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Variational Monte Carlo methods have recently been applied to the calculation of excited states; however, it is still an open question what objective function is most effective. A promising approach is to optimize excited states using a…

Computational Physics · Physics 2023-12-04 William A. Wheeler , Kevin G. Kleiner , Lucas K. Wagner

The calculation of molecular excited states is critically important to decipher a plethora of molecular properties. In this manuscript, we develop an equation of motion formalism on top of a bi-exponentially parametrized ground state…

Chemical Physics · Physics 2024-01-09 Anish Chakraborty , Pradipta Kumar Samanta , Rahul Maitra

Density functional theory can be extended to excited states by means of a unified variational approach for passive state ensembles. This extension overcomes the restriction of the typical density functional approach to ground states, and…

Chemical Physics · Physics 2019-07-10 Tim Gould , Stefano Pittalis

In quantum chemistry, obtaining a system's mean-field solution and incorporating electron correlation in a post Hartree-Fock (HF) manner comprise one of the standard protocols for ground-state calculations. In principle, this scheme can…

Chemical Physics · Physics 2020-09-02 Hong-Zhou Ye , Troy Van Voorhis

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…

Strongly Correlated Electrons · Physics 2015-05-13 Fernando A. Reboredo

We report the first study using active-orbital-based and adaptive CC($P$;$Q$) approaches to describe excited electronic states. These CC($P$;$Q$) methodologies are applied, alongside their completely renormalized (CR) coupled-cluster (CC)…

Chemical Physics · Physics 2025-01-08 Karthik Gururangan , Jun Shen , Piotr Piecuch

We apply the transcorrelated method to problems of multireference character. For this, we show that the choice of reference wavefunction during the Jastrow optimisation procedure is vital, and we propose a workflow wherein we use…

Variational methods have proven to be excellent tools to approximate ground states of complex many body Hamiltonians. Generic tools like neural networks are extremely powerful, but their parameters are not necessarily physically motivated.…

Strongly Correlated Electrons · Physics 2022-03-04 Agnes Valenti , Eliska Greplova , Netanel H. Lindner , Sebastian D. Huber

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. $\textbf{14}$,…

Chemical Physics · Physics 2024-09-23 P. Bernát Szabó , Zeno Schätzle , Mike T. Entwistle , Frank Noé

We present a novel approach for efficient preparation of electronic ground states, leveraging the optimizer ExcitationSolve [J\"ager et al., Comm. Phys. (2025)] and established variational quantum eigensolver-based operator selection…

Quantum Physics · Physics 2026-02-13 Max Haas , Thierry N. Kaldenbach , Thomas Hammerschmidt , Daniel Barragan-Yani

The excited electronic states involved in the optical cycle preparation of a pure spin state of the negatively charged NV-defect in diamond are calculated using the HSE06 hybrid density functional and variational optimization of the…

Materials Science · Physics 2025-10-29 Lei Sun , Elvar Örn Jónsson , Aleksei Ivanov , Ji Chen , Hannes Jónsson

Calculations of highly excited and delocalized molecular vibrational states are computationally challenging tasks, which strongly depends on the choice of coordinates for describing vibrational motions. We introduce a new method that…

In an excitable Delaunay triangulation every node takes three states (resting, excited and refractory) and updates its state in discrete time depending on a ratio of excited neighbours. All nodes update their states in parallel. By varying…

Cellular Automata and Lattice Gases · Physics 2011-08-02 Andrew Adamatzky

State-space mixed-frequency vector autoregressions are now widely used for nowcasting. Despite their popularity, estimating such models can be computationally intensive, especially for large systems with stochastic volatility. To tackle the…

Econometrics · Economics 2021-12-22 Joshua C. C. Chan , Aubrey Poon , Dan Zhu

Recently, it has been shown that the ground-state energy of a quantum many-body system can be written in terms of cumulants. In this paper we show that the energies of excited states can be expressed similarly. These representations are…

Condensed Matter · Physics 2007-05-23 T. Schork , P. Fulde

The accuracy and efficiency of ab-initio quantum Monte Carlo (QMC) algorithms benefits greatly from compact variational trial wave functions that accurately reproduce ground state properties of a system. We investigate the possibility of…

Materials Science · Physics 2019-01-30 Shivesh Pathak , Lucas K. Wagner

The similarity transformed equation of motion coupled cluster (STEOM-CC) method is benchmarked against CC3 and EOM-CCSDT-3 for a large test set of valence excited states of organic molecules studied by Schreiber et al. [M. Schreiber, M.R.…

Chemical Physics · Physics 2018-01-09 J. Sous , P. Goel , M. Nooijen

Functionals that have local minima at the excited states of a non degenerate Hamiltonian are presented. Then, improved mutually orthogonal approximants of the ground and the first excited state are reported.

Quantum Physics · Physics 2008-01-25 Naoum C. Bacalis

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.…

Chemical Physics · Physics 2026-01-05 Robert A. Lang , Shashank G. Mehendale , Ilya G. Ryabinkin , Artur F. Izmaylov

Quantum Monte Carlo simulations of interacting electrons in solids often use Slater-Jastrow trial wave functions. The Jastrow function takes into account correlations between pairs of electrons. In simulations of solids, it is common to use…

Materials Science · Physics 2007-05-23 A. Garcia-Lekue , M. Nekovee , J. M. Pitarke , R. Gaudoin