Attosecond nonlinear polarization and light-matter energy transfer in solids.

Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques have provided experimental access to this important observable up to frequencies of several terahertz. Here we demonstrate that attosecond metrology extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750 nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light-matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible-infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.

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.

Magnetic circular dichroism in real-time time-dependent density functional theory.

We apply the adiabatic time-dependent density functional theory to magnetic circular dichroism (MCD) spectra using the real-space, real-time computational method. The standard formulas for the MCD response and its A and B terms are derived from the observables in the time-dependent wave function. We find real-time method is well suited for calculating the overall spectrum, particularly at higher excitation energies where individual excited states are numerous and overlapping. The MCD sum rules are derived and intepreted in the real-time formalism; we find that they are very useful for normalization purposes and assessing the accuracy of the theory. The method is applied to MCD spectrum of C(60) using the adiabatic energy functional from the local density approximation. The theory correctly predicts the signs of the A and B terms for the lowest allowed excitations. However, the magnitudes of the terms only show qualitative agreement with experiment.

Time-dependent density-functional theory simulation for electron-ion dynamics in molecules under intense laser pulses.

We have developed a simulation method to describe three-dimensional dynamics of electrons and ions in a molecule based on the time-dependent density-functional theory. We solve the time-dependent Kohn-Sham equation for electrons employing the real-space and real-time method, while the ion dynamics are described in classical mechanics by the Ehrenfest method. For an efficient calculation in massively parallel computers, the code is parallelized dividing the spatial grid points. We apply the method to the Coulomb explosion of the H(2)S molecule under an intense and ultrashort laser pulse and investigate the mechanism of the process.

First-principles calculation of the electron dynamics in crystalline SiO(2).

We present a first-principles description for electron dynamics in crystalline SiO(2) induced by an optical field in both weak and intense regimes. We rely upon the time-dependent density-functional theory with the adiabatic local-density approximation, and a real-space and real-time method is employed to solve the time-dependent Kohn-Sham equation. The response calculation to a weak field provides us with information on the dielectric function, while the response to an intense field shows the optical dielectric breakdown. We discuss the critical threshold for the dielectric breakdown of crystalline SiO(2), in comparison with the results for diamond.

Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond.

Short, intense laser pulses can be used to access the transition regime between classical and quantum optical responses in dielectrics. In this regime, the relative roles of inter- and intraband light-driven electronic transitions remain uncertain. We applied attosecond transient absorption spectroscopy to investigate the interaction between polycrystalline diamond and a few-femtosecond infrared pulse with intensity below the critical intensity of optical breakdown. Ab initio time-dependent density functional theory calculations, in tandem with a two-band parabolic model, accounted for the experimental results in the framework of the dynamical Franz-Keldysh effect and identified infrared induction of intraband currents as the main physical mechanism responsible for the observations.

Ultrafast dynamics. Attosecond band-gap dynamics in silicon.

Electron transfer from valence to conduction band states in semiconductors is the basis of modern electronics. Here, attosecond extreme ultraviolet (XUV) spectroscopy is used to resolve this process in silicon in real time. Electrons injected into the conduction band by few-cycle laser pulses alter the silicon XUV absorption spectrum in sharp steps synchronized with the laser electric field oscillations. The observed ~450-attosecond step rise time provides an upper limit for the carrier-induced band-gap reduction and the electron-electron scattering time in the conduction band. This electronic response is separated from the subsequent band-gap modifications due to lattice motion, which occurs on a time scale of 60 ± 10 femtoseconds, characteristic of the fastest optical phonon. Quantum dynamical simulations interpret the carrier injection step as light-field-induced electron tunneling.

First-principles description for coherent phonon generation in diamond.

We report a first-principles description for coherent phonon generation in diamond based on the time-dependent density functional theory. The time-dependent Kohn-Sham equation is solved in real time in order to calculate the electron dynamics in periodic solid exposed to an ultrashort laser pulse. We find that the calculated forces acting on ions are consistent with measurements as regards the selection rule and the dependence on the laser intensity.