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The projection-based quantum embedding method is applied to electronically excited states of valence, Rydberg, and charge-transfer character, valence- and core-ionized states, as well as bound and temporary radical anions. We embed…

Chemical Physics · Physics 2021-06-10 Valentina Parravicini , Thomas-C. Jagau

Metal Organic Frameworks (MOFs) are promising materials to help mitigate the effects of global warming by selectively absorbing $\text{CO}_{2}$ for direct capture. Accurate quantum chemistry simulations are a useful tool to help select and…

The oxygen vacancy formation energy ($\Delta E_{vf}$) governs defect dynamics and is a useful metric to perform materials selection for a variety of applications. However, density functional theory (DFT) calculations of $\Delta E_{vf}$ come…

The structure of oxide-supported metal nanoclusters plays an essential role in their sharply enhanced catalytic activity over bulk metals. Simulations provide the atomic-scale resolution needed to understand these systems. However, the…

Materials Science · Physics 2024-05-22 Benjamin X. Shi , David J. Wales , Angelos Michaelides , Chang Woo Myung

We perform full-potential screened-hybrid density-functional theory (DFT) calculations to compare the thermodynamic stability of neutral and charged states of the surface oxygen vacancy at the rutile TiO$_2$(110) surface. Solid-state…

Materials Science · Physics 2015-08-19 Daniel Berger , Harald Oberhofer , Karsten Reuter

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

Excited states exhibiting double excitation character are notoriously difficult to model using conventional single-reference methods, such as adiabatic time-dependent density-functional theory (TD-DFT) or equation-of-motion coupled cluster…

The study of isolated defects in solids is a natural target for classical or quantum embedding methods that treat the defect at a high level of theory and the rest of the solid at a lower level of theory. Here, in the context of…

Materials Science · Physics 2023-01-25 Bryan T. G. Lau , Brian Busemeyer , Timothy C. Berkelbach

Density functional theory (DFT) is the most widely used method for calculating molecular properties; however, its accuracy is often insufficient for quantitative predictions. Coupled-cluster (CC) theory is the most successful method for…

Cavity quantum electrodynamics (QED) generalizations of time-dependent (TD) density functional theory (DFT) and equation-of-motion (EOM) coupled-cluster (CC) theory are used to model small molecules strongly coupled to optical cavity modes.…

Chemical Physics · Physics 2023-07-19 Marcus D. Liebenthal , Nam Vu , A. Eugene DePrince

We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by…

Chemical Physics · Physics 2024-12-23 Stefano Battaglia , Max Rossmannek , Vladimir V. Rybkin , Ivano Tavernelli , Jürg Hutter

The equation of motion coupled cluster singles and doubles model (EOM-CCSD) is an accurate, black-box correlated electronic structure approach to investigate electronically excited states and electron attachment or detachment processes. It…

Chemical Physics · Physics 2023-09-18 Loïc Halbert , Andre Severo Pereira Gomes

An efficient simulation framework is proposed to model collective emission in disordered ensembles of quantum emitters. Using a cumulant expansion approach, the computational complexity scales polynomially as opposed to exponentially with…

Optics · Physics 2025-12-17 Qingyi Zhou , Wenxin Wu , Maryam Zahedian , Zongfu Yu , Jennifer T. Choy

Valence excitation spectra are computed for all deep-center silicon-vacancy defect types in 3C, 4H, and 6H silicon carbide (SiC) and comparisons are made with literature photoluminescence measurements. Nuclear geometries surrounding the…

Chemical Physics · Physics 2018-03-14 Jesse J. Lutz , Xiaofeng F. Duan , Larry W. Burggraf

Quantum embedding schemes have the potential to significantly reduce the computational cost of first principles calculations, whilst maintaining accuracy, particularly for calculations of electronic excitations in complex systems. In this…

Materials Science · Physics 2022-03-10 Joseph C. A. Prentice

We aim to understand the formation of cloud condensation nuclei in oxygen-rich substellar atmospheres by calculating fundamental properties of the energetically most favorable vanadium oxide molecules and clusters. A hierarchical…

Earth and Planetary Astrophysics · Physics 2024-10-02 Helena Lecoq-Molinos , David Gobrecht , J. P. Sindel , Christiane Helling , Leen Decin

Orbital-free density functional theory (OFDFT) offers a challenging way of electronic-structure calculations scaled as $\mathcal{O}(N)$ computation for system size $N$. We here develop a scheme of the OFDFT calculations based on the…

Computational Physics · Physics 2021-09-06 Fumihiro Imoto , Masatoshi Imada , Atsushi Oshiyama

Computational high-throughput studies, especially in research on high-entropy materials and catalysts, are hampered by high-dimensional composition spaces and myriad structural microstates. They present bottlenecks to the conventional use…

Materials Science · Physics 2024-03-18 Christian M. Clausen , Jan Rossmeisl , Zachary W. Ulissi

Diamond defects are among the most promising qubits. Modelling their properties through accurate quantum mechanical simulations can further their development into robust units of information. We use the recently developed capped density…

Quantum Physics · Physics 2026-03-23 John Mark P. Martirez

We study theoretically large metal clusters containing vacancies. We propose an approach, which combines the Kohn-Sham results for monovacancy in a bulk of metal and analytical expansions in small parameters $c_{v}$ (relative concentration…

Mesoscale and Nanoscale Physics · Physics 2018-02-14 V. V. Pogosov , V. I. Reva
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