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We experimentally and theoretically show that the electron energy spectra strongly depend on the relative helicity in highly intense, circularly polarized two-color laser fields which is an unexpected finding. The employed counter-rotating two-color (CRTC) fields and the co-rotating two-color (CoRTC) fields are both a superposition of circularly polarized laser pulses at a central wavelength of 390 nm and 780 nm (intensitiy ratio $I_{390}/I_{780}approx 250$). For the CRTC field, the measured electron energy spectrum is dominated by peaks that are spaced by 3.18 eV (corresponds to the photon energy of light at a wavelength of 390 nm). For the CoRTC field, we observe additional energy peaks (sidebands). Using our semi-classical, trajectory-based models, we conclude that the sideband intensity is modulated by a sub-cycle interference, which sensitively depends on the relative helicity in circularly polarized two-color fields.
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We report on three-dimensional (3D) electron momentum distributions from single ionization of helium by a laser pulse consisting of two counterrotating circularly polarized fields (390 nm and 780 nm). A pronounced 3D low energy structure and sub-cycle interferences are observed experimentally and reproduced numerically using a trajectory based semi-classical simulation. The orientation of the low energy structure in the polarization plane is verified by numerical simulations solving the time dependent Schrodinger equation.
The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.
Strong-field ionization of polar molecules contains rich dynamical processes such as tunneling, excitation, and Stark shift. These processes occur on a sub-cycle time scale and are difficult to distinguish in ultrafast measurements. Here, with a developed strong-field model considering effects of both Coulomb and permanent dipole, we show that photoelectron momentum distributions (PMDs) in orthogonal two-color laser fields can be utilized to resolve these processes with attosecond-scale resolution. A feature quantity related to the asymmetry in PMDs is obtained, with which the complex electron dynamics of polar molecules in each half laser cycle is characterized and the subtle time difference when electrons escaping from different sides of the polar molecule is identified.
We investigate the interwoven dynamic evolutions of neutral nitrogen molecules together with nitrogen ions created through transient tunnel ionization in an intense laser field. By treating the molecules as open quantum systems, it is found that considering real-time injection of ions and strong couplings among their electronic states, nitrogen molecular ions are primarily populated in the electronically excited states, rather than staying in the ground state as predicted by the well-known tunneling theory. The unexpected result is attributed to sub-cycle switch-on of time-dependent polarization by transient ionization and dynamic Stark shift mediated near-resonant multiphoton transitions. Their combined contribution also causes that the vibrational distribution of N$_2^+$ does not comply with Franck-Condon principle. These findings corroborate the mechanism of nitrogen molecular ion lasing and are likely to be universal. The present work opens a new route to explore the important role of transient ionization injection in strong-field induced non-equilibrium dynamics.
Magnetic control of reactive scattering is realized in an ultracold mixture of $^{23}$Na atoms and $^{23}$Na$^{6}$Li molecules via Feshbach resonances. In most molecular systems, particles form lossy collision complexes at short range with unity probability for chemical reaction or inelastic scattering leading to the so-called universal loss rate. In contrast, Na${+}$NaLi is shown to have ${<}4%$ loss probability at short range when spin polarization suppresses loss. By controlling the phase of the wavefunction via a Feshbach resonance, we modify the loss rate by more than a factor of hundred, from far below the universal limit to far above, demonstrated here for the fist time. The results are explained in analogy with an optical Fabry-Perot interferometer by constructive and destructive interference of reflections at short and long range. Our work demonstrates quantum control of chemistry by magnetic fields with the full dynamic range predicted by our models.
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