Generalized Hartree–Fock with Nonperturbative Treatment of Strong Magnetic Fields: Application to Molecular Spin Phase Transitions

Sun, Shichao; Williams‐Young, David B.; Stetina, Torin F.; Li, Xiaosong

doi:10.1021/acs.jctc.8b01140

Cited by 45 publications

(79 citation statements)

References 68 publications

(94 reference statements)

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“…In this work, the time‐independent Hamiltonian is cast in a set of complex London orbitals within the complex generalized Hartree‐Fock (ℂ‐GHF) framework. This framework allows for the variational treatment of non‐collinear spin and magnetic field perturbations . Since the theoretical framework of ℂ‐GHF with London orbitals has been recently developed, we only present a brief review of the method.…”

Section: Methodsmentioning

confidence: 99%

“…the orbital‐Zeeman term, may vary with the choice of the gauge origin of the external electromagnetic field . In order to correct for this problem, the use of London orbitals provide a complex plane‐wave augmentation to atom‐centered basis sets, which preserve gauge‐origin independence, known as gauge‐including atomic orbitals (GIAO) . Recent work has established the evaluation of one and two electron integrals using London orbitals, introducing the finite magnetic field non‐perturbatively, and also implementations of complex generalized Hartree‐Fock .…”

Section: Introductionmentioning

confidence: 99%

“…In order to correct for this problem, the use of London orbitals provide a complex plane‐wave augmentation to atom‐centered basis sets, which preserve gauge‐origin independence, known as gauge‐including atomic orbitals (GIAO) . Recent work has established the evaluation of one and two electron integrals using London orbitals, introducing the finite magnetic field non‐perturbatively, and also implementations of complex generalized Hartree‐Fock . In this work, we present a linear response time‐dependent complex generalized Hartree‐Fock method for calculating magneto‐optical spectra of atomic and molecular systems, with a focus on understanding how spectroscopic signals change in the presence of a uniform magnetic field.…”

Section: Introductionmentioning

confidence: 99%

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Modeling Magneto‐Photoabsorption Using Time‐Dependent Complex Generalized Hartree‐Fock

et al. 2019

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Magneto-optical spectroscopy provides a glimpse into the hidden electronic structure of molecules and materials that normally cannot be resolved with regular optical absorption spectroscopy. The magneto-optical signal is difficult to simulate computationally due to the necessity of modeling perturbations from both uniform magnetic and oscillating electric fields. In this work, we introduce a time-dependent complex generalized Hartree-Fock framework for calculating electronic magneto-optical spectra of atomic and molecular systems. Complexvalued gauge including atomic orbitals are used in a nonperturbative treatment of the uniform magnetic field. The magneto-photoabsorption spectra of atomic alkalis and aromatic systems are investigated with a focus on understanding how spectroscopic signals change in the presence of a uniform magnetic field. Methodology Magneto-Optical HamiltonianIn the non-relativistic framework, the interaction of an electron with external fields, defined by their vector (A i ) and scalar (U i )[a] T.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Modeling Magneto‐Photoabsorption Using Time‐Dependent Complex Generalized Hartree‐Fock

et al. 2019

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“…For the formation of the GIAO Fock matrix, the magnetic field manifests both as explicit terms added to the spin component of the Fock matrix as well as an implicit dependence of the CGTO basis function through the addition of a complex phase factor,

χ^{CGTO} ((), boldr - boldR) \mapsto \exp ((), \frac{i}{2} ((), boldR \times boldB) \cdot ((), boldr - boldR)) χ^{CGTO} ((), boldr - boldR)

where χ CGTO is a CGTO centered at R and B is the external magnetic field. In addition, ChronusQ includes orbital–Zeeman, spin–Zeeman, and diamagnetic field interactions of the nonrelativistic Pauli Hamiltonian in the GIAO methods . GIAO Fock matrices may be formed directly in the atomic orbital (AO) basis through a generalization of the direct SCF method of Almlöf, et al for complex integrals.…”

Section: Current Program Featuresmentioning

confidence: 99%

“…GIAO Fock matrices may be formed directly in the atomic orbital (AO) basis through a generalization of the direct SCF method of Almlöf, et al for complex integrals. To the best of the authors' knowledge, ChronusQ contains the only publicly available implementation of two‐component spinor GIAO methods at this time.…”

Section: Current Program Featuresmentioning

confidence: 99%

The Chronus Quantum software package

Williams‐Young

Petrone

Sun

et al. 2019

WIREs Comput Mol Sci

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The Chronus Quantum (ChronusQ) software package is an open source (under the GNU General Public License v2) software infrastructure which targets the solution of challenging problems that arise in ab initio electronic structure theory. Special emphasis is placed on the consistent treatment of time dependence and spin in the electronic wave function, as well as the inclusion of relativistic effects in said treatments. In addition, ChronusQ provides support for the inclusion of uniform finite magnetic fields as external perturbations through the use of gauge‐including atomic orbitals. ChronusQ is a parallel electronic structure code written in modern C++ which utilizes both message passing implementation and shared memory (OpenMP) parallelism. In addition to the examination of the current state of code base itself, a discussion regarding ongoing developments and developer contributions will also be provided. This article is categorized under: Software > Quantum Chemistry Electronic Structure Theory > Ab Initio Electronic Structure Methods Electronic Structure Theory > Density Functional Theory

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Real-Time Time-Dependent Electronic Structure Theory

et al. 2020

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Real-time electronic structure methods provide an unprecedented view of electron dynamics and ultrafast spectroscopy on the atto-and femtosecond time scale with vast potential to yield new insights into the electronic behavior of molecules and materials. In this Review, we discuss the fundamental theory underlying various real-time electronic structure methods as well as advantages and disadvantages of each. We give an overview of the numerical techniques that are widely used for real-time propagation of the quantum electron dynamics with an emphasis on Gaussian basis set methods. We also showcase many of the chemical applications and scientific advances made by using real-time electronic structure calculations and provide an outlook of possible new directions. CONTENTS 1. Introduction 9951 2. Theory of Real-Time Time-Dependent Electronic Structure Methods 9953 2.1. Real-Time Time-Dependent Hartree−Fock and Density Functional Theory 9953 2.1.1. The Adiabatic Approximation in TDDFT 9955 2.1.2. Accuracy of TDHF and TDDFT 9956 2.2. Real-Time Time-Dependent Semi-Empirical Methods 9957 2.3. Real-Time Time-Dependent Configuration-Interaction Methods 9957 2.4. Real-Time Time-Dependent Coupled-Cluster Methods 9958 2.5. Real-Time Time-Dependent Two-Component and Relativistic Methods 9961 2.6. Real-Time Methods in Complex and Nonequilibrium Environments 9962 3. Numerical Techniques 9963 3.1. Basis Set Representations 9963 3.2. Time Propagation Methods 9963 3.3. Signal Processing 9964 4. Application of Real-Time Time-Dependent Electronic Structure Methods 9966 4.1. UV/Vis Spectroscopy 9966 4.2. X-ray Absorption Spectroscopy 9967 4.3. Excited State Absorption and Emission 9967 4.4. Charge Transfer, Plasmon Excitations, and Exciton Dynamics 9968 4.5. Nonlinear Properties and Multidimensional Spectroscopy 9971 4.6. Spin and Magnetization Dynamics 4.7. Electronic Circular Dichroism and Magnetic Circular Dichroism 4.8. Electron Dynamics in Strong Fields 5. Outlook

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Generalized Hartree–Fock with Nonperturbative Treatment of Strong Magnetic Fields: Application to Molecular Spin Phase Transitions

Cited by 45 publications

References 68 publications

Modeling Magneto‐Photoabsorption Using Time‐Dependent Complex Generalized Hartree‐Fock

Modeling Magneto‐Photoabsorption Using Time‐Dependent Complex Generalized Hartree‐Fock

The Chronus Quantum software package

Real-Time Time-Dependent Electronic Structure Theory

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