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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

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

Many-body Green's functions theory within the GW approximation and the Bethe-Salpeter Equation (BSE) is implemented in the open-source VOTCA-XTP software, aiming at the calculation of electronically excited states in complex molecular…

We review the Bethe-Salpeter equation (BSE) approach to the calculation of electronic excitation energies of molecular systems. We recall the general Green's function many-theory formalism and give the working equations of the BSE approach…

Chemical Physics · Physics 2013-04-05 Elisa Rebolini , Julien Toulouse , Andreas Savin

Inspired by Grimme's simplified Tamm-Dancoff density functional theory approach [S. Grimme, J. Chem. Phys. \textbf{138}, 244104 (2013)], we describe a simplified approach to excited state calculations within the GW approximation to the…

Mesoscale and Nanoscale Physics · Physics 2021-09-10 Yeongsu Cho , Sylvia J. Bintrim , Timothy C. Berkelbach

Excitonic effects due to electron-hole coupling play a fundamental role in renormalising energy levels in dye sensitised and organic solar cells determining the driving force for electron extraction. We show that first-principles…

Materials Science · Physics 2017-02-15 Margherita Marsili , Edoardo Mosconi , Filippo De Angelis , Paolo Umari

Accurate predictions of charge excitation energies of molecules in the disordered condensed phase are central to the chemical reactivity, stability, and optoelectronic properties of molecules and critically depend on the specific…

Chemical Physics · Physics 2021-08-25 Guorong Weng , Vojtech Vlcek

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…

Computational Physics · Physics 2019-08-02 Monika Dash , Jonas Feldt , Saverio Moroni , Anthony Scemama , Claudia Filippi

We present a hybrid approach for GW/Bethe-Salpeter Equation (BSE) calculations of core excitation spectra, including x-ray absorption (XAS), electron energy loss spectra (EELS), and non-resonant inelastic x-ray scattering (NRIXS). The…

Materials Science · Physics 2015-05-20 J. Vinson , E. L. Shirley , J. J. Rehr , J. J. Kas

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…

Chemical Physics · Physics 2025-03-26 Zeno Schätzle , P. Bernát Szabó , Alice Cuzzocrea , Frank Noé

Machine learning applications in the chemical sciences, especially when based on neural networks, critically depend on the availability of large quantities of high quality data. As they provide excellent accuracy for both charged and…

Chemical Physics · Physics 2025-12-12 Dario Baum , Arno Förster , Lucas Visscher

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…

Other Condensed Matter · Physics 2009-11-10 Friedemann Schautz , Francesco Buda , Claudia Filippi

We present a novel hybrid quantum/classical (QM/MM) approach to the calculation of charged excitations in molecular solids based on the many-body Green's function $GW$ formalism. Molecules described at the $GW$ level are embedded into the…

Chemical Physics · Physics 2018-02-14 Jing Li , Gabriele D'Avino , Ivan Duchemin , David Beljonne , Xavier Blase

We present a first-principles method for the calculation of optical excitations in nanosystems. The method is based on solving the Bethe-Salpeter equation (BSE) for neutral excitations. The electron self-energy is evaluated within the GW…

Materials Science · Physics 2009-11-11 Murilo L. Tiago , James R. Chelikowsky

Quantum Monte Carlo (QMC) techniques are used to calculate the one-body density matrix and excitation energies for the valence electrons of bulk silicon. The one-body density matrix and energies are obtained from a Slater-Jastrow wave…

Condensed Matter · Physics 2009-10-31 P. R. C. Kent , Randolph Q. Hood , M. D. Towler , R. J. Needs , G. Rajagopal

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

We calculate single-particle excitation energies for a series of 33 molecules using fully selfconsistent GW, one-shot G$_0$W$_0$, Hartree-Fock (HF), and hybrid density functional theory (DFT). All calculations are performed within the…

Materials Science · Physics 2015-05-14 C. Rostgaard , K. W. Jacobsen , K. S. Thygesen

Charged excitations of the oligoacene family of molecules, relevant for astrophysics and technological applications, are widely studied and therefore provide an excellent system for benchmarking theoretical methods. In this work, we…

Chemical Physics · Physics 2016-05-18 Tonatiuh Rangel , Samia M. Hamed , Fabien Bruneval , Jeffrey B. Neaton

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…

Nuclear Theory · Physics 2008-11-26 Steven C. Pieper , R. B. Wiringa , J. Carlson

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…

Chemical Physics · Physics 2025-09-16 Ankit Mahajan , Sandeep Sharma , Shiwei Zhang , David R. Reichman
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