Searcharxiv⌕ Search

arXiv subjects

Takeshi Sato

Publications and source records attributed to Takeshi Sato.

At least 55 records · Page 3Linked to original sources

Time-dependent optimized coupled-cluster method for multielectron dynamics

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 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 to intense-laser driven correlated electron dynamics in Ar atom is reported.

physics.chem-ph↗

Implementation of infinite-range exterior complex scaling to the time-dependent complete-active-space self-consistent-field method

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.

physics.atom-ph↗

Time-dependent Hartree-Fock study of electron-hole interaction effects on high-harmonic generation from periodic crystals

We investigate the multielectron effects on high-harmonic generation from solid-state materials using the time-dependent Hartree-Fock theory. We find qualitative change in harmonic spectra, in particular, multiple-plateau formation at significantly lower laser intensities than within the independent-electron approximation. We reveal its origin in terms of interband polarization, i.e, electron-hole polarization, enabling interband excitation at remote crystal momenta via Coulomb potential.

physics.optics↗

Fully general time-dependent multiconfiguration self-consistent-field method for the electron-nuclear Dynamics

We present the fully general time-dependent multiconfiguration self-consistent-field method to describe the dynamics of a system consisting of arbitrary different kinds and numbers of interacting fermions and bosons. The total wave function is expressed as a superposition of different configurations constructed from time-dependent spin-orbitals prepared for each particle kind. We derive equations of motion followed by configuration-interaction (CI) coefficients and spin-orbitals for general, not restricted to full-CI, configuration spaces. The present method provides a flexible framework for the first-principles theoretical study of, e.g., correlated multielectron and multinucleus quantum dynamics in general molecules induced by intense laser fields and attosecond light pulses.

physics.atom-ph↗

High-harmonic generation enhanced by dynamical electron correlation

We theoretically study multielectron effects in high-harmonic generation (HHG), using all-electron first-principles simulations for a one-dimensional (1D) model atom. In addition to usual plateau and cutoff (from a cation in the present case, since the neutral is immediately ionized), we find a prominent resonance peak far above the plateau and a second plateau extended beyond the first cutoff. These features originate from the dication response enhanced by orders of magnitude due to the action of the Coulomb force from the rescattering electron, and, hence, are a clear manifestation of electron correlation. Although the present simulations are done in 1D, the physical mechanism underlying the dramatic enhancement is expected to hold also for three-dimensional real systems. This will provide new possibilities to explore dynamical electron correlation in intense laser fields using HHG, which is usually considered to be of single-electron nature in most cases.

physics.atom-ph↗

Trajectory analysis of high-harmonic generation from periodic crystals

We theoretically study high-harmonic generation (HHG) from solids driven by intense laser pulses using a one-dimensional model periodic crystal. By numerically solving the time-dependent Schrödinger equation directly on a real-space grid, we successfully reproduce experimentally observed unique features of solid-state HHG such as the linear cutoff-energy scaling and the sudden transition from a single- to multiple-plateau structure. Based on the simulation results, we propose a simple model that incorporates vector-potential-induced intraband displacement, interband tunneling, and recombination with the valence-band hole. One key parameter is the valley-to-peak amplitude of the pulse vector potential, which determines the crystal momentum displacement during the half cycle. When the maximum peak-to-valley amplitude $A_{\rm peak}$ reaches the half width $\fracπ{a}$ of the Brillouin zone with $a$ being the lattice constant, the HHG spectrum exhibits a transition from a single- to multiple-plateau structure, and even further plateaus appear at $A_{\rm peak} = \frac{2π}{a}, \frac{3π}{a}, \cdots$. The multiple cutoff positions are given as functions of $A_{\rm peak}$ and the second maximum $A_{\rm peak}^{\prime}$, in terms of the energy difference between different bands. Using our recipe, one can draw electron trajectories in the momentum space, from which one can deduce, for example, the time-frequency structure of HHG without elaborate quantum-mechanical calculations. Finally, we reveal that the cutoff positions depend on not only the intensity and wavelength of the pulse, but also its duration, in marked contrast to the gas-phase case. Our model can be viewed as a solid-state and momentum-space counterpart of the familiar three-step model, highly successful for gas-phase HHG, and provide a unified basis to understand HHG from solid-state materials and gaseous media.

physics.optics↗

Accurate high-harmonic spectra from time-dependent two-particle reduced density matrix theory

The accurate description of the non-linear response of many-electron systems to strong-laser fields remains a major challenge. Methods that bypass the unfavorable exponential scaling with particle number are required to address larger systems. In this paper we present a fully three-dimensional implementation of the time-dependent two-particle reduced density matrix (TD-2RDM) method for many-electron atoms. We benchmark this approach by a comparison with multi-configurational time-dependent Hartree-Fock (MCTDHF) results for the harmonic spectra of beryllium and neon. We show that the TD-2RDM is very well-suited to describe the non-linear atomic response and to reveal the influence of electron-correlation effects.

physics.atom-ph↗

Multiscale simulation of polymer melt spinning by using the dumbbell model

We investigated the spinning process of a polymeric material by using a multiscale simulation method which connects the macroscopic and microscopic states through the stress and strain-rate tensor fields, by using Lagrangian particles (filled with polymer chains) along the spinning line. We introduce a large number of Lagrangian fluid particles into the fluid, each containing Np-Hookean-dumbbells to mimic the polymer chains (Np=$10^4$), which is equivalent to the upper convected Maxwell fluid in the limit that Np$\rightarrow \infty$. Depending on the Reynolds number Re, we studied the dynamical behaviors of fibers for the (a) Re =0 and (b) finite Re cases, for different draw ratios Dr, ranging from 10 to 30, and two typical Deborah numbers De=$10^{-3}$ and De=$10^{-2}$. In the limit Re$\rightarrow$ 0 (a), as the Deborah number De increases, the elastic effect makes the system stable. At finite Re (b), we found that inertial effects play an important role in determining the dynamical behavior of the spinning process, and for Dr=$10^{-2}$ the system is quite stable, at least up to a draw ratio of Dr=30. We also found that the fiber velocity and cross section area are determined solely by the draw ratio. By comparing the velocity and cross section area profiles with the end-point distribution for the dumbbell connective vectors, for dumbbells located in Lagrangian particles along typical places along the spinning line, we show that our multiscale simulation method successfully bridges the microscopic state of the system with its simultaneous macroscopic flow behavior. It is also confirmed that the present schemes gives good agreements with the results obtained by the Maxwell constitutive equation.

cond-mat.soft↗

Time-dependent complete-active-space self-consistent-field method for atoms: Application to high-harmonic generation

We present the numerical implementation of the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method [Phys. Rev. A, 88, 023402 (2013)] for atoms driven by a strong linearly polarized laser pulse. The present implementation treats the problem in its full dimensionality and introduces a gauge-invariant frozen-core approximation, an efficient evaluation of the Coulomb mean field scaling linearly with the number of basis functions, and a split-operator method specifically designed for stable propagation of stiff spatial derivative operators. We apply this method to high-harmonic generation in helium, beryllium, and neon and explore the role of electron correlations.

physics.atom-ph↗

Implementation of the multiconfiguration time-dependent Hatree-Fock method for general molecules on a multi-resolution Cartesian grid

We report a three-dimensional numerical implementation of multiconfiguration time-dependent Hartree-Fock (MCTDHF) based on a multi-resolution Cartesian grid, with no need to assume any symmetry of molecular structure. We successfully compute high-harmonic generation (HHG) of H2 and H2O. The present implementation will open a way to the first-principle theoretical study of intense-field and attosecond-pulse induced ultrafast phenomena in general molecules.

physics.comp-ph↗

A Review on Ab Initio Approaches for Multielectron Dynamics

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 action of those laser pulses. Here we review major ab initio wave-function-based numerical approaches to simulate multielectron dynamics in atoms and molecules driven by intense long-wavelength and/or ultrashort short-wavelength laser pulses. Direct solution of the time-dependent Schrödinger equation (TDSE), though its applicability is limited to He, ${\rm H}_2$, and Li, can provide an exact description and has been greatly contributing to the understanding of dynamical electron-electron correlation. Multiconfiguration self-consistent-field (MCSCF) approach offers a flexible framework from which a variety of methods can be derived to treat both atoms and molecules, with possibility to systematically control the accuracy. The equations of motion of configuration interaction coefficients and molecular orbitals for general MCSCF ansatz have recently been derived. Time-dependent extension of the $R$-matrix theory, originally develop for electron-atom collision, can realistically and accurately describe laser-driven complex multielectron atoms.

physics.atom-ph↗

Time-dependent multiconfiguration self-consistent-field method based on occupation restricted multiple active space model for multielectron dynamics in intense laser fields

The time-dependent multiconfiguration self-consistent-field method based on the occupation-restricted multiple active space model is proposed (TD-ORMAS) for multielectron dynamics in intense laser fields. Extending the previously proposed time-dependent complete-active-space self-consistent-field method [TD-CASSCF; Phys. Rev. A, {\bf 88}, 023402 (2013)], which divides the occupied orbitals into core and active orbitals, the TD-ORMAS method {\it further} subdivides the active orbitals into an arbitrary number of subgroups, and poses the {\it occupation restriction} by giving the minimum and maximum number of electrons distributed in each subgroup. This enables highly flexible construction of the configuration interaction (CI) space, allowing a large-active-space simulation of dynamics, e.g., the core excitation or ionization. The equations of motion both for CI coefficients and spatial orbitals are derived based on the time-dependent variational principle, and an efficient algorithm is proposed to solve for the orbital time derivatives. In-depth descriptions of the computational implementation are given in a readily programmable manner. The numerical application to the one-dimensional lithium hydride cluster models demonstrates that the high flexibility of the TD-ORMAS framework allows for the cost-effective simulations of multielectron dynamics, by exploiting systematic series of approximations to the TD-CASSCF method.

physics.atom-ph↗

The structure of approximate two electron wavefunctions in intense laser driven ionization dynamics

The structure of approximate two electron wavefunction is deeply investigated, both theoretically and numerically, in the strong-field driven ionization dynamics. Theoretical analyses clarify that for two electron singlet systems, the previously proposed time-dependent extended Hartree-Fock (TD-EHF) method [Phys. Rev. A 51, 3999 (1995)] is equivalent to the multiconfiguration time-dependent Hartree-Fock method with two occupied orbitals. The latter wavefunction is further transformed into the natural expansion form, enabling the direct propagation of the natural orbitals (NOs). These methods, as well as the conventional time-dependent Hartree-Fock (TDHF) method, are numerically assessed for the description of ionization dynamics of one-dimensional helium atom model. This numerical analysis (i) explains the reason behind the well-known failure of TDHF method to describe tunneling ionization, (ii) demonstrates the interpretive power of the TD-EHF wavefunction both in the original nonorthogonal and the NO-based formulations, and (iii) highlights different manifestations of the electron correlation (effect beyond the single determinant description), in tunneling ionization, high harmonic generation, and nonsequential double ionization. Possible extensions of the NO basis approach to multielectron systems are briefly discussed.

physics.atom-ph↗

Propagating two-particle reduced density matrices without wavefunctions

Describing time-dependent many-body systems where correlation effects play an important role remains a major theoretical challenge. In this paper we develop a time-dependent many-body theory that is based on the two-particle reduced density matrix (2-RDM). We develop a closed equation of motion for the 2-RDM employing a novel reconstruction functional for the three-particle reduced density matrix (3-RDM) that preserves norm, energy, and spin symmetries during time propagation. We show that approximately enforcing $N$-representability during time evolution is essential for achieving stable solutions. As a prototypical test case which features long-range Coulomb interactions we employ the one-dimensional model for lithium hydride (LiH) in strong infrared laser fields. We probe both one-particle observables such as the time-dependent dipole moment and two-particle observables such as the pair density and mean electron-electron interaction energy. Our results are in very good agreement with numerically exact solutions for the $N$-electron wavefunction obtained from the multiconfigurational time-dependent Hartree-Fock method.

physics.atom-ph↗

Analysis of strong-field enhanced ionization of molecules using Bohmian trajectories

We theoretically investigate the mechanism of enhanced ionization in two-electron molecules by analyzing Bohmian trajectories for a one-dimensional H2 in an intense laser field. We identify both types of ionizing trajectories corresponding to the ejection from the up-field and down-field cores. The trajectories of the two electrons are correlated with each other in the former while correlation is negligible in the latter. The contributions from the two ionization types, though depending on laser intensity and internuclear distance, are comparable to each other.

quant-ph↗

Time-dependent complete-active-space self-consistent field method for multielectron dynamics in intense laser fields

The time-dependent complete-active-space self-consistent-field (TD-CASSCF) method for the description of multielectron dynamics in intense laser fields is presented, and a comprehensive description of the method is given. It introduces the concept of frozen-core (to model tightly bound electrons with no response to the field), dynamical-core (to model electrons tightly bound but responding to the field), and active (fully correlated to describe ionizing electrons) orbital subspaces, allowing compact yet accurate representation of ionization dynamics in many-electron systems. The classification into the subspaces can be done flexibly, according to simulated physical situations and desired accuracy, and the multiconfiguration time-dependent Hartree-Fock (MCTDHF) approach is included as a special case. To assess its performance, we apply the TD-CASSCF method to the ionization dynamics of one-dimensional lithium hydride (LiH) and LiH dimer models, and confirm that the present method closely reproduces rigorous MCTDHF results if active orbital space is chosen large enough to include appreciably ionizing electrons. The TD-CASSCF method will open a way to the first-principle theoretical study of intense-field induced ultrafast phenomena in realistic atoms and molecules.

physics.atom-ph↗

Recent progress in silica aerogel Cherenkov radiator

In this paper, we present recent progress in the development of hydrophobic silica aerogel as a Cherenkov radiator. In addition to the conventional method, the recently developed pin-drying method for producing high-refractive-index aerogels with high transparency was studied in detail. Optical qualities and large tile handling for crack-free aerogels were investigated. Sufficient photons were detected from high-performance aerogels in a beam test.

physics.ins-det↗

D-brane Dynamics and Creations of Open and Closed Strings after Recommbination

A quantum-mechanical technique is used within the framework of U(2) super-Yang-Mills theory to investigate what happens in the process after recombination of two D-p-branes at one angle. Two types of initial conditions are considered, one of which with $p=4$ is a candidate of inflation mechanism. It is observed that the branes' shapes come to have three extremes due to localization of tachyon condensation. Furthermore, open string pairs connecting the decaying D-branes are shown to be created; most part of the released energy is used to create them. It also strongly suggests that creation of closed strings happens afterward. Closed strings as gravitational radiation from the D-branes are also shown to be created. A few speculations are also given on implications of the above phenomena for an inflation model.

hep-th↗