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Generation of broad XUV continuous high harmonic spectra and isolated attosecond pulses with intense mid-infrared lasers

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 Added by Carlos Trallero
 Publication date 2011
  fields Physics
and research's language is English




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We present experimental results showing the appearance of a near-continuum in the high-order harmonic generation (HHG) spectra of atomic and molecular species as the driving laser intensity of an infrared pulse increases. Detailed macroscopic simulations reveal that these near-continuum spectra are capable of producing IAPs in the far field if a proper spatial filter is applied. Further, our simulations show that the near-continuum spectra and the IAPs are a product of strong temporal and spatial reshaping (blue shift and defocusing) of the driving field. This offers a possibility of producing IAPs with a broad range of photon energy, including plateau harmonics, by mid-IR laser pulses even without carrier-envelope phase stabilization.



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We report theoretical calculations of high-order harmonic generation (HHG) of Xe with the inclusion of multi-electron effects and macroscopic propagation of the fundamental and harmonic fields in an ionizing medium. By using the time-frequency analysis we show that the reshaping of the fundamental laser field is responsible for the continuum structure in the HHG spectra. We further suggest a method for obtaining an isolated attosecond pulse (IAP) by using a filter centered on axis to select the harmonics in the far field with different divergence. We also discuss the carrier-envelope-phase dependence of an IAP and the possibility to optimize the yield of the IAP. With the intense few-cycle mid-infrared lasers, this offers a possible method for generating isolated attosecond pulses.
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 Schrodinger equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order 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.
High harmonic generation driven by femtosecond lasers makes it possible to capture the fastest dynamics in molecules and materials. However, to date the shortest attosecond (as) pulses have been produced only in the extreme ultraviolet (EUV) region of the spectrum below 100 eV, which limits the range of materials and molecular systems that can be explored. Here we use advanced experiment and theory to demonstrate a remarkable convergence of physics: when mid-infrared lasers are used to drive the high harmonic generation process, the conditions for optimal bright soft X-ray generation naturally coincide with the generation of isolated attosecond pulses. The temporal window over which phase matching occurs shrinks rapidly with increasing driving laser wavelength, to the extent that bright isolated attosecond pulses are the norm for 2 mu m driving lasers. Harnessing this realization, we demonstrate the generation of isolated soft X-ray attosecond pulses at photon energies up to 180 eV for the first time, that emerge as linearly chirped 300 as pulses with a transform limit of 35 as. Most surprisingly, we find that in contrast to as pulse generation in the EUV, long-duration, multi-cycle, driving laser pulses are required to generate isolated soft X-ray bursts efficiently, to mitigate group velocity walk-off between the laser and the X-ray fields that otherwise limit the conversion efficiency. Our work demonstrates a clear and straightforward approach for robustly generating bright attosecond pulses of electromagnetic radiation throughout the soft X ray region of the spectrum.
Relativistic surface high harmonics have been considered a unique source for the generation of intense isolated attosecond pulses in the extreme ultra-violet (XUV) and X-ray spectral range. However, its experimental realization is still a challenging task requiring identification of the optimum conditions for the generation of isolated attosecond pulses as well as their temporal characterization. Here, we demonstrate measurements in both directions. Particularly, we have made a first step towards the temporal characterization of the emitted XUV radiation by adapting the attosecond streak camera concept to identify the time domain characteristics of relativistic surface high harmonics. The results, supported by PIC simulations, set the upper limit for the averaged (over many shots) XUV duration to <6 fs, even when driven by not CEP controlled relativistic few-cycle optical pulses. Moreover, by measuring the dependence of the spectrum of the relativistic surface high harmonics on the carrier envelope phase (CEP) of the driving infrared laser field, we experimentally determined the optimum conditions for the generation of intense isolated attosecond pulses.
Resonant enhancement of high harmonic generation can be obtained in plasmas containing ions with strong radiative transitions resonant with harmonic orders. The mechanism for this enhancement is still debated. We perform the first temporal characterization of the attosecond emission from a tin plasma under near-resonant conditions for two different resonance detunings. We show that the resonance considerably changes the relative phase of neighbouring harmonics. For very small detunings, their phase locking may even be lost, evidencing strong phase distortions in the emission process and a modified attosecond structure. These features are well reproduced by our simulations, allowing their interpretation in terms of the phase of the recombination dipole moment.
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