Zhangjin Chen

Accurate retrieval of structural information from laser-induced photoelectron and high-order harmonic spectra by few-cycle laser pulses.

By analyzing accurate theoretical results from solving the time-dependent Schrödinger equation of atoms in few-cycle laser pulses, we established the general conclusion that laser-generated high-energy electron momentum spectra and high-order harmonic spectra can be used to extract accurate differential elastic scattering and photo-recombination cross sections of the target ion with free electrons, 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 implies that existing few-cycle infrared lasers can be implemented for ultrafast imaging of transient molecules with temporal resolution of a few femtoseconds.

Strong-field rescattering physics—self-imaging of a molecule by its own electrons

When an atom or molecule is exposed to a short intense laser pulse, electrons that were removed at an earlier time may be driven back by the oscillating electric field of the laser to recollide with the parent ion, to incur processes like high-order harmonic generation (HHG), high-energy above-threshold ionization (HATI) and nonsequential double ionization (NSDI). Over the years, a rescattering model (the three-step model) has been used to understand these strong field phenomena qualitatively, but not quantitatively. Recently we have established such a quantitative rescattering (QRS) theory. According to QRS, the yields for HHG, HATI and NSDI can be expressed as the product of a returning electron wave packet with various field-free electron–ion scattering cross sections, namely photo-recombination, elastic electron scattering and electron-impact ionization, respectively. The validity of QRS is first demonstrated by comparing with accurate numerical results from solving the time-dependent Schrodinger equation (TDSE) for atoms. It is then applied to atoms and molecules to explain recent experimental data. According to QRS, accurate field-free electron scattering and photoionization cross sections can be obtained from the HATI and HHG spectra, respectively. These cross sections are the conventional tools for studying the structure of a molecule; thus, QRS serves to provide the required theoretical foundation for the self-imaging of a molecule in strong fields by its own electrons. Since infrared lasers of duration of a few femtoseconds are readily available today, these results imply that they are suitable for probing the dynamics of molecules with temporal resolutions of a few femtoseconds.

Quantitative rescattering theory for laser-induced high-energy plateau photoelectron spectra

A comprehensive quantitative rescattering QRS theory for describing the production of high-energy photoelectrons generated by intense laser pulses is presented. According to the QRS, the momentum distributions of these electrons can be expressed as the product of a returning electron wave packet with the elastic differential cross sections DCS between free electrons with the target ion. We show that the returning electron wave packets are determined mostly by the lasers only and can be obtained from the strong field approximation. The validity of the QRS model is carefully examined by checking against accurate results from the solution of the time-dependent Schrodinger equation for atomic targets within the single active electron approximation. We further show that experimental photoelectron spectra for a wide range of laser intensity and wavelength can be explained by the QRS theory, and that the DCS between electrons and target ions can be extracted from experimental photoelectron spectra. By generalizing the QRS theory to molecular targets, we discuss how few-cycle infrared lasers offer a promising tool for dynamic chemical imaging with temporal resolution of a few femtoseconds. DOI: 10.1103/PhysRevA.79.033409

Single ionization of helium by 102 eV electron impact: three-dimensional images for electron emission

Single ionization of helium by 102 eV electron impact has been studied by measuring the momentum vectors of all final-state particles, i.e., two electrons and the He + ion, with an advanced reaction microscope. Fully differential cross sections for asymmetric scattering geometry, which have been normalized to an absolute scale, have been obtained covering a large range of emission angles for the emitted low-energy (E ≤ 15 eV) electron and different scattering angles for the fast electron. Strong electron emission out of the projectile scattering plane is confirmed for electron impact, as was observed before for heavy-ion impact ionization. The data are compared with theoretical predictions from a three-Coulomb wavefunction model, first-order and second-order distorted-wave approaches, as well as a convergent close-coupling calculation.

Self-imaging of molecules from diffraction spectra by laser-induced rescattering electrons

We study high-energy angle-resolved photoelectron spectra of molecules in strong fields. In an oscillating laser electric field, electrons released earlier in the pulse may return to recollide with the target ion, in a process similar to scattering by laboratory prepared electrons. If midinfrared lasers are used, we show that the images generated by the returning electrons are similar to images observed in typical gas-phase electron diffraction (GED). These spectra can be used to retrieve the positions of atoms in a molecule as in GED. Since infrared laser pulses of durations of a few femtoseconds are already available today, the study of these high-energy photoelectrons offers the opportunity of imaging the structure of transient molecules with temporal resolution of a few femtoseconds.

Potential for ultrafast dynamic chemical imaging with few-cycle infrared lasers

We studied the photoelectron spectra generated by an intense few-cycle infrared laser pulse. By focusing on the angular distributions of the back rescattered high energy photoelectrons, we show that accurate differential elastic scattering cross-sections of the target ion by free electrons can be extracted. Since the incident direction and the energy of the free electrons can be easily changed by manipulating the lasers polarization, intensity and wavelength, these extracted elastic scattering cross-sections, in combination with more advanced inversion algorithms, may be used to reconstruct the effective single-scattering potential of the molecule, thus opening up the possibility of using few-cycle infrared lasers as powerful table-top tools for imaging chemical and biological transformations, with the desired unprecedented temporal and spatial resolutions.

Second-order distorted wave calculation for electron-impact ionization of helium to He+(n = 1 and 2)

Second-order distorted wave calculations are presented for electron-impact ionization of helium with the residual ion left in the n = 1 and 2 states at intermediate energies in coplanar asymmetric geometry. Whereas previous second-order calculations have used the plane wave Born approximation and have used approximations to simplify the evaluation of the second-order term, we perform a full distorted wave calculation and make no approximations in the evaluation of the second-order amplitude (i.e. we sum over all contributing intermediate states). The triple differential cross sections are compared with experimental measurements.

Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography

Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. In addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. We showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules.

Retrieval of experimental differential electron?ion elastic scattering cross sections from high-energy ATI spectra of rare gas atoms by infrared lasers

Based on the concept of the recently developed quantitative rescattering theory for the momentum distributions of high-energy photoelectrons generated by infrared lasers, we applied the theory to extract large-angle elastic differential cross sections (DCS) of the target ions with free electrons. Using experimental photoelectron spectra for rare gas atoms of Ne, Ar, Kr and Xe, we showed that the extracted DCS are in good agreement with the DCS calculated theoretically. The current method of retrieval does not require precise knowledge of the peak laser intensities. The results show that accurate DCS between electron–ion scattering indeed can be retrieved from experimental photoelectron spectra generated by lasers, thus paving the way for using infrared laser pulses for dynamic chemical imaging of transient molecules with temporal resolution of few femtoseconds.

Second-Order Distorted Wave Calculation for Electron Impact Ionization of Hydrogen

The triple differential cross sections for ionization of atomic hydrogen by electron impact are analysed in the case of coplanar, asymmetric geometry within the framework of second-order distorted wave theory. Detailed calculations are performed without making any approximations (other than numerical) in the evaluation of the second-order amplitude. The present results are compared with experimental measurements and other theoretical calculations for incident energies of 250, 150 and 54.4 eV. It is found that the second-order calculations represent a marked improvement over the results obtained from first-order theories for impact energies of 150 eV and higher. The close agreement between the present second-order plane wave calculation and those of Byron et al calculated using the closure approximation at an incident energy of 250 eV implies that the closure approximation is valid for this energy. The large difference between the present second-order distorted wave calculations and experiment at an incident energy of 54.4 eV suggests that higher order effects are important for incident energies less than 100 eV.