricted open-shell…

We extend our hybrid linear-method/accelerated-descent variational Monte Carlo optimization approach to excited states and investigate its efficacy in double excitations. In addition to showing a superior statistical efficiency when…

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…

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…

In this communication, we propose a method for obtaining isolated excited states within the Full Configuration Interaction Quantum Monte Carlo framework. This method allows for stable sampling with respect to collapse to lower energy states…

Monte Carlo techniques have been widely employed in statistical physics as well as in quantum theory in the Lagrangian formulation. However, in the conventional approach, it is extremely difficult to compute the excited states. Here we…

Quantum Monte Carlo (QMC) methods have proven to be highly accurate for computing excited states, but the choice of optimization strategies for multiple states remains an active topic of investigation. In this work, we revisit the…

We show that recently developed quantum Monte Carlo methods, which provide accurate vertical transition energies for single excitations, also successfully treat double excitations. We study the double excitations in medium-sized molecules,…

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…

A quantum Monte Carlo method is introduced to optimize excited state trial wavefunctions. The method is applied in a correlation function Monte Carlo calculation to compute ground and excited state energies of bosonic van der Waals clusters…

We present a new method for modeling electronically excited states that overcomes a key failing of linear response theory by allowing the underlying ground state ansatz to relax in the presence of an excitation. The method is variational,…

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…

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…

We demonstrate that a broad class of excited state variational principles is not size consistent. In light of this difficulty, we develop and test an approach to excited state optimization that transforms between variational principles in…

A variational Monte Carlo method is used to generate sets of orthogonal trial functions, Psi_T(J^pi,T), for given quantum numbers in various light p-shell nuclei. These Psi_T are then used as input to Green's function Monte Carlo…

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. $\textbf{14}$,…