相关论文: Calculate electronic excited states using neural n…

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…

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 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…

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…

Electronic excited states of molecules are central to many physical and chemical processes, and yet they are typically more difficult to compute than ground states. In this paper we leverage the advantages of quantum computers to develop an…

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…

Deep learning techniques have opened a new venue for electronic structure theory in recent years. In contrast to traditional methods, deep neural networks provide much more expressive and flexible wave function ansatz, resulting in better…

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…

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…

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…

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…

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…

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 have trained a deep (convolutional) neural network to predict the ground-state energy of an electron in four classes of confining two-dimensional electrostatic potentials. On randomly generated potentials, for which there is no analytic…

Certain point defects in solids can efficiently be used as qubits for applications in quantum technology. They have spin states that are initializable, readable, robust, and can be manipulated optically. New theoretical methods are needed…

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 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…

Accurately solving the Schr\"odinger equation remains a central challenge in computational physics, chemistry, and materials science. Here, we propose an alternative eigenvalue problem based on a system's autocorrelation function, avoiding…

[New and updated results were published in Nature Chemistry, doi:10.1038/s41557-020-0544-y.] The electronic Schr\"odinger equation describes fundamental properties of molecules and materials, but can only be solved analytically for the…