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Register a new userAccurate retrieval of structural information from laser-induced photoelectron and high-harmonic spectra by few-cycle laser pulses
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By analyzing ``exact theoretical results from solving the time-dependent Schrodinger equation of atoms in few-cycle laser pulses, we established the general conclusion that differential elastic scattering and photo-recombination cross sections of the target ion with {em free} electrons can be extracted accurately from laser-generated high-energy electron momentum spectra and high-order harmonic spectra, respectively. Since both electron scattering and photoionization (the inverse of photo-recombination) are the conventional means for interrogating the structure of atoms and molecules, this result shows that existing few-cycle infrared lasers can be implemented for ultrafast imaging of transient molecules with temporal resolution of a few femtoseconds.
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We illustrate an iterative method for retrieving the internuclear separations of N$_2$, O$_2$ and CO$_2$ molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is preferable to retrieve the interatomic separation iteratively by fitting the extracted dipole moment. Our results show that time-resolved chemical imaging of molecules using infrared laser pulses with femtosecond temporal resolutions is possible.
In this work we study the impact of chromatic focusing of few-cycle laser pulses on high-order harmonic generation (HHG) through analysis of the emitted extreme ultraviolet (XUV) radiation. Chromatic focusing is usually avoided in the few-cycle regime, as the pulse spatio-temporal structure may be highly distorted by the spatiotemporal aberrations. Here, however, we demonstrate it as an additional control parameter to modify the generated XUV radiation. We present experiments where few-cycle pulses are focused by a singlet lens in a Kr gas jet. The chromatic distribution of focal lengths allows us to tune HHG spectra by changing the relative singlet-target distance. Interestingly, we also show that the degree of chromatic aberration needed to this control does not degrade substantially the harmonic conversion efficiency, still allowing for the generation of supercontinua with the chirped-pulse scheme, demonstrated previously for achromatic focussing. We back up our experiments with theoretical simulations reproducing the experimental HHG results depending on diverse parameters (input pulse spectral phase, pulse duration, focus position) and proving that, under the considered parameters, the attosecond pulse train remains very similar to the achromatic case, even showing cases of isolated attosecond pulse generation for near single-cycle driving pulses.
Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.
This work describes the first observations of the ionisation of neon in a metastable atomic state utilising a strong-field, few-cycle light pulse. We compare the observations to theoretical predictions based on the Ammosov-Delone-Krainov (ADK) theory and a solution to the time-dependent Schrodinger equation (TDSE). The TDSE provides better agreement with the experimental data than the ADK theory. We optically pump the target atomic species and demonstrate that the ionisation rate depends on the spin state of the target atoms and provide physically transparent interpretation of such a spin dependence in the frameworks of the spin-polarised Hartree-Fock and random-phase approximations.
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.
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