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- ItemMultidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields(Cambridge [u.a.] : Soc., 2016) Bruner, Barry D.; Mašín, Zdeněk; Negro, Matteo; Morales, Felipe; Brambila, Danilo; Devetta, Michele; Faccialà, Davide; Harvey, Alex G.; Ivanov, Misha; Mairesse, Yann; Patchkovskii, Serguei; Serbinenko, Valeria; Soifer, Hadas; Stagira, Salvatore; Vozzi, Caterina; Dudovich, Nirit; Smirnova, OlgaHigh harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
- ItemKinematic origin for near-zero energy structures in mid-IR strong field ionization(Bristol : IOP Publ., 2016) Pisanty, Emilio; Ivanov, MishaWe propose and discuss a kinematic mechanism underlying the recently discovered 'near-zero energy structure' in the photoionization of atoms in strong mid-infrared laser fields, based on trajectories which revisit the ion at low velocities exactly analogous to the series responsible for low-energy structures. The different scaling of the new series, as $E\sim {I}_{p}^{2}/{U}_{p}$, suggests that the near-zero energy structure can be lifted to higher energies, where it can be better resolved and studied, using harder targets with higher ionization potential.
- ItemAttosecond recorder of the polarization state of light([London] : Nature Publishing Group UK, 2018) Jiménez-Galán, Álvaro; Dixit, Gopal; Patchkovskii, Serguei; Smirnova, Olga; Morales, Felipe; Ivanov, MishaHigh harmonic generation in multi-color laser fields opens the opportunity of generating isolated attosecond pulses with high ellipticity. Such pulses hold the potential for time-resolving chiral electronic, magnetization, and spin dynamics at their natural timescale. However, this potential cannot be realized without characterizing the exact polarization state of light on the attosecond timescale. Here we propose and numerically demonstrate a complete solution of this problem. Our solution exploits the extrinsic two-dimensional chirality induced in an atom interacting with the chiral attosecond pulse and a linearly polarized infrared probe. The resulting asymmetry in the photoelectron spectra allows to reconstruct the complete polarization state of the attosecond pulse, including its possible time dependence. The challenging problem of distinguishing circularly polarized, partially polarized, or unpolarized pulses in the extreme ultraviolet range is also resolved. We expect this approach to become the core ingredient for attosecond measurements of chiral-sensitive processes in gas and condensed phase.
- ItemHigh harmonic interferometry of the Lorentz force in strong mid-infrared laser fields([Bad Honnef] : Dt. Physikalische Ges., 2018-05-11) Pisanty, Emilio; Hickstein, Daniel D.; Galloway, Benjamin R.; Durfee, Charles G.; Kapteyn, Henry C.; Murnane, Margaret M.; Ivanov, MishaThe interaction of intense mid-infrared laser fields with atoms and molecules leads to a range of new opportunities, from the production of bright, coherent radiation in the soft x-ray range, to imaging molecular structures and dynamics with attosecond temporal and sub-angstrom spatial resolution. However, all these effects, which rely on laser-driven recollision of an electron removed by the strong laser field and its parent ion, suffer from the rapidly increasing role of the magnetic field component of the driving pulse: the associated Lorentz force pushes the electrons off course in their excursion and suppresses all recollision-based processes, including high harmonic generation as well as elastic and inelastic scattering. Here we show how the use of two non-collinear beams with opposite circular polarizations produces a forwards ellipticity which can be used to monitor, control, and cancel the effect of the Lorentz force. This arrangement can thus be used to re-enable recollision-based phenomena in regimes beyond the long-wavelength breakdown of the dipole approximation, and it can be used to observe this breakdown in high harmonic generation using currently available light sources.
- ItemAttosecond control of spin polarization in electron–ion recollision driven by intense tailored fields([Bad Honnef] : Dt. Physikalische Ges., 2017-07-07) Ayuso, David; Jiménez-Galán, Alvaro; Morales, Felipe; Ivanov, Misha; Smirnova, OlgaTunnel ionization of noble gas atoms driven by a strong circularly polarized laser field in combination with a counter-rotating second harmonic generates spin-polarized electrons correlated to the spin-polarized ionic core. Crucially, such two-color field can bring the spin-polarized electrons back to the parent ion, enabling the scattering of the spin-polarized electron on the spin-polarized parent ion. Here we show how one can control the degree of spin polarization as a function of electron energy and recollision time by tuning the laser parameters, such as the relative intensities of the counter-rotating fields. The attosecond precision of the control over the degree of spin polarization opens the door for attosecond control and spectroscopy of spin-resolved dynamics.
- ItemSymmetry breaking and strong persistent plasma currents via resonant destabilization of atoms(Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2017) Brée, Carsten; Hofmann, Michael; Babushkin, Ihar; Demircan, Ayhan; Morgner, Uwe; Kosareva, Olga G.; Savelev, Andrei B.; Husakou, Anton; Ivanov, MishaThe ionization rate of an atom in a strong optical field can be resonantly enhanced by the presence of long-living atomic levels (so called Freeman resonances). This process is most prominent in the multiphoton ionization regime meaning that ionization event takes many optical cycles. Nevertheless, here we show that these resonances can lead to fast subcycle-scale plasma buildup at the resonant values of the intensity in the pump pulse. The fast buildup can break the cycletocycle symmetry of the ionization process, resulting in generation of persistent macroscopic plasma currents which remain after the end of the pulse. This, in turn, gives rise to a broadband radiation of unusual spectral structure forming a comb from terahertz (THz) to visible. This radiation contains fingerprints of the attosecond electronic dynamics in Rydberg states during ionization.