Guardians Ad Litem as Surrogate Parents: Implication for Role Definition and Confidentiality

SALMON (Scalable Ab-initio Light–Mattersimulator 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. Program summary Program Title: SALMON: Scalable Ab-initio Light–Matter simulator for Optics and Nanoscience Program Files doi:http://dx.doi.org/10.17632/8pm5znxtsb.1 Licensing provisions: Apache-2.0 Programming language: Fortran 2003 Nature of problem: Electron dynamics in molecules, nanostructures, and crystalline solids induced by an external electric field is calculated based on first-principles time-dependent density functional theory. Using a weak impulsive field, linear optical properties such as polarizabilities, photoabsorptions, and dielectric functions are extracted. Using an optical laser pulse, the ultrafast electronic response that may be highly nonlinear with respect to the exciting field strength is described as well. The propagation of the laser pulse in bulk solids and thin films is considered by coupling the electron dynamics in many microscopic unit cells using Maxwell’s equations describing the time evolution of the electromagnetic field. Solution method: Electron dynamics is calculated by solving the time-dependent Kohn–Sham equation in real time and real space. For this, the electronic orbitals are discretized on a uniform Cartesian grid in three dimensions. Norm-conserving pseudopotentials are used to account for the interactions between the valence electrons and the ionic cores. Grid spacings in real space and time, typically 0.02 nm and 1 as respectively, determine the spatial and temporal resolutions of the simulation results. In most calculations, the ground state is first calculated by solving the static Kohn–Sham equation, in order to prepare the initial conditions. The orbitals are evolved in time with an explicit integration algorithm such as a truncated Taylor expansion of the evolution operator, together with a predictor–corrector step when necessary. For the propagation of the laser pulse in a bulk solid, Maxwell’s equations are solved using a finite-difference scheme. By this, the electric field of the laser pulse and the electron dynamics in many microscopic unit cells of the crystalline solid are coupled in a multiscale framework

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 $\alpha$-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

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.Comment: 11 pages, 9 figure

Electronic Structure and Magnetic Properties of Solids

We review basic computational techniques for simulations of various magnetic properties of solids. Several applications to compute magnetic anisotropy energy, spin wave spectra, magnetic susceptibilities and temperature dependent magnetisations for a number of real systems are presented for illustrative purposes.Comment: Review article; To appear in Journal of Computational Crystallograph

Time-dependent density functional theory for strong electromagnetic fields in crystalline solids

We apply the coupled dynamics of time-dependent density functional theory and Maxwell equations to the interaction of intense laser pulses with crystalline silicon. As a function of electromagnetic field intensity, we see several regions in the response. At the lowest intensities, the pulse is reflected and transmitted in accord with the dielectric response, and the characteristics of the energy deposition is consistent with two-photon absorption. The absorption process begins to deviate from that at laser intensities ~ 10^13 W/cm^2, where the energy deposited is of the order of 1 eV per atom. Changes in the reflectivity are seen as a function of intensity. When it passes a threshold of about 3 \times 1012 W/cm2, there is a small decrease. At higher intensities, above 2 \times 10^13 W/cm^2, the reflectivity increases strongly. This behavior can be understood qualitatively in a model treating the excited electron-hole pairs as a plasma.Comment: 27 pages; 11 figure

Nonadiabatic generation of coherent phonons

The time-dependent density functional theory (TDDFT) is the leading computationally feasible theory to treat excitations by strong electromagnetic fields. Here the theory is applied to coherent optical phonon generation produced by intense laser pulses. We examine the process in the crystalline semimetal antimony (Sb), where nonadiabatic coupling is very important. This material is of particular interest because it exhibits strong phonon coupling and optical phonons of different symmetries can be observed. The TDDFT is able to account for a number of qualitative features of the observed coherent phonons, despite its unsatisfactory performance on reproducing the observed dielectric functions of Sb. A simple dielectric model for nonadiabatic coherent phonon generation is also examined and compared with the TDDFT calculations.Comment: 19 pages, 11 figures. This is prepared for a special issue of Journal of Chemical Physics on the topic of nonadiabatic processe

HARES: an efficient method for first-principles electronic structure calculations of complex systems

We discuss our new implementation of the Real-space Electronic Structure method for studying the atomic and electronic structure of infinite periodic as well as finite systems, based on density functional theory. This improved version which we call HARES (for High-performance-fortran Adaptive grid Real-space Electronic Structure) aims at making the method widely applicable and efficient, using high performance Fortran on parallel architectures. The scaling of various parts of a HARES calculation is analyzed and compared to that of plane-wave based methods. The new developments that lead to enhanced performance, and their parallel implementation, are presented in detail. We illustrate the application of HARES to the study of elemental crystalline solids, molecules and complex crystalline materials, such as blue bronze and zeolites.Comment: 17 two-column pages, including 9 figures, 5 tables. To appear in Computer Physics Communications. Several minor revisions based on feedbac

Ultrafast electron dynamics in metals

During the last decade, significant progress has been achieved in the rapidly growing field of the dynamics of {\it hot} carriers in metals. Here we present an overview of the recent achievements in the theoretical understanding of electron dynamics in metals, and focus on the theoretical description of the inelastic lifetime of excited hot electrons. We outline theoretical formulations of the hot-electron lifetime that is originated in the inelastic scattering of the excited {\it quasiparticle} with occupied states below the Fermi level of the solid. {\it First-principles} many-body calculations are reviewed. Related work and future directions are also addressed.Comment: 17 pages, two columns, 13 figures, to appear in ChemPhysChe