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The development of a novel exact two-component (X2C) scheme with the inclusion of the picture-change correction for the fluctuation potential, the X2Ccorr scheme, is reported, hereby establishing a hierarchy of X2C schemes with systematic…

Chemical Physics · Physics 2026-03-02 Xubo Wang , Sen Wang , Yixuan Wu , Lan Cheng

Based on our previous study [S. Wang $\textit{et al}$. J. Chem. Phys. $\textbf{153}$, 184102 (2020)], we generalize the theory of molecular emission power spectra (EPS) from one molecule to multichromophoric systems in the framework of…

Chemical Physics · Physics 2024-12-19 Siwei Wang , Jia-Liang Huang , Liang-Yan Hsu

We extend the recently introduced phaseless auxiliary-field quantum Monte Carlo (QMC) approach to any single-particle basis, and apply it to molecular systems with Gaussian basis sets. QMC methods in general scale favorably with system…

Computational Physics · Physics 2007-05-23 W. A. Al-Saidi , Shiwei Zhang , Henry Krakauer

In parallel with the evolution of femtosecond and attosecond laser as well as free-electron laser technology, a variety of theoretical methods have been developed to describe the behavior of atoms, molecules, clusters, and solids under the…

Atomic Physics · Physics 2015-11-12 Kenichi L. Ishikawa , Takeshi Sato

In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…

Density matrix embedding theory (DMET) is a fully quantum-mechanical embedding method which shows great promise as a method of defeating the inherent exponential cost scaling of multiconfigurational wave function-based calculations by…

Chemical Physics · Physics 2019-02-07 Matthew R. Hermes , Laura Gagliardi

We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of…

Chemical Physics · Physics 2020-12-11 Linda Goletto , Tommaso Giovannini , Sarai D. Folkestad , Henrik Koch

To obtain the basis for combining various many-body techniques to QED in a consistent manner, we investigate the theory of quantum electrodynamical self-consistent fields. The reserch interest was born mainly of the electronic structure…

Atomic Physics · Physics 2007-05-23 Tadafumi Ohsaku

The ever-growing intersection of quantum electrodynamics (QED) and molecular processes has shown remarkable and unanticipated advancements in altering molecular properties and reactivity by exploiting light-matter couplings. In recent…

Chemical Physics · Physics 2023-11-09 Xinyang Li , Yu Zhang

Single-molecule magnets (SMMs) are promising candidates for molecular-scale data storage and processing due to their strong magnetic anisotropy and long spin relaxation times. However, as temperature rises, interactions between electronic…

Materials Science · Physics 2024-12-11 Soumi Haldar , Lorenzo A. Mariano , Alessandro Lunghi , Laura Gagliardi

The time-dependent restricted-active-space self-consistent-field (TD-RASSCF) method is formulated based on the TD variational principle. In analogy with the configuration-interaction singles (CIS), singles-and-doubles (CISD),…

Quantum Physics · Physics 2014-06-26 Haruhide Miyagi , Lars Bojer Madsen

We investigate the method to combine the techniques of quantum chemisty with QED. In our theory, we treat the N-electron system and the Dirac sea on an equal footing; we regard both of them as the dynamical degrees of freedom of a many-body…

Chemical Physics · Physics 2007-05-23 Tadafumi Ohsaku , Kizashi Yamaguchi

This work constructs an advanced force field, the Completely Multipolar Model (CMM), to quantitatively reproduce each term of an energy decomposition analysis (EDA) for aqueous solvated alkali metal cations and halide anions and their ion…

Chemical Physics · Physics 2024-10-14 J. P. Heindel , L. Kim , M. Head-Gordon , T. Head-Gordon

Kohn-Sham density functional theory (KS-DFT) has found widespread application in accurate electronic structure calculations. However, it can be computationally demanding especially for large-scale simulations, motivating recent efforts…

Computational Physics · Physics 2024-06-25 Feitong Song , Ji Feng

The localized active space self consistent field (LASSCF) method factorizes a complete active space (CAS) wave function into an antisymmetrized product of localized active space wave function fragments. Correlation between fragments is then…

Chemical Physics · Physics 2024-03-26 Valay Agarawal , Daniel King , Matthew R. Hermes , Laura Gagliardi

This review presents a concise, yet comprehensive discussion on the evolution of theoretical methods employed to determine the ground and excited states of molecules in weak and strong magnetic fields. The weak-field cases have been studied…

Atomic and Molecular Clusters · Physics 2021-05-31 Mihir Date , R. W. A Havenith

Strong-field quantum electrodynamics (SF-QED) plays a crucial role in ultraintense laser matter interactions, and demands sophisticated techniques to understand the related physics with new degrees of freedom, including spin angular…

Taking N2 and O2 as examples, we theoretically study the post-ionization dynamics of molecules in strong laser fields using a density matrix method for open systems, focusing on the effect of ionization-produced coherence on the dynamics of…

Atomic Physics · Physics 2024-12-12 Shan Xue , Wenli Yang , Ping Li , Yuxuan Zhang , Pengji Ding , Song-Feng Zhao , Hongchuan Du , Anh-Thu Le

Upcoming high-intensity laser systems will be able to probe the quantum-induced nonlinear regime of electrodynamics. So far unobserved QED phenomena such as the discovery of a nonlinear response of the quantum vacuum to macroscopic…

High Energy Physics - Phenomenology · Physics 2009-10-29 Holger Gies

Iron-sulfur clusters comprise an important functional motif of the catalytic centers of biological systems, capable of enabling important chemical transformations at ambient conditions. This remarkable capability derives from a notoriously…