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While recent experiments provided compelling evidence for an intricate dependence of attosecond photoemission-time delays on the solid’s electronic band structure, the extent to which electronic transport and dispersion in solids can be imaged in time-resolved photoelectron (PE) spectra remains poorly understood. Emphasizing the distinction between photoemission time delays measured with two-photon, two-color interferometric spectroscopy, and transport times, we demonstrate how the effect of energy dispersion in the solid on photoemission delays can, in principle, be observed in interferometric photoemission. We reveal analytically a scaling relation between the PE transport time in the solid and the observable photoemission delay and confirm this relation in numerical simulations for a model system. We trace photoemission delays to the phase difference the PE accumulates inside the solid and, in particular, predict negative photoemission delays. Based on these findings, we suggest a novel time-domain interferometric solid-state energy-momentum-dispersion imaging method. 

We theoretically examine the rotational and vibrational dynamics of O2+ molecular ions exposed to intense, short laser pulses for conditions realized in contemporary pump-probe experiments.We solve the time-dependent Schrödinger equation within the Born-Oppenheimer approximation for an initial distribution of randomly aligned molecular ions. For fixed peak intensities, our numerical results show that total, angle-integrated O2+ → O(3P) + O+(4S0 ) dissociation yields do not monotonically increase with increasing infrared-probe pulse duration. We find this pulse-duration-dependent stabilization to be consistent with the transient trapping of nuclear probability density in a light-induced (bond-hardening) potential-energy surface and robust against rotational excitation. We analyze this stabilization effect and its underlying bond-hardening mechanism (i) in the time domain, by following the evolution of partial nuclear probability densities associated with the dipole-coupled O2+(a 4Pi u ) and O2+( f 4 Pi g) cationic states, and (ii) in the frequency domain, by examining rovibrational quantum-beat spectra for the evolution of the partial nuclear probability densities associated with these states. Our analysis reveals the characteristic timescale for the bond-hardening mechanism in O2+ and explains the onset of bond stabilization for sufficiently long pulse durations. 

To solve the time-dependent Schrödinger equation in spatially inhomogeneous pulses of electromagnetic radiation, we propose an iterative semiclassical complex trajectory approach. In numerical applications, we validate this method agains ab initio numerical solutions by scrutinizing (a) electronic sates in combined Coulomb and spatially homogeneous laser felds and (b) sreaked photoemission from hydrogen atoms and plasmonic gold nanospheres. In comparison with sreaked photoemission calculations performed in srong-feld approximation, we demonsrate the improved reconsruction of the spatially inhomogeneous induced plasmonic infrared feld near a nanoparticle surface from sreaked photoemission spectra. 

Photoemission from solid targets includes the excitation and motion of electrons inside the substrate, followed by their propagation in vacuum and detection. It thus depends on the electronic band structure of the solid in the two distinct spectral domains of bound initial and continuum final states. While the imprint of the static (initial-state) valence electronic structure of solids on photoemission spectra is routinely examined in standard photoemission spectroscopy in the energy domain, state-of-the-art time-resolved photoelectron spectroscopy allows, in addition, the scrutiny of photoelectron propagation in the electronic continuum. Within a quantum-mechanical model for attosecond time-resolved interferometric photoelectron emission from solids, we calculated photoemission spectra as a function of the delay between the exciting primary attosecond pulse train and assisting infrared (IR) laser pulse. Accounting for final-state interactions of the photoelectron with the IR laser electric field and the periodic substrate, our numerical results for interferometric photoemission from the 3d-valence band of Cu(111) surfaces show a striking resonantly enhanced sideband yield at photoelectron kinetic energies near 24 eV, in conjunction with a pronounced increase of the photoelectron wave-function amplitude inside the solid on a length scale of a few nanometers. This resonant shift of final-state photoelectron-probability density towards the bulk can be interpreted as an increase in the photoelectron propagation time in the solid and is commensurate with the resonantly enhanced spectral sideband-phase shifts observed in recent two-pathway two-photon interference spectra by Kasmi et al. [Optica 4, 1492 (2017)]. 

We analytically and numerically investigate the emission of high-order harmonic radiation from model solids by intense few-cycle midinfrared laser pulses. In single-active-electron approximation, we expand the active electron’s wave function in a basis of adiabatic Houston states and describe the solid’s electronic band structure in terms of an adjustable Kronig-Penney model potential. For high-order harmonic generation (HHG) from MgO crystals, we examine spectra from two-band and converged multiband numerical calculations. We discuss the characteristics of intra- and interband contributions to the HHG spectrum for computations including initial crystal momenta either from the  point at the center of the first Brillouin zone (BZ) only or from the entire first BZ. For sufficiently high intensities of the driving laser field, we find relevant contributions to HHG from the entire first BZ. Based on numerically calculated spectra, we scrutinize the cutoff harmonic orders as a function of the laser peak intensity and find good qualitative agreement with our analytical saddle-point-approximation predictions and published theoretical data.