We develop theoretically and confirm both numerically and experimentally a comprehensive analytical model which describes the propensity rules in the emission of circularly polarized high harmonics by systems driven by two-color counter-rotating fields, a fundamental and its second harmonic. We identify and confirm the three propensity rules responsible for the contrast between the 3N+1 and 3N+2 harmonic lines in the HHG spectra of noble gas atoms. We demonstrate how these rules depend on the laser parameters and how they can be used in the experiment to shape the polarization properties of the emitted attosecond pulses.
We study the higher-harmonic generation (HHG) using elliptically polarized two-color driving fields. The HHG via bi-chromatic counter-rotating laser fields is a promising source of circularly polarized ultrashort XUV radiation at the attosecond time scale. The ellipticity or the polarization of the attosecond pulses can be tweaked by modifying the emitted harmonics ellipticity, which can be controlled by varying the driver fields. We propose a simple setup to control the polarization of the driving fields, which eventually changes the ellipticity of the attosecond pulses. A well-defined scaling law for the ellipticity of the attosecond pulse as a function of the rotation angle of the quarter-wave plate is also deduced by solving the time-dependent Schrodinger equation (TDSE) in two dimensions. The scaling law can further be explored to obtain the attosecond pulses of the desired degree of polarization, ranging from linear to elliptical to circular polarization.
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 demonstrate significant enhancement of frustrated double ionization (FDI) in the two-electron triatomic molecule D$_{3}^{+}$ when driven by counter-rotating two-color circular (CRTC) laser fields. We employ a three-dimensional semiclassical model that fully accounts for electron and nuclear motion in strong fields. For different pairs of wavelengths, we compute the probabilities of the FDI pathways as a function of the ratio of the two field-strengths. We identify a pathway of frustrated double ionization that is not present in strongly-driven molecules with linear fields. In this pathway the first ionization step is frustrated and electronic correlation is essentially absent. This pathway is responsible for enhancing frustrated double ionization with CRTC fields. We also employ a simple model that predicts many of the main features of the probabilities of the FDI pathways as a function of the ratio of the two field-strengths.
Ultrafast processes in matter can be captured and even controlled by using sequences of few-cycle optical pulses, which need to be well characterized, both in amplitude and phase. The same degree of control has not yet been achieved for few-cycle extreme ultraviolet pulses generated by high-order harmonic generation in gases, with duration in the attosecond range. Here, we show that by varying the spectral phase and carrier-envelope phase (CEP) of a high-repetition rate laser, using dispersion in glass, we achieve a high degree of control of the relative phase and CEP between consecutive attosecond pulses. The experimental results are supported by a detailed theoretical analysis based upon the semiclassical three-step model for high-order harmonic generation.
The ionization of two-active-electron systems by intense laser fields is investigated theoretically. In comparison with time-dependent Hartree-Fock and exact two electron simulation, we show that the ionization rate is overestimated in SAE approximation. A modified single-active-electron model is formulated by taking into account of the dynamical core polarization. Applying the new approach to Ca atoms, it is found that the polarization of the core can be considered instantaneous and the large polarizability of the cation suppresses the ionization by 50% while the photoelectron cut-off energy increases slightly. The existed tunneling ionization formulation can be corrected analytically by considering core polarization.