arXiv subjects

Kazuhiro Yabana

Publications and source records attributed to Kazuhiro Yabana.

At least 37 records · Page 2Linked to original sources

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↗

arXiv2021

First-principles study of ultrafast and nonlinear optical properties of graphite thin films

We theoretically investigate ultrafast and nonlinear optical properties of graphite thin films based on first-principles time-dependent density functional theory. We first calculate electron dynamics in a unit cell of graphite under a strong pulsed electric field and explore the transient optical properties of graphite. It is shown that the optical response of graphite shows a sudden change from conducting to insulating phase at a certain intensity range of the applied electric field. It also appears as a saturable absorption, the saturation in the energy transfer from the electric field to electrons. We next investigate a light propagation in graphite thin films by solving coupled dynamics of the electrons and the electromagnetic fields simultaneously. It is observed that the saturable absorption manifests in the propagation with small attenuation in the spatial region where the electric field amplitude is about $4 \sim 7 \times 10^{-2}$ V/Angstrom.

physics.optics↗

arXiv2020

Attosecond state-resolved carrier motion in quantum materials probed by soft X-ray XANES

Recent developments in attosecond technology led to tabletop X-ray spectroscopy in the soft X-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the element- and state-specificity at the transition metal L-edge of the quantum material allows to unambiguously identify how and where the optical field influences charge carriers. This precision elucidates that the Ti:3d conduction band states are efficiently photo-doped to a density of 1.9 x 10^21 cm^-3 and that the light-field induces coherent motion of intra-band carriers across 38% of the first Brillouin zone. Lastly, we describe the prospects with such unambiguous real-time observation of carrier dynamics in specific bonding or anti-bonding states and speculate that such capability will bring unprecedented opportunities towards an engineered approach for designer materials with pre-defined properties and efficiency. Examples are composites of semiconductors and insulators like Si, Ge, SiO2, GaN, BN, quantum materials like graphene, TMDCs, or high-Tc superconductors like NbN or LaBaCuO. Exiting are prospects to scrutinize canonical questions in multi-body physics such as whether the electrons or lattice trigger phase transitions.

cond-mat.mtrl-sci↗

arXiv2020

Modulation of probe signal in coherent phonon detection revisited: Analytical and first-principles computational analyses

Modulation of probe signal in pump-probe measurements of coherent phonons in dielectrics, with and without spectral resolution, are investigated theoretically taking diamond as an example. Analytical investigation as well as first-principles calculations based on time-dependent density functional theory is utilized to clarify the mechanism of the modulation of the probe signals. Boundary and bulk effects are investigated systematically, putting emphasis on the phase relation between the modulation and the atomic motion of the coherent phonon. They are summarized as follows: Modulation by the boundary effect is in phase with the coherent phonon amplitude, while that by the bulk effect shows $π/2$ phase difference. Strong frequency dependence appears in the modulation by the bulk effect, while no frequency dependence by the boundary effect. First-principles calculations support the reliability of the analytical result.

physics.optics↗

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↗

arXiv2019

Operation of Quantum Plasmonic Metasurfaces Using Electron Transport through Subnanometer Gaps

Herein, we investigate the optical properties of quantum plasmonic metasurfaces composed of metallic nano-objects with subnanometer gaps according to the time-dependent density functional theory, a fully quantum mechanical approach. When the quantum and classical descriptions are compared, the transmission, reflection, and absorption rates of the metasurface exhibit substantial differences at shorter gap distances. The differences are caused by electron transport through the gaps of the nano-objects. The electron transport has profound influences for gap distances less-than or approximately 0.2 nm; that is, almost equal to half of the distance found in conventional gap plasmonics in isolated systems, such as metallic nanodimers. Furthermore, it is shown that the electron transport makes the plasmon features of the metasurface unclear and produces broad spectral structures in the optical responses. In particular, the reflection response exhibits rapid attenuation as the gap distance decreases, while the absorption response extends over a wide spectral range.

physics.optics↗

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

Nonlinear polarization evolution using time-dependent density functional theory

We propose a theoretical and computational approach to investigate temporal behavior of a nonlinear polarization in perturbative regime induced by an intense and ultrashort pulsed electric field. First-principles time-dependent density functional theory is employed to describe the electron dynamics. Temporal evolution of third-order nonlinear polarization is extracted from a few calculations of electron dynamics induced by pulsed electric fields with the same time profile but different amplitudes. We discuss characteristic features of the nonlinear polarization evolution as well as an extraction of nonlinear susceptibilities and time delays by fitting the polarization. We also carry out a decomposition of temporal and spatial changes of the electron density in power series with respect to the field amplitude. It helps to get insight into the origin of the nonlinear polarization in atomic scale.

physics.optics↗

arXiv2018

Time-dependent density functional theory for a unified description of ultrafast dynamics: pulsed light, electrons, and atoms in crystalline solids

We have developed a novel multiscale computational scheme to describe coupled dynamics of light electromagnetic field with electrons and atoms in crystalline solids, where first-principles molecular dynamics based on time-dependent density functional theory is used to describe the microscopic dynamics. The method is applicable to wide phenomena in nonlinear and ultrafast optics. To show usefulness of the method, we apply it to a pump-probe measurement of coherent phonon in diamond where a Raman amplification takes place during the propagation of the probe pulse.

physics.comp-ph↗

arXiv2018

Energy transfer from intense laser pulse to dielectrics in time-dependent density functional theory

Energy transfer processes from a high-intensity ultrashort laser pulse to electrons in simple dielectrics, silicon, diamond, and $α$-quartz are theoretically investigated by first-principles calculations based on time-dependent density functional theory (TDDFT). Dependences on frequency as well as intensity of the laser pulse are examined in detail, making a comparison with the Keldysh theory. Although the Keldysh theory reliably reproduces the main features of the TDDFT calculation, we find some deviations between results by the two theories. The origin of the differences is examined in detail.

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↗

arXiv2017

Ab-initio multi-scale simulation of high-harmonic generation in solids

High-harmonic generation by a highly non-linear interaction of infrared laser fields with matter allows for the generation of attosecond pulses in the XUV spectral regime. This process, well established for atoms, has been recently extended to the condensed phase. Remarkably well pronounced harmonics up to order ~30 have been observed for dielectrics. We present the first ab-initio multi-scale simulation of solid-state high-harmonic generation. We find that mesoscopic effects of the extended system, in particular the realistic sampling of the entire Brillouin zone, the pulse propagation in the dense medium, and the inhomogeneous illumination of the crystal have a strong effect on the formation of clean harmonic spectra. Our results provide a novel explanation for the formation of clean harmonics and have implications for a wide range of non-linear optical processes in dense media.

physics.optics↗

arXiv2016

Time-dependent density-functional description of nuclear dynamics

We present the basic concepts and recent developments in the time-dependent density functional theory (TDDFT) for describing nuclear dynamics at low energy. The symmetry breaking is inherent in nuclear energy density functionals (EDFs), which provides a practical description of important correlations at the ground state. Properties of elementary modes of excitation are strongly influenced by the symmetry breaking and can be studied with TDDFT. In particular, a number of recent developments in the linear response calculation have demonstrated their usefulness in description of collective modes of excitation in nuclei. Unrestricted real-time calculations have also become available in recent years, with new developments for quantitative description of nuclear collision phenomena. There are, however, limitations in the real-time approach; for instance, it cannot describe the many-body quantum tunneling. Thus, we treat the quantum fluctuations associated with slow collective motions assuming that time evolution of densities are determined by a few collective coordinates and momenta. The concept of collective submanifold is introduced in the phase space associated with the TDDFT and used to quantize the collective dynamics. Selected applications are presented to demonstrate the usefulness and quality of the new approaches. Finally, conceptual differences between nuclear and electronic TDDFT are discussed, with some recent applications to studies of electron dynamics in the linear response and under a strong laser field.

nucl-th↗

arXiv2016

Time-dependent Hartree-Fock calculations for multinucleon transfer and quasifission processes in the $^{64}$Ni+$^{238}$U reaction

Background: Multinucleon transfer (MNT) and quasifission (QF) processes are dominant processes in low-energy collisions of two heavy nuclei. They are expected to be useful to produce neutron-rich unstable nuclei. Nuclear dynamics leading to these processes depends sensitively on nuclear properties such as deformation and shell structure. Purpose: We elucidate reaction mechanisms of MNT and QF processes involving heavy deformed nuclei, making detailed comparisons between microscopic time-dependent Hartree-Fock (TDHF) calculations and measurements for the $^{64}$Ni+$^{238}$U reaction. Methods: Three-dimensional Skyrme-TDHF calculations are performed. Particle-number projection method is used to evaluate MNT cross sections from the TDHF wave function after collision. Results: Fragment masses, total kinetic energy (TKE), scattering angle, contact time, and MNT cross sections are investigated for the $^{64}$Ni+$^{238}$U reaction. They show reasonable agreements with measurements. At small impact parameters, collision dynamics depends sensitively on the orientation of deformed $^{238}$U. In tip (side) collisions, we find a larger (smaller) TKE and a shorter (longer) contact time. In tip collisions, we find a strong influence of quantum shells around $^{208}$Pb. Conclusions: It is confirmed that the TDHF calculations reasonably describe both MNT and QF processes in the $^{64}$Ni+$^{238}$U reaction. Analyses of this system indicates the significance of the nuclear structure effects such as deformation and quantum shells in nuclear reaction dynamics at low energies.

nucl-th↗

arXiv2015

Multinucleon transfer reaction in time-dependent Hartree-Fock theory

Time-dependent Hartree-Fock (TDHF) theory has achieved a remarkable success in describing and understanding nuclear many-body dynamics from nucleons' degrees of freedom. We here report our investigation of multinucleon transfer (MNT) processes employing the TDHF theory. To calculate transfer probabilities for channels specified by the number of protons and neutrons included in reaction products, a particle-number projection (PNP) method has been developed. The PNP method is also used to calculate excitation energies of reaction products. Combined use of the PNP method with a statistical model, we can evaluate MNT cross sections taking account of effects of particle evaporation. Using these methods, we evaluate MNT cross sections for $^{40,48}$Ca+$^{124}$Sn, $^{40}$Ca+$^{208}$Pb, and $^{58}$Ni+$^{208}$Pb reactions. From systematic analyses, we find that cross sections for channels with a large reaction probability are in good agreement with experimental data. However, the agreement becomes less accurate as the number of transferred nucleons increases. Possible directions to improve the description are discussed.

nucl-th↗

arXiv2015

Nonlinear electronic excitations in crystalline solids using meta-generalized gradient approximation and hybrid functional in time-dependent density functional theory

We develop numerical methods to calculate electron dynamics in crystalline solids in real-time time-dependent density functional theory employing exchange-correlation potentials which reproduce band gap energies of dielectrics; a meta generalized gradient approximation (meta-GGA) proposed by Tran and Blaha [Phys. Rev. Lett. 102, 226401 (2009)] (TBm-BJ) and a hybrid functional proposed by Heyd, Scuseria, and Ernzerhof [J. Chem. Phys. 118, 8207 (2003)] (HSE). In time evolution calculations employing the TB-mBJ potential, we have found it necessary to adopt a predictor-corrector step for stable time-evolution. Since energy functional is not known for the TB-mBJ potential, we propose a method to evaluate electronic excitation energy without referring to the energy functional. Calculations using the HSE hybrid functional is computationally expensive due to the nonlocal Fock-like term. We develop a computational method for the operation of the Fock-like term in Fourier space, for which we employ massively parallel computers equipped with graphic processing units. To demonstrate significances of utilizing potentials providing correct band gap energies, we compare electronic excitations induced by femtosecond laser pulses using the TB-mBJ, HSE, and a simple local density approximation (LDA). At low laser intensities, electronic excitations are found to be sensitive to the band gap energy: results using TB-mBJ and HSE are close to each other, while the excitation of the LDA calculation is more intensive than the others. At high laser intensities close to a damage threshold, we have found that electronic excitation energies are similar among the three cases.

cond-mat.mtrl-sci↗

arXiv2015

Observation of molecular dipole excitations by attosecond self-streaking

We propose a protocol to probe the ultrafast evolution and dephasing of coherent electronic excitation in molecules in the time domain by the intrinsic streaking field generated by the molecule itself. Coherent electronic motion in the endohedral fullerene \Necsixty~is initiated by a moderately intense femtosecond UV-VIS pulse leading to coherent oscillations of the molecular dipole moment that persist after the end of the laser pulse. The resulting time-dependent molecular near-field is probed through the momentum modulation of photoemission from the central neon atom by a time-delayed attosecond XUV pulse. Our ab-initio time-dependent density functional theory and classical trajectory simulations predict that this self-streaking signal accurately traces the molecular dipole oscillations in real time. We discuss the underlying processes and give an analytical model that captures the essence of our ab-initio simulations.

physics.optics↗

arXiv2015

Controlling ultrafast currents by the non-linear photogalvanic effect

We theoretically investigate the effect of broken inversion symmetry on the generation and control of ultrafast currents in a transparent dielectric (SiO2) by strong femto-second optical laser pulses. Ab-initio simulations based on time-dependent density functional theory predict ultrafast DC currents that can be viewed as a non-linear photogalvanic effect. Most surprisingly, the direction of the current undergoes a sudden reversal above a critical threshold value of laser intensity I_c ~ 3.8*10^13 W/cm2. We trace this switching to the transition from non-linear polarization currents to the tunneling excitation regime. We demonstrate control of the ultrafast currents by the time delay between two laser pulses. We find the ultrafast current control by the non-linear photogalvanic effect to be remarkably robust and insensitive to laser-pulse shape and carrier-envelope phase.

physics.optics↗