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Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell…

化学物理 · 物理学 2024-05-07 Kalman Szenes , Maximilian Moerchen , Paul Fischill , Markus Reiher

An accurate description of strong correlation is quintessential for the exploration of emerging chemical phenomena. While near-term variational quantum algorithms provide a theoretically scalable framework for quantum chemical problems, the…

量子物理 · 物理学 2025-10-20 Arpan Choudhury , Sonaldeep Halder , Rahul Maitra , Debashree Ghosh

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

化学物理 · 物理学 2020-04-16 Christopher J. Stein , Markus Reiher

Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required…

化学物理 · 物理学 2016-09-08 Christopher J. Stein , Vera von Burg , Markus Reiher

We propose a multiconfigurational hybrid density-functional theory which rigorously combines a multiconfiguration self-consistent-field calculation with a density-functional approximation based on a linear decomposition of the…

化学物理 · 物理学 2012-08-20 Kamal Sharkas , Andreas Savin , Hans Jørgen Aa. Jensen , Julien Toulouse

The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

We present a new hybrid multiconfigurational method based on the concept of range-separation that combines the density matrix renormalization group approach with density functional theory. This new method is designed for the simultaneous…

Solvation effect might have a tremendous influence on chemical reactions. However, precise quantum chemistry calculations are most often done either in vacuum neglecting the role of the solvent or using continuum solvent model ignoring its…

化学物理 · 物理学 2020-07-14 Guillaume Jeanmairet , Maximilien Levesque , Daniel Borgis

While the treatment of chemically relevant systems containing hundreds or even thousands of electrons remains beyond the reach of quantum devices, the development of quantum-classical hybrid algorithms to resolve electronic correlation…

The accurate electronic structure calculation for strongly correlated chemical systems requires an adequate description for both static and dynamic electron correlation, and is a persistent challenge for quantum chemistry. In order to…

强关联电子 · 物理学 2020-08-18 Yinxuan Song , Yifan Cheng , Yingjin Ma , Haibo Ma

We present an efficient \textit{ab initio} method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to…

强关联电子 · 物理学 2014-07-01 Y. X. Yao , J. Liu , C. Liu , W. C. Lu , C. Z. Wang , K. M. Ho

We use density-matrix renormalization group, applied to a one-dimensional model of continuum Hamiltonians, to accurately solve chains of hydrogen atoms of various separations and numbers of atoms. We train and test a machine-learned…

强关联电子 · 物理学 2016-12-28 Li Li , Thomas E. Baker , Steven R. White , Kieron Burke

Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…

量子物理 · 物理学 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

Efficiently recovering dynamic correlation in strongly correlated systems without incurring prohibitive computational costs remains a central challenge in quantum chemistry. In this Perspective, we review and benchmark methods capable of…

化学物理 · 物理学 2026-05-22 Michał Hapka , Aleksandra Tucholska , Katarzyna Pernal

We investigate fully self-consistent multiscale quantum-classical algorithms on current generation superconducting quantum computers, in a unified approach to tackle the correlated electronic structure of large systems in both quantum…

The development of numerical methods capable of simulating realistic materials with strongly correlated electrons, with controllable errors, is a central challenge in quantum many-body physics. Here we describe how a hybrid between…

强关联电子 · 物理学 2015-04-23 Alexei A. Kananenka , Emanuel Gull , Dominika Zgid

The electron pair approximation offers a resource efficient variational quantum eigensolver (VQE) approach for quantum chemistry simulations on quantum computers. With the number of entangling gates scaling quadratically with system size…

Many chemical systems cannot be described by quantum chemistry methods based on a singlereference wave function. Accurate predictions of energetic and spectroscopic properties require a delicate balance between describing the most important…

化学物理 · 物理学 2018-06-12 Erik Donovan Hedegård , Julien Toulouse , Hans Jørgen Aagaard Jensen

Complexity in strongly correlated electron systems is analyzed by considering decoherence process between the localized state, |L> and the itinerant state, |I>. The coherent superposition state of a|I> + b|L> decoheres to the pointer states…

强关联电子 · 物理学 2011-01-04 Byung Gyu Chae

We present an efficient approach to the electron correlation problem that is well-suited for strongly interacting many-body systems, but requires only mean-field-like computational cost. %which is based on orbital optimization of electron…

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