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State-specific electronic structure theory provides a route towards balanced excited-state wave functions by exploiting higher-energy stationary points of the electronic energy. Multiconfigurational wave function approximations can describe…

Chemical Physics · Physics 2023-07-19 Antoine Marie , Hugh G. A. Burton

We investigate pfaffian trial wave functions with singlet and triplet pair orbitals by quantum Monte Carlo methods. We present mathematical identities and the key algebraic properties necessary for efficient evaluation of pfaffians.…

Other Condensed Matter · Physics 2013-05-29 M. Bajdich , L. Mitas , L. K. Wagner , K. E. Schmidt

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

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…

Strongly Correlated Electrons · Physics 2014-10-10 George H. Booth , Garnet Kin-Lic Chan

We propose here a single Pfaffian correlated variational ansatz, that dramatically improves the accuracy with respect to the single determinant one, while remaining at a similar computational cost. A much larger correlation energy is indeed…

Chemical Physics · Physics 2020-07-28 Claudio Genovese , Tomonori Shirakawa , Kousuke Nakano , Sandro Sorella

An intrinsic measure of the quality of a variational wave function is given by its overlap with the ground state of the system. We derive a general formula to compute this overlap when quantum dynamics in imaginary time is accessible. The…

Statistical Mechanics · Physics 2007-07-26 Christophe Mora , Xavier Waintal

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…

Chemical Physics · Physics 2018-08-09 Anthony Scemama , Anouar Benali , Denis Jacquemin , Michel Caffarel , Pierre-François Loos

Variational quantum calculations have borrowed many tools and algorithms from the machine learning community in the recent years. Leveraging great expressive power and efficient gradient-based optimization, researchers have shown that trial…

Disordered Systems and Neural Networks · Physics 2024-08-19 Matija Medvidović , Javier Robledo Moreno

Neural-network quantum states (NQS) offer a powerful and expressive ansatz for representing quantum many-body wave functions. However, their training via Variational Monte Carlo (VMC) methods remains challenging. It is well known that some…

Quantum Physics · Physics 2025-07-09 Antoine Misery , Luca Gravina , Alessandro Santini , Filippo Vicentini

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…

Chemical Physics · Physics 2023-02-07 Leon Otis , Eric Neuscamman

We investigate the use of different variational principles in quantum Monte Carlo, namely energy and variance minimization, prompted by the interest in the robust and accurate estimate of electronic excited states. For two prototypical,…

Chemical Physics · Physics 2021-11-19 Alice Cuzzocrea , Anthony Scemama , Wim J. Briels , Saverio Moroni , Claudia Filippi

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…

Computational Physics · Physics 2009-11-06 M. P. Nightingale , Vilen Melik-Alaverdian

A study of the first excited states of beryllium atom starting from explicitly correlated wave functions is carried out. Several properties are obtained and discussed focusing on the analysis of the Hund's rules in terms of the…

Atomic Physics · Physics 2009-11-07 F. J. Galvez , E. Buendia , A. Sarsa

We construct a family of BCS paired composite fermion wavefunctions that generalize, but remain in the same topological phase as, the Moore-Read Pfaffian state for the half-filled Landau level. It is shown that for a wide range of…

Mesoscale and Nanoscale Physics · Physics 2008-02-21 Gunnar Moller , Steven H. Simon

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

Neural network parametrizations have increasingly been used to represent the ground and excited states in variational Monte Carlo (VMC) with promising results. However, traditional VMC methods only optimize the wave function in regions of…

Computational Physics · Physics 2025-07-03 Huan Zhang , Robert J. Webber , Michael Lindsey , Timothy C. Berkelbach , Jonathan Weare

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…

Computational Physics · Physics 2025-04-15 Stuart Shepard , Anthony Scemama , Saverio Moroni , Claudia Filippi

We present high-accuracy correlated calculations of small Si$_x$H$_y$ molecular systems both in the ground and excited states. We employ quantum Monte Carlo (QMC) together with a variety of many-body wave function approaches based on basis…

Chemical Physics · Physics 2020-10-21 Guangming Wang , Abdulgani Annaberdiyev , Lubos Mitas

It is proven that the exact excited-state wave function and energy may be obtained by minimizing the energy expectation value of trial wave functions that are constrained only to have the correct nodes of the state of interest. This…

Quantum Physics · Physics 2018-08-24 Federico Zahariev , Mark S. Gordon , Mel Levy

Functional magnetic resonance imaging (fMRI) enables indirect detection of brain activity changes via the blood-oxygen-level-dependent (BOLD) signal. Conventional analysis methods mainly rely on the real-valued magnitude of these signals.…

Methodology · Statistics 2023-10-31 Zhengxin Wang , Daniel B. Rowe , Xinyi Li , D. Andrew Brown