Terahertz radiation from tunneling ionization of gaseous atoms and molecules in the two-color laser fields with various polarizations has been investigated. We experimentally demonstrate that the efficiency of terahertz emission in the circularly polarized laser fields with the same helicity is 5 times higher than that with linearly polarized two-color femtosecond pulses in high laser intensity. By solving time-dependent Schrödinger equation, this enhancement is well explained based on the analysis of electron tunneling ionization and subsequent dynamics.

Understanding the evolution of molecular electronic structures is the key to explore and control photochemical reactions and photobiological processes. Subjected to strong laser fields, electronic holes are formed upon ionization and evolve in the attosecond timescale. It is crucial to probe the electronic dynamics in real time with attosecond-temporal and atomic-spatial precision. Here, we present molecular attosecond interferometry that enables the in situ manipulation of holes in carbon dioxide molecules via the interferometry of the phase-locked electrons (propagating in opposite directions) of a laser-triggered rotational wave packet. The joint measurement on high-harmonic and terahertz spectroscopy (HATS) provides a unique tool for understanding electron dynamics from picoseconds to attoseconds. The optimum phases of two-color pulses for controlling the electron wave packet are precisely determined owing to the robust reference provided with the terahertz pulse generation. It is noteworthy that the contribution of HOMO-1 and HOMO-2 increases reflecting the deformation of the hole as the harmonic order increases. Our method can be applied to study hole dynamics of complex molecules and electron correlations during the strong-field process. The threefold control through molecular alignment, laser polarization, and the two-color pulse phase delay allows the precise manipulation of the transient hole paving the way for new advances in attochemistry.

We study the generation of terahertz radiation from atoms and molecules driven by an ultrashort fundamental laser and its second-harmonic field by solving the time-dependent Schrödinger equation (TDSE). The comparisons between one-, two-, and three-dimensional TDSE numerical simulations show that the initial ionized wave packet and its subsequent acceleration in the laser field and rescattering with long-range Coulomb potential play key roles. We also present the dependence of the optimum phase delay and yield of terahertz radiation on the laser intensity, wavelength, duration, and ratio of two-color laser components. Terahertz wave generation from model hydrogen molecules is further investigated by comparing with high harmonic emission. It is found that the terahertz yield follows the alignment dependence of the ionization rate, while the optimal two-color phase delays vary by a small amount when the alignment angle changes from 0 to 90 degrees, which reflects the alignment dependence of attosecond electron dynamics. Finally, we show that terahertz emission might be used to clarify the origin of interference in high harmonic generation from aligned molecules by coincidentally measuring the alignment-dependent THz yields.

We theoretically investigate the high-harmonic generation (HHG) from periodical structures driven by an intense laser pulse. Including the full bands, the single electron time-dependent Schrödinger equation is numerically solved in the velocity gauge using Bloch states to obtain the emission spectra. The contributions from different crystal sites are identified using the localized Wannier functions and time-frequency analysis. It is found that the cutoff energy of harmonics is depending on the migration distance of the electron and the instantaneous laser field strength when the electron transports into the related sites. We show that the coherence among different sites during electron propagation is crucial for HHG from solids which can be taken advantage to control the individual site contribution to the certain frequency range of the total harmonic spectra.

We propose a novel approach based on the subcycle injection of carriers to extend the high-energy cutoff in solid-state high harmonics. The mechanism is first examined by employing the standard single-cell semiconductor Bloch equation (SC SBE) method for one-dimensional (1D) Mathieu potential model for ZnO subjected to the intense linearly polarized midinfrared laser field and extreme-ultraviolet pulse. Then, we use coupled solution of Maxwell propagation equation and SC SBE to propagate the fundamental laser field through the sample, and find that the high-harmonics pulse train from the entrance section of the sample can inject carriers to the conduction bands with attosecond timing, subsequently leading to a dramatic extension of high-energy cutoff in harmonics from the backside. We predict that for a peak intensity at $2\times {10}^{11}\mathrm{W}/{\mathrm{cm}}^2$, as a result of the self-seeding, the high-energy cutoff shifts from 20th (7.75 eV) order to around 50th (19.38 eV) order harmonics.

Photocurrents generated in few-cycle circularly polarized laser fields are investigated by solving the time-dependent Schrödinger equation and by means of classical-trajectory Monte Carlo simulations. After confirming the offset angles of the total final currents and electron spectra to be the same, we illustrate the effects of the Coulomb potential and ground state depletion on the offset angles of the total final current, by analyzing how electrons’ trajectories and momenta change with laser intensities. Using various atom systems at different laser wavelengths, we find that the behaviors of currents’ offset angles as a function of laser intensities seem to be universal.