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Adiabatic mixed quantum/classical molecular dynamics simulations were used to generate snapshots of the hydrated electron (e-) in liquid water at 300 K. Water cluster anions that include two complete solvation shells centered on the e- were…

Data Analysis, Statistics and Probability · Physics 2016-09-28 Ilya A. Shkrob , William J. Glover , Ross E. Larsen , Benjamin J. Schwartz

Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several…

Chemical Physics · Physics 2023-02-15 Yorick L. A. Schmerwitz , Gianluca Levi , Hannes Jónsson

We present the theoretical framework, implementation, and benchmark results for a reduced-cost relativistic equation-of-motion coupled cluster singles and doubles (EOM-CCSD) method based on state-specific frozen natural spinors (SS-FNS). In…

Near-term quantum computers are expected to facilitate material and chemical research through accurate molecular simulations. Several developments have already shown that accurate ground-state energies for small molecules can be evaluated…

Electron spins in quantum dots under coherent control exhibit a number of novel feedback processes. Here, we present experimental and theoretical evidence of a feedback process between nuclear spins and a single electron spin in a single…

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

Nuclear electric resonance (NER) spectroscopy is currently experiencing a revival as a tool for nuclear spin-based quantum computing. Compared to magnetic or electric fields, local electron density fluctuations caused by changes in the…

Quantum Physics · Physics 2025-01-30 Johannes K. Krondorfer , Andreas W. Hauser

Downfolding coupled cluster (CC) techniques are powerful tools for reducing the dimensionality of many-body quantum problems. This work investigates how ground-state downfolding formalisms can target excited states using non-Aufbau…

Chemical Physics · Physics 2023-10-24 Nicholas P. Bauman

We calculate the contribution of the decay products of excited nuclear cluster states to the event-by-event fluctuations of protons in the energy range from $\sqrt{s_{NN}}=2-5$~GeV within the statistical model. We find that the inclusion of…

Nuclear Theory · Physics 2024-12-09 Boris Tomasik , Marcus Bleicher

Phase Resolved Optical Emission Spectroscopy (PROES) measurements combined with 1d3v Particle-in-Cell/Monte Carlo Collisions (PIC/MCC) simulations are used to study the electron power absorption and excitation/ionization dynamics in…

Plasma Physics · Physics 2022-09-28 A. Derzsi , P. Hartmann , M. Vass , B. Horváth , M. Gyulai , I. Korolov , J. Schulze , Z. Donkó

Nuclear quantum effects are essential for correctly describing hydrogen-rich materials at high pressures. Superconducting hydrides and ice are prime examples of such systems, requiring the inclusion of lattice anharmonicity and nuclear…

In the realm of photochemistry, the significance of double excitations (also known as doubly-excited states), where two electrons are concurrently elevated to higher energy levels, lies in their involvement in key electronic transitions…

Chemical Physics · Physics 2024-07-15 Fábris Kossoski , Martial Boggio-Pasqua , Pierre-François Loos , Denis Jacquemin

We propose the multi-state complete-active-space second-order perturbation theory spin-orbit method (MS-CASPT2-SO) for electronic structure calculations. It is a two-step spin-orbit coupling method that does not make use of energy shifts…

Chemical Physics · Physics 2010-12-30 Zoila Barandiaran , Luis Seijo

Measurements and a theoretical interpretation of the excitation spectrum of a two-electron quantum dot fabricated on a parabolic Ga[Al]As quantum well are reported. Experimentally, excited states are found beyond the well-known lowest…

Mesoscale and Nanoscale Physics · Physics 2021-12-30 T. Ihn , C. Ellenberger , K. Ensslin , Constantine Yannouleas , Uzi Landman , D. C. Driscoll , A. C. Gossard

We present the first implementation of spin-orbit coupling effects in fully internally contracted second-order quasidegenerate N-electron valence perturbation theory (SO-QDNEVPT2). The SO-QDNEVPT2 approach enables the computations of…

Chemical Physics · Physics 2023-03-07 Rajat Majumder , Alexander Yu. Sokolov

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

Single reference coupled-cluster (CC) methods for electronic excitation are based on a biorthogonal representation (bCC) of the (shifted) Hamiltonian in terms of excited CC states, also referred to as correlated excited (CE) states, and an…

Other Condensed Matter · Physics 2012-08-07 J. Schirmer , F. Mertins

We introduce a new equation-of-motion coupled-cluster method based on a pair coupled-cluster doubles (pCCD) reference, termed frozen-pair EOM-CCSD (EOM-fpCCSD). This approach combines the computational efficiency of the pCCD ansatz with a…

Chemical Physics · Physics 2026-05-06 Katharina Boguslawski , Paweł Tecmer

We present a novel theory and implementation for computing coupled electronic and quantal nuclear subsystems on a single potential energy surface, moving beyond the standard Born-Oppenheimer (BO) separation of nuclei and electrons. We…

Chemical Physics · Physics 2021-11-15 Ziyong Chen , Jun Yang

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