相关论文: Charge-transfer excited states: Seeking a balanced…
We propose an accurate variational Monte Carlo method applicable in the presence of the strong spin-orbit interaction. Our variational wave functions consist of generalized Pfaffian-Slater wave functions that involve mixtures of singlet and…
We employ a generalized variational principle to improve the stability, reliability, and precision of fully excited-state-specific complete active space self-consistent field theory. Compared to previous approaches that similarly seek to…
We investigate energy transport in several two-level atom or spin-1/2 models by a direct coupling to heat baths of different temperatures. The analysis is carried out on the basis of a recently derived quantum master equation which…
We investigate how the fixed-node diffusion Monte Carlo energy of solids depends on single-particle orbitals used in Slater--Jastrow wave functions. We demonstrate that the dependence can be significant, in particular in the case of 3d…
Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several…
A quantum Monte Carlo method is presented for determining multi-determinantal Jastrow-Slater wave functions for which the energy is stationary with respect to the simultaneous optimization of orbitals and configuration interaction…
A recently developed self-healing diffusion Monte Carlo algorithm [PRB 79, 195117] is extended to the calculation of excited states. The formalism is based on an excited-state fixed-node approximation and the mixed estimator of the…
A method is introduced to optimize excited state trial wave functions. The method is applied to ground and vibrationally excited states of bosonic van der Waals clusters of upto seven particles. Employing optimized trial wavefunctions with…
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 the regime where traditional approaches to electronic structure cannot afford to achieve accurate energy differences via exhaustive wave function flexibility, rigorous approaches to balancing different states' accuracies become…
We investigate an extension of excited state mean-field theory in which the energy expression is augmented with density functional components in an effort to include the effects of weak electron correlations. The approach remains…
A systematic method for determining correlated wavefunctions of extended systems in the ground and excited states is presented. It allows to fully exploit the power of quantum-chemical programs designed for correlation calculations of…
The attention mechanism has transformed artificial intelligence research by its ability to learn relations between objects. In this work, we explore how a many-body wavefunction ansatz constructed from a large-parameter self-attention…
Despite significant advances in electronic structure methods for the treatment of excited states, attaining an accurate description of the photoinduced processes in photoactive biomolecules is proving very difficult. For the prototypical…
The implementation and reliability of a quadratic diffusion Monte Carlo method for the study of ground-state properties of atoms are discussed. We show in the simple yet non-trivial calculation of the binding energy of the Li atom that the…
We present a flexible, automated, and basis-set insensitive domain-based charge-transfer (CT) decomposition framework that can be combined with any CI-type excited-state wavefunction. Our approach is not based on excited-state densities and…
A new computational method for finite-temperature properties of strongly correlated electrons is proposed by extending the variational Monte Carlo method originally developed for the ground state. The method is based on the path integral in…
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…
We present a modification to variational Monte Carlo's linear method optimization scheme that addresses a critical memory bottleneck while maintaining compatibility with both the traditional ground state variational principle and our…
We present a theoretical investigation of resonant charge transfer in low-energy Li$^+$ ions backscattered from a MoS$_2$ surface, focusing on the influence of excited projectile states. Using a time-dependent Anderson model in the…