Time-Dependent Complete-Active-Space Self-Consistent-Field Method for Ultrafast Intense Laser Science

Sato, Takeshi; Orimo, Yuki; Teramura, Takuma; Tugs, Oyunbileg; Ishikawa, Kenichi L.

doi:10.1007/978-3-030-03786-4_8

Cited by 11 publications

(12 citation statements)

References 77 publications

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“…TD-CI electron dynamics have been used to model photoionization, ,− ,,− ,,, linear spectroscopies, ,,,,, and nonlinear optical responses. ,,,,,, Time-dependent configuration interaction singles (TD-CIS) is the most commonly used multiconfigurational approach. TD-CIS is particularly useful when the underlying chemical processes are mostly driven by single-electron dynamics, such those in linear optical response and photoionization.…”

Section: Theory Of Real-time Time-dependent Electronic Structure Methodsmentioning

confidence: 99%

“…Recent years have also seen the development of TD-CASSCF, where the wave function obeys the time-dependent variational principle by allowing variations in both the CI coefficients and the orbitals; ,,,, this approach contrasts with TD-CASCI wherein the orbitals remain fixed. This technique has also been extended to the RAS partitioning, allowing a detailed analysis of the role that multielectron excitations play in the description of nonlinear properties, as well as the study of high harmonic generation spectra and ionization of carbon and beryllium atoms. , …”

Section: Theory Of Real-time Time-dependent Electronic Structure Methodsmentioning

confidence: 99%

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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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Section: Theory Of Real-time Time-dependent Electronic Structure Methodsmentioning

confidence: 99%

Section: Theory Of Real-time Time-dependent Electronic Structure Methodsmentioning

confidence: 99%

Real-Time Time-Dependent Electronic Structure Theory

et al. 2020

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“…Among the theoretical approaches capable to account for ME effects in strong-field processes are the time-dependent density-functional theory [34] (see Ref. [35] for a textbook treatment), multiconfiguration time-dependent Hartree-Fock theory [36,37], timedependent restricted-active-space self-consistent-field theory [38], time-dependent completeactive-space self-consistent-field theory [39], time-dependent R-matrix theory [40,41], Rmatrix method with time-dependence [42,43], time-dependent configuration-interactionsingles [44,45], time-dependent restricted-active space configuration-interaction methods [46,47], time-dependent analytical R-matrix theory [48], and various semiclassical models (see, e.g., Refs. [26][27][28][29][30]32]).…”

Section: Introductionmentioning

confidence: 99%

Multielectron polarization effects in strong-field ionization: Narrowing of momentum distributions and imprints in interference structures

2018

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We extend the semiclassical two-step model [Phys. Rev. A 94, 013415 (2016)] to include a multielectron polarization-induced dipole potential. Using this model we investigate the imprints of multielectron effects in the momentum distributions of photoelectrons ionized by a linearly polarized laser pulse. We predict narrowing of the longitudinal momentum distributions due to electron focusing by the induced dipole potential. We show that the polarization of the core also modifies interference structures in the photoelectron momentum distributions. Specifically, the number of fanlike interference structures in the low-energy part of the electron momentum distribution may be altered. We analyze the mechanisms underlying this interference effect. The account of the multielectron dipole potential seems to improve the agreement between theory and experiment. * n79@narod.ru

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“…In order to solve the scaled TDSE (4) numerically, we employ the MCTDHF method [39,40,[44][45][46][47]. In the MCTDHF method, the two-electron wave function is expanded in…”

Section: B Mctdhfmentioning

confidence: 99%

Static-field ionization model of He-like ions for diagnostics of light-field intensity

2020

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We study static-field ionization of He-like ions with nuclear charge number in the range of 2 ≤ Z ≤ 36. Both the tunneling and over-the-barrier regimes are considered. We calculate the ionization rates by three approximate methods: a fitting formula based on the Perelemov-Popov-Terent'ev (PPT) formula, a perturbative expansion in powers of 1/Z, and a single-active electron approximation, and compare them with reference ionization rates computed by the multiconfiguration time-dependent Hartree-Fock (MCTDHF) approach. The relative deviation of the rates computed by the PPT-based fitting formula and the third-order perturbation theory from the rates computed by the MCTDHF approach is found to be around 10%. We discuss quantitatively the contribution from the exchange interaction during the ionization by comparing the single-active electron rates and the reference rates in which multielectron effects are included. We find that a single-active electron approximation, where the exchange interaction is neglected, results in the overestimation of the ionization rates by 30% for He and 2% for He-like Kr, showing that the magnitude of the effect of the exchange interaction scales approximately as 1/Z.

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Time-Dependent Complete-Active-Space Self-Consistent-Field Method for Ultrafast Intense Laser Science

Cited by 11 publications

References 77 publications

Real-Time Time-Dependent Electronic Structure Theory

Real-Time Time-Dependent Electronic Structure Theory

Multielectron polarization effects in strong-field ionization: Narrowing of momentum distributions and imprints in interference structures

Static-field ionization model of He-like ions for diagnostics of light-field intensity

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