Perspective: Ab initio force field methods derived from quantum mechanics The Journal of Chemical Physics 148, 090901 (2018) Time-dependent coupled-cluster method with time-varying orbital functions, called time-dependent optimized coupled-cluster (TD-OCC) method, is formulated for multielectron dynamics in an intense laser field. We have successfully derived the equations of motion for CC amplitudes and orthonormal orbital functions based on the real action functional, and implemented the method including double excitations (TD-OCCD) and double and triple excitations (TD-OCCDT) within the optimized active orbitals. The present method is size extensive and gauge invariant, a polynomial cost-scaling alternative to the time-dependent multiconfiguration self-consistent-field method. The first application of the TD-OCC method of intense-laser driven correlated electron dynamics in Ar atom is reported. Published by AIP Publishing. https://doi

We present a numerical implementation of the infinite-range exterior complex scaling (irECS) [Phys. Rev. A 81, 053845 (2010)] as an efficient absorbing boundary to the time-dependent complete-active-space self-consistent field (TD-CASSCF) method [Phys. Rev. A 94, 023405 (2016)] for multielectron atoms subject to an intense laser pulse. We introduce Gauss-Laguerre-Radau quadrature points to construct discrete variable representation basis functions in the last radial finite element extending to infinity. This implementation is applied to strong-field ionization and high-harmonic generation in He, Be, and Ne atoms. It efficiently prevents unphysical reflection of photoelectron wave packets at the simulation boundary, enabling accurate simulations with substantially reduced computational cost, even under significant (≈ 50%) double ionization. For the case of a simulation of high-harmonic generation from Ne, for example, 80% cost reduction is achieved, compared to a mask-function absorption boundary.

2160-3308=20=10(3)=031070(14) 031070-1 Published by the American Physical Society involving absorption and emission of an infrared photon is extracted. Our method can be used for extraction of a phase difference between single-photon and two-photon pathways and provides a new tool for attosecond science, which is complementary to RABBITT.

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We present a numerical implementation of the time-dependent surface flux (tSURFF) method [New J. Phys. 14, 013021 (2012)], an efficient computational scheme to extract photoelectron energy spectra, to the time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method. Extending the original tSURFF method developed for single particle systems, we formulate the equations of motion for the spectral amplitude of orbital functions constutiting the TD-MCSCF wave function, from which the angle-resolved photoelectron energy spectrum, and more generally, photoelectron reduced density matrices (RDMs) are readiliy obtained. The tSURFF method applied to the TD-MCSCF wave function, in combination with an efficient absorbing boundary offered by the infinite-range exterior complex scaling, enables accurate ab initio computations of photoelectron energy spectra from multielectron systems subject to an intense and ultrashort laser pulse with a computational cost significantly reduced compared to that required in projecting the total wave function onto scattering states. We apply the present implementation to the photoionization of Ne exposed to an attosecond extreme-ultraviolet (XUV) pulse and above-threshold ionization of Ar irradiated by an intense mid-infrared laser field, demonstrating both accuracy and efficiency of the present method.

We present the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method to simulate multielectron dynamics in ultrafast intense laser fields from the first principles. While based on multiconfiguration expansion, it divides the orbital space into frozen-core (tightly bound electrons with no response to the field), dynamical-core (electrons tightly bound but responding to the field), and active (fully correlated to describe highly excited and ejected electrons) orbital subspaces. The subspace decomposition can be done flexibly, conforming to phenomena under investigation and desired accuracy. The method is gauge invariant and size extensive. Infinite-range exterior complex scaling in addition to maskfunction boundary is adopted as an efficient absorbing boundary. We show numerical examples and illustrate how to extract relevant physical quantities such as ion-

We present an implementation of the multiconfiguration time-dependent Hartree–Fock method based on the adaptive finite element method for molecules under intense laser pulses. For efficient simulations, orbital functions are propagated by a stable propagator using the short iterative Arnoldi scheme and our implementation is parallelized for distributed memory computing. This is demonstrated by simulating high-harmonic generation from a water molecule and achieves a simulation of multielectron dynamics with overwhelmingly less computational time, compared to our previous work [Sawada, R. et al. Phys. Rev. A, 2016, 93, 023434].

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