arXiv subjects

Shunsuke Yamada

Publications and source records attributed to Shunsuke Yamada.

16 recordsLinked to original sources

arXiv2026

SALMON 2.3: Implementation of divide-and-conquer ground-state initialization for large-scale real-time TDDFT

In large-scale real-time time-dependent density functional theory (TDDFT), preparing the ground-state electronic structure can be more expensive than the subsequent time propagation, limiting simulations of nonequilibrium electron dynamics in realistic systems containing thousands of atoms. This bottleneck is especially important for disordered materials, liquids, nanostructures, and heterogeneous condensed-matter systems, where nonlinear and strong-field phenomena such as high-harmonic generation and light-induced phase transitions require explicit real-time treatment. SALMON is an open-source first-principles code for light-matter interaction simulations based on real-time TDDFT on real-space grids, supporting massively parallel calculations with MPI combined with OpenMP or GPU acceleration. In SALMON 2.3, we implement a divide-and-conquer density functional theory (DC-DFT) scheme and combine it with a postprocessing method that reconstructs spatially extended Kohn-Sham orbitals of the entire system. These reconstructed global orbitals are used directly as initial states for the standard real-time, real-space TDDFT module of SALMON. The resulting workflow connects efficient DC-DFT ground-state preparation to conventional real-time TDDFT. The DC-DFT self-consistent-field procedure exhibits linear scaling with system size, addressing a major bottleneck in large-scale electron-dynamics simulations while retaining the robustness and broad applicability of SALMON's established time-propagation scheme. We describe the computational procedure, parallelization strategy, and input/output design. Weak-scaling tests using Si supercells on Fugaku confirm the linear-scaling behavior. Accuracy tests for a 512-atom amorphous Si system and a bulk H2O liquid system containing 4134 atoms demonstrate that the workflow enables practical large-scale real-time TDDFT simulations.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast Spin Injection in Graphene via Dynamical Carrier Filtering at Transition Metal Dichalcogenide Interfaces

We report a real-time first-principles study of ultrafast spin injection in a WSe$_2$-graphene heterobilayer under circularly polarized laser irradiation, using time-dependent density functional theory. Contrary to conventional expectations, spin transfer into graphene is not a passive process but is actively driven by spin-selective carrier filtering at the interface. Spin-polarized carriers generated in the WSe$_2$ layer induce a preferential migration of opposite-spin carriers from graphene, which results in net spin magnetization in graphene. This process is governed by interlayer band offsets, density-of-state asymmetry, and Pauli blocking. These findings indicate a microscopic mechanism of spin injection in non-magnetic systems and identify a guiding principle for the design of ultrafast opto-spintronic functionalities in van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

SALMON VR: Visualizing Light-Matter Dynamics

This study presents SALMON VR, a visualization program designed to visualize the time evolution of electronic density changes and vector potentials in virtual reality (VR) space. The time-series electronic density data computed by SALMON are stored in CUBE format. SALMON VR processes these data to construct isosurfaces of electronic density variations and two-dimensional representations of vector potentials. Equipped with a user-friendly interface using VR technology, the program is available in two versions: one for the Meta Quest 3 head-mount display (Meta Platforms Inc., California) and one for PCs. Atoms are displayed as spheres of different sizes and colors according to their elemental properties. This visual representation facilitates a deeper understanding of the complex interactions between light and electrons. Users can easily manipulate the isosurface values, speed of animation, and color map of the vector potential. SALMON VR will enable researchers and educators to enhance their understanding of physical phenomena and improve engagement in learning environments.

cond-mat.mtrl-sci↗

arXiv2024

Saturable absorption in highly excited silicon and its suppression at the surface

Nonlinear electronic excitation in laser-irradiated silicon at finite electron temperatures is numerically investigated by first-principles calculations based on the time-dependent density functional theory. In bulk silicon at finite temperatures under near-infrared laser irradiation, we found that the absorbed energy is saturated when using a certain laser intensity even with a few-cycle pulse. Although one-photon processes of conduction-to-conduction and valence-to-valence transitions are dominant at such a laser intensity, the Pauli blocking inhibits further one-photon transition. With higher intensities, multi-photon excitation across the bandgap overwhelms the one-photon excitation and the saturable absorption disappears. At the surface of finite-temperature silicon, the Pauli blocking is suppressed by the symmetry breaking and the absorbed energy is relatively enhanced from the energy of the saturable absorption in the bulk region.

cond-mat.mtrl-sci↗

arXiv2024

Wide-bandgap optical materials for high-harmonics generation at the nanoscale

High-order harmonics generation (HHG) is the only process that enables table-top-size sources of extreme-ultraviolet (XUV) light. The HHG process typically involves light interactions with gases or plasma-material phases that hinder wider adoption of such sources. This motivates the research in HHG from nanostructured solids. Here we investigate theoretically material platforms for HHG at the nanoscale using first-principle supercomputer simulations. We reveal that wide bandgap semiconductors, aluminium nitride AlN and silicon nitride SiN, are highly promising for XUV light generation when compared to one of the most common nonlinear nanophotonic material -- silicon. In our calculations we assume excitation with 100 fs pulse duration, 10^13 W/cm^2 peak power and 800 nm central wavelength. We demonstrate that in AlN material the interplay between the crystal symmetry and the incident light direction and polarization can enable the generation of both even and odd harmonics. Our results should advance the developments of high-harmonics generation of XUV light from nanostructured solids.

physics.optics↗

arXiv2023

Subcycle control of valley-selective excitation via dynamical Franz-Keldysh effect in WSe$_2$ monolayer

This study performed first-principles calculations based on the time-dependent density functional theory to control the valley degree of freedom relating to the dynamical Franz-Keldysh effect (DFKE) in a monolayer of transition metal dichalcogenide. By mimicking the attosecond transient absorption spectroscopy, we performed numerical pump-probe experiments to observe DFKE around the $K$ or $K'$ valley in WSe$_2$ monolayer with a linearly-polarized pump field and a circularly-polarized probe pulse. We found that the circularly-polarized probe pulse with a given helicity can selectively observe the transient conductivity modulated by DFKE in each valley. The transient conductivity and excitation probability around each valley oscillate with the pump field frequency $Ω$. The phases of the $Ω$ oscillation for the $K$ and $K'$ valleys are opposite to each other. Furthermore, the pump-driven DFKE alters the absorption rate of WSe$_2$ monolayer and yields the valley-dependent $Ω$ oscillation of the electron excitation induced by the pump plus probe field. With a simplified two-band model, we identified the $Ω$ oscillation of the off-diagonal conductivity caused by the band asymmetry around the valleys as the physical mechanism responsible for the valley-selective DFKE.

cond-mat.mtrl-sci↗

arXiv2023

Enhancement of valley selective excitation by a linearly polarized two-color laser pulse

Here we proposed the valley selective excitations via a two-color (\ensuremathω + \ensuremath{2ω}) laser field, made by superimposing two linearly polarized pulses at frequencies \ensuremathω and \ensuremath{2ω}. We have studied the intensity ratio between a few-cycle pulse of \ensuremathω and \ensuremath{2ω} laser, and its enhancement factor by employing the time-dependent first-principle calculations. The valley polarization depends on the carrier envelope phases (CEPs) of pulses and the intensity ratio $I_ω/I_{2ω}$. We found that the two-color field enhances the valley polarization as much as 1.2 times larger than the single-color pulse. The maximum valley asymmetry is achieved for the intensity ratio $I_ω/I_{2ω}$ of 36 with the relative CEP of \ensuremathπ. In our previous work, we found that the asymmetric vector potential induces the valley polarization (Phys. Rev. B 105,115403 (2022)). In this work, we find that the asymmetry of the electric field modulates the valley polarization. Our two-color scheme offers a new path toward the optical control of valley pseudospins. \end{abstract}

physics.optics↗

arXiv2022

Propagation effects in high-harmonic generation from dielectric thin films

Theoretical investigation is conducted of high-order harmonic generation (HHG) in silicon thin films to elucidate the effect of light propagation in reflected and transmitted waves. The first-principles simulations are performed of the process in which an intense pulsed light irradiates silicon thin films up to 3 $μ$m thickness. Our simulations are carried within the time-dependent density functional theory (TDDFT) with the account of coupled dynamics of the electromagnetic fields and the electronic motion. It was found that the intensity of transmission HHG gradually decreases with the thickness, while the reflection HHG becomes constant from a certain thickness. Detailed analyses show that transmission HHG have two origins: the HHG generated near the front edge and propagating to the back surface, and that generated near the back edge and emitted directly. The dominating mechanism of the transmission HHG is found to depend on the thickness of the thin film and the frequency of the HHG. At the film thickness of 1 $μ$m, the transmission HHG with the frequency below 20 eV is generated near the back edge, while that with the frequency above 20 eV is generated near the front edge and propagates from there to the back surface.

cond-mat.mtrl-sci↗

arXiv2022

High order harmonic generation in semiconductors driven at near- and mid-IR wavelengths

We study high order harmonics generation (HHG) in crystalline silicon and diamond subjected to near and mid-infrared laser pulses. We employ time-dependent density functional theory and solve the time-dependent Kohn-Sham equation in the single-cell geometry. We demonstrate that clear and clean HHG spectra can be generated with careful selection of the pulse duration. In addition, we simulate dephasing effects in a large silicon super-cell through displacement of atomic positions prepared by a molecular dynamics simulation. We compare our results with the previous calculations by Floss et al. [arXiv:1705.10707] [Phys. Rev. A 97, 011401(R) (2018)] on Diamond at 800 nm and by Tancogne-Dejean et al. [arXiv:1609.09298] [Phys. Rev. Lett. 118, 087403 (2017)] on Si at 3000 nm.

cond-mat.mtrl-sci↗

arXiv2021

Nonlinear dynamics of electromagnetic field and valley polarization in WSe$_{2}$ monolayer

Linear and nonlinear optical response of WSe$_{2}$ monolayer is investigated by two-dimensional Maxwell plus time-dependent density functional theory with spin-orbit interaction. By applying the chiral resonant pulses, the electron dynamics along with high harmonic generation are examined at weak and strong laser fields. WSe$_{2}$ monolayer shows the linear optical response at the intensity I = 10$^{10}$~W/cm$^{2}$ while a complex nonlinear behavior is observed at I = 10$^{12}$~W/cm$^{2}$. The nonlinear response of WSe$_{2}$ monolayer in terms of saturable absorption is observed at strong laser field. By changing the chirality of the resonant light, a strong circular dichroic effect is observed in the excited state population. A relatively weak laser field shows effective valley polarization while strong field induces spin-polarized carrier peak between $K$($K'$) and $\mathitΓ$-point via nonlinear process. On the other hand, the strong laser field shows high harmonics up to the 11th order. Our results demonstrate that circularly polarized resonant pulse generate high harmonics in WSe$_{2}$ monolayer of order 3n$\pm1$.

cond-mat.mtrl-sci↗

arXiv2021

Valley polarization control in WSe2 monolayer by a single-cycle laser pulse

Abstract The valley degree of freedom in two-dimensional materials provides an opportunity to extend the functionalities of valleytronics devices. Very short valley lifetimes demand the ultrafast control of valley pseudospin. Here, we theoretically demonstrate the control of valley pseudospin in WSe2 monolayer by single-cycle linearly polarized laser pulse. We use the asymmetric electric field controlled by the carrier-envelope phase (CEP) to make the valley polarization between K and K'-point in the Brillouin zone (BZ). Time-dependent density functional theory with spin-orbit interaction reveals that no valley asymmetry and its CEP dependence is observed within the linear-optical limit. In the nonlinear-optical regime, linearly polarized pulse induces a high degree of valley polarization and this polarization is robust against the field strength. Valley polarization strongly depends and oscillates as a function of CEP. The carrier density distribution forms nodes as the laser intensity increases, our results indicate that the position of the carrier density in the BZ can be controlled by the laser intensity. From the analysis by the massive Dirac Hamiltonian model, the nodes of the carrier density can be attributed to the Landau-Zener-Stückelberg interference of wave packets of the electron wave function.

physics.optics↗

arXiv2021

Determining the optimum thickness for high harmonic generation from nanoscale thin films: an ab initio computational study

We theoretically investigate high harmonic generation (HHG) from silicon thin films with thicknesses from a few atomic layers to a few hundreds of nanometers, to determine the most efficient thickness for producing intense HHG in the reflected and transmitted pulses. For this purpose, we employ a few theoretical and computational methods. The most sophisticated method is the ab initio time-dependent density functional theory coupled with the Maxwell equations in a common spatial resolution. This enables us to explore such effects as the surface electronic structure and light propagation, as well as electronic motion in the energy band in a unified manner. We also utilize a multiscale method that is applicable to thicker films. Two-dimensional approximation is introduced to obtain an intuitive understanding of the thickness dependence of HHG. From these ab initio calculations, we find that the HHG signals are the strongest in films with thicknesses of 2-15 nm, which is determined by the bulk conductivity of silicon. We also find that the HHG signals in the reflected and transmitted pulses are identical in such thin films. In films whose thicknesses are comparable to the wavelength in the medium, the intensity of HHG signals in the reflected (transmitted) pulse is found to correlate with the magnitude of the electric field at the front (back) surface of the thin film.

cond-mat.mtrl-sci↗

arXiv2020

Symmetry properties of attosecond transient absorption spectroscopy in crystalline dielectrics

We theoretically investigate a relation between the crystalline symmetry and the transient modulation of optical properties of crystalline dielectrics in pump-probe measurements using intense pump and attosecond probe fields. When the photon energy of the pump field is much below the bandgap energy, the modulation of the optical conductivity is caused by the intraband electronic motion, that is, the dynamical Franz-Keldysh effect. We analytically investigate symmetry properties of the modulated optical conductivity utilizing the Houston function, and derive a formula that relates the temporal oscillation in the absorption with the transformation properties of the modulated optical conductivity. To verify the validity of the formula, we perform real-time first-principles calculations based on the time-dependent density functional theory for a pump-probe process taking 4H-SiC crystal as an example.

cond-mat.mtrl-sci↗

arXiv2018

Time-dependent density functional theory for interaction of ultrashort light pulse with thin materials

We present a comprehensive theoretical description for an irradiation of an ultrashort light pulse normally on thin materials based on first-principles time-dependent density functional theory. As the most elaborate scheme, we develop a microscopic description solving Maxwell equations for light electromagnetic fields and the time-dependent Kohn-Sham equation for electron dynamics simultaneously in the time domain using a common spatial grid. We call it the microscopic Maxwell-TDDFT scheme. We test this scheme for silicon thin films of various thickness, from a few atomic layers to a few tens of nm. We show that the microscopic Maxwell-TDDFT scheme provides a satisfactory description incorporating the electronic structure of thin films in the first-principles level, multiple reflections of the electromagnetic fields at the surfaces, and nonlinear light-matter interaction when the incident light pulse is strong. However, the calculation becomes expensive as the thickness increases. We then consider two limiting cases of extremely thin and sufficiently thick films and develop approximate schemes. For the extremely thin case including two-dimensional atomic-layered materials, a two-dimensional macroscopic electromagnetism is developed: a two-dimensional susceptibility is introduced for a weak field, while time evolution equation is derived for an intense field. For sufficiently thick films, the microscopic Maxwell-TDDFT scheme is expected to coincide with a description utilizing ordinary macroscopic electromagnetism. We numerically confirm it comparing the calculated results: For a weak field, a comparison is made with a description using the bulk dielectric susceptibility. For a strong field, a comparison is made with a multiscale Maxwell-TDDFT scheme which the authors' group developed previously.

physics.optics↗

arXiv2018

SALMON: Scalable Ab-initio Light-Matter simulator for Optics and Nanoscience

SALMON (Scalable Ab-initio Light-Matter simulator for Optics and Nanoscience, http://salmon-tddft.jp) is a software package for the simulation of electron dynamics and optical properties of molecules, nanostructures, and crystalline solids based on first-principles time-dependent density functional theory. The core part of the software is the real-time, real-space calculation of the electron dynamics induced in molecules and solids by an external electric field solving the time-dependent Kohn-Sham equation. Using a weak instantaneous perturbing field, linear response properties such as polarizabilities and photoabsorptions in isolated systems and dielectric functions in periodic systems are determined. Using an optical laser pulse, the ultrafast electronic response that may be highly nonlinear in the field strength is investigated in time domain. The propagation of the laser pulse in bulk solids and thin films can also be included in the simulation via coupling the electron dynamics in many microscopic unit cells using Maxwell's equations describing the time evolution of the electromagnetic fields. The code is efficiently parallelized so that it may describe the electron dynamics in large systems including up to a few thousand atoms. The present paper provides an overview of the capabilities of the software package showing several sample calculations.

physics.comp-ph↗

arXiv2016

An efficient method for calculating spatially extended electronic states of large systems with a divide-and-conquer approach

We present an efficient post-processing method for calculating the electronic structure of nanosystems based on the divide-and-conquer approach to density functional theory (DC-DFT), in which a system is divided into subsystems whose electronic structure is solved separately. In this post process, the Kohn-Sham Hamiltonian of the total system is easily derived from the orbitals and orbital energies of subsystems obtained by DC-DFT without time-consuming and redundant computation. The resultant orbitals spatially extended over the total system are described as linear combinations of the orbitals of the subsystems. The size of the Hamiltonian matrix can be much reduced from that for conventional calculation, so that our method is fast and applicable to general huge systems for investigating the nature of electronic states.

cond-mat.mtrl-sci↗