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Register a new userTheoretical study of terahertz generation from atoms and aligned molecules driven by two-color laser fields
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We study the generation of terahertz radiation from atoms and molecules driven by an ultrashort fundamental laser and its second harmonic field by solving time-dependent Schrodinger equation (TDSE). The comparisons between one-, two-, and three- dimensional TDSE numerical simulations show that 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 the ratio of two-color laser components. Terahertz wave generation from model hydrogen molecules are further investigated by comparing with high harmonic emission. It is found that the terahertz yield is following the alignment dependence of ionization rate, while the optimal two-color phase delays varies by a small amount when the alignment angle changes from 0 to 90 degrees, which reflects 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 coincidently measuring the angle-resolved THz yields.
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We study the influence of the polarization states of femtosecond two-color pulses ionizing gases on the emitted terahertz radiation. A local-current model and plane-wave evaluations justify the previously-reported impact on the THz energy yield and an (almost) linearly-polarized THz field when using circularly-polarized laser harmonics. For such pump pulses, the THz yield is independent on the relative phase between the two colors. When the pump pulses have same helicity, the increase in the THz yield is associated to longer ionization sequences and higher electron transverse momenta acquired in the driving field. Reversely, for two color pulses with opposite helicity, the dramatic loss of THz power comes from destructive interferences driven by the highly symmetric response of the photocurrents lined up on the third harmonic of the fundamental pulse. While our experiments confirm an increased THz yield for circularly polarized pumps of same helicity, surprisingly, the emitted THz radiation is not linearly-polarized. This effect is explained by means of comprehensive 3D numerical simulations highlighting the role of the spatial alignment and non-collinear propagation of the two colors.
We consider harmonics generation and wave-mixing by two-color multi photon resonant excitation of three-level atoms/molecules in strong laser fields. The coherent part of the spectra corresponding to multicolor harmonics generation is investigated. The obtained analytical results on the basis of generalized rotating wave approximation are in a good agreement with numerical calculations. The results applied to the hydrogen atom and homonuclear diatomic molecular ion show that one can achieve efficient generation of moderately high multicolor harmonics via multiphoton resonant excitation by appropriate laser pulses.
We report the first experimental observation of non-adiabatic field-free orientation of a heteronuclear diatomic molecule (CO) induced by an intense two-color (800 and 400 nm) femtosecond laser field. We monitor orientation by measuring fragment ion angular distributions after Coulomb explosion with an 800 nm pulse. The orientation of the molecules is controlled by the relative phase of the two-color field. The results are compared to quantum mechanical rigid rotor calculations. The demonstrated method can be applied to study molecular frame dynamics under field-free conditions in conjunction with a variety of spectroscopy methods, such as high-harmonic generation, electron diffraction and molecular frame photoemission.
We investigate the generation of broadband terahertz (THz) pulses with phase singularity from air plasmas created by fundamental and second harmonic laser pulses. We show that when the second harmonic beam carries a vortex charge, the THz beam acquires a vortex structure as well. A generic feature of such THz vortex is that the intensity is modulated along the azimuthal angle, which can be attributed to the spatially varying relative phase difference between the two pump harmonics. Fully space and time resolved numerical simulations reveal that transverse instabilities of the pump further affect the emitted THz field along nonlinear propagation, which produces additional singularities resulting in a rich vortex structure. The predicted intensity modulation is experimentally demonstrated with a thermal camera, in excellent agreement with simulation results. The presence of phase singularities in the experiment is revealed by astigmatic transformation of the beam using a cylindrical mirror.
We present the experimental and theoretical details of our recent published letter [Phys. Rev. Lett. 115. 123002] on synchronized high-harmonic and terahertz-wave spectroscopy (HATS) from nonadiabatically aligned nitrogen molecules in dual-color laser fields. Associating the alignment-angle dependent terahertz wave generation with the synchronizing high-harmonic signal, the angular differential photoionization cross section (PICS) for molecules can be reconstructed, and the minima of the angle on PICS show great convergence between the theoretical predictions and the experimental deduced results. We also show the optimal relative phase between the dual-color laser fields for terahertz wave generation dose not change with the alignment angle at a precision of $50$ attoseconds. This all-optical method provides an alternative for investigating molecular structures and dynamics.
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