Nonlinear polarization evolution using time-dependent density functional theory

Abstract

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.

arXiv comment11 pages, 9 figures

References in corpus (10)

• A real-space, rela-time method for the dielectric function
• Time-dependent density functional theory for strong electromagnetic fields in crystalline solids
• SALMON: Scalable Ab-initio Light-Matter simulator for Optics and Nanoscience
• A real-time approach to the optical properties of solids and nano-structures: the time-dependent Bethe-Salpeter equation
• A time-dependent density functional theory scheme for efficient calculations of dynamic (hyper)polarizabilities
• Nonlinear optics from an ab-initio approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors
• Velocity-gauge real-time TDDFT within a numerical atomic orbital basis set
• Nonlinear optical spectrum of diamond at femtosecond regime
• Nonlinear electronic excitations in crystalline solids using meta-generalized gradient approximation and hybrid functional in time-dependent density functional theory
• Dielectrics in a time-dependent electric field: a real-time approach based on density-polarization functional theory

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