Abstract. We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrödinger equation, for the case of H + 2 in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining highorder harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.
We study the ionization of atomic hydrogen in the direction of polarization due to a linearly polarized XUV pulse in the presence a strong field IR. We describe the photoelectron spectra as an interference problem in the time domain. Electron trajectories steming from different optical laser cycles give rise to intercycle interference energy peaks known as sidebands. These sidebands are modulated by a grosser structure coming from the intracycle interference of the two electron trajectories born during the same optical cycle. We make use of a simple semiclassical model which offers the possibility to establish a connection between emission times and the photoelectron kinetic energy. We compare the semiclassical predictions with the continuum-distorted wave strong field approximation and the ab initio solution of the time dependent Schrödinger equation. We analyze such interference pattern as a function of the time delay between the IR and XUV pulse and also as a function of the laser intensity.
We present a theoretical study of ionization of the hydrogen atom due to an XUV pulse in the presence of an IR laser with both fields linearly polarized in the same direction. In particular, we study the energy distribution of photoelectrons emitted perpendicularly to the polarization direction. By means of a very simple semiclassical model which considers electron trajectories born at different ionization times, the electron energy spectrum can be interpreted as the interplay of intraand intercycle interferences. The intracycle interference pattern stems from the coherent superposition of four electron trajectories giving rise to (i) interference of electron trajectories born during the same half cycle (intrahalfcycle interference) and (ii) interference between electron trajectories born during the first half cycle with those born during the second half cycle (interhalfcycle interference). The intercycle interference is responsible for the formation of the sidebands. We also show that the destructive interhalfcycle interference for the absorption and emission of an even number of IR laser photons is responsible for the characteristic sidebands in the perpendicular direction separated by twice the IR photon energy. We analyze the dependence of the energy spectrum on the laser intensity and the time delay between the XUV pulse and the IR laser. Finally, we show that our semiclassical simulations are in very good agreement with quantum calculations within the strong field approximation and the numerical solution of the time-dependent Schrödinger equation.
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