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The band structure of silicon is calculated at the Gamma, X, and L wave vectors using diffusion quantum Monte Carlo methods. Excited states are formed by promoting an electron from the valence band into the conduction band. We obtain good…

Condensed Matter · Physics 2009-10-31 A. J. Williamson , Randolph Q. Hood , R. J. Needs , G. Rajagopal

Donor-based quantum devices in silicon are attractive platforms for universal quantum computing and analog quantum simulations. The nearly-atomic precision in dopant placement promises great control over the quantum properties of these…

Quantum Physics · Physics 2025-03-05 Maicol A. Ochoa , Keyi Liu , Piotr Różański , Michał Zieliński , Garnett W. Bryant

A quantitative description of the excited electronic states of point defects and impurities is crucial for understanding materials properties, and possible applications of defects in quantum technologies. This is a considerable challenge…

We present a computationally efficient framework for predicting the excited-state properties of thermally activated delayed fluorescence (TADF) emitters, integrating extended tight-binding (\xtb), simplified Tamm-Dancoff approximation…

Recent work from our research group has demonstrated that symmetry-projected Hartree--Fock (HF) methods provide a compact representation of molecular ground state wavefunctions based on a superposition of non-orthogonal Slater determinants.…

Chemical Physics · Physics 2015-06-17 Carlos A. Jiménez-Hoyos , R. Rodríguez-Guzmán , Gustavo E. Scuseria

The high computational cost of ab-initio methods limits their application in predicting electronic properties at the device scale. Therefore, an efficient method is needed to map the atomic structure to the electronic structure quickly.…

Materials Science · Physics 2025-09-09 Yunlong Wang , Zhixin Liang , Chi Ding , Junjie Wang , Zheyong Fan , Hui-Tian Wang , Dingyu Xing , Jian Sun

Time-dependent density functional theory (TD-DFT) and correlated ab initio methods have been applied to the electronically excited states of vitamin B12 (cyanocobalamin or CNCbl). Different experimental techniques have been used to probe…

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

We propose a two-step protocol for inverting ultrafast spectroscopy experiments on a molecular aggregate to extract the time-evolution of the excited state density matrix. The first step is a deconvolution of the experimental signal to…

Quantum Physics · Physics 2013-05-29 Stephan Hoyer , K. Birgitta Whaley

We present a spin-dependent localized Hartree-Fock (SLHF) density-functional approach for the treatment of the inner-shell excited-state calculation of atomic systems. In this approach, the electron spin-orbitals in an electronic…

Atomic Physics · Physics 2009-11-11 Zhongyuan Zhou , Shih-I Chu

We present a method for finding individual excited states' energy stationary points in complete active space self-consistent field theory that is compatible with standard optimization methods and highly effective at overcoming difficulties…

Strongly Correlated Electrons · Physics 2019-04-12 Lan Nguyen Tran , Jacqueline A. R. Shea , Eric Neuscamman

In recent years, metal halide perovskites (MHPs) for optoelectronic applications have attracted the attention of the scientific community due to their outstanding performance. The fundamental understanding of their physicochemical features…

Materials Science · Physics 2021-04-06 J. M. Vicent-Luna , S. Apergi , S. Tao

We perform excited-state variational Monte Carlo and diffusion Monte Carlo calculations using a simple and efficient wave function ansatz. This ansatz follows the recent variation-after-response formalism, accurately approximating a…

Strongly Correlated Electrons · Physics 2018-12-24 Nick S. Blunt , Eric Neuscamman

Quantum computing methods for excited-state calculations remain underexplored in Noisy Intermediate-Scale Quantum (NISQ) hardware, despite their critical role in photochemistry and material science. Herein, we propose a resource-efficient…

Quantum Physics · Physics 2025-06-16 Qianjun Yao , He Li

We study theoretically poly-diacetylene chains diluted in their monomer matrix. We employ the density-matrix renormalization group method (DMRG) on finite chains to calculate the ground state and low-lying excitations of the corresponding…

Strongly Correlated Electrons · Physics 2014-10-07 Gergely Barcza , William Barford , Florian Gebhard , Örs Legeza

We present two new methods for performing ab initio calculations of excited states for closed-shell systems within the in-medium similarity renormalization group (IMSRG) framework. Both are based on combining the IMSRG with simple many-body…

Nuclear Theory · Physics 2017-05-10 N. M. Parzuchowski , T. D. Morris , S. K. Bogner

The importance of singlet fission as a fundamental process with a variety of implications in energy harvesting cannot be overstated. The challenge is in characterizing the energy states of these large singlet fission molecular aggregates…

Chemical Physics · Physics 2025-09-05 Supriyo Santra , Amartya Bose , Debashree Ghosh

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

Chemical Physics · Physics 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer

The computational investigation of photochemical processes often entails the calculation of excited state geometries, energies, and energy gradients. The nuclear-electronic orbital (NEO) approach treats specified nuclei, typically protons,…

We extend our previous symmetrized path-integral molecular dynamics approach to calculate tunneling splittings of molecules in rotationally excited states. In this new formalism, the system is rigorously projected onto selected rotational…

Chemical Physics · Physics 2026-04-15 Lea Zupan , Yu-Chen Wang , Jeremy O. Richardson