Search

We report on the results of a joint experimental and numerical study on the sub-cycle laser field-driven electron dynamics that underlie the population of highly excited electronic states in multiply ionized argon dimers by electron recapture processes. Our experiments using few-cycle laser pulses with a known carrier-envelope phase (CEP) in combination with reaction microscopy reveal a distinct CEP-dependence of the electron emission and recapture process and, furthermore, a small but significant CEP-offset to the scenario in which no excited argon dimers are produced. With the help of classical ensemble trajectory simulations we trace down these different CEP-dependencies to subtle differences in the laser-driven sub-cycle electron trajectory dynamics that involve in both cases the transfer of an electron from one argon ion across the system boundary to the neighboring ion and its transient capture on this ion. [ABSTRACT FROM AUTHOR]

Attoclock provides a powerful tool for probing the ultrafast electron dynamics in strong laser fields. However, this technique has remained restricted to single electron or sequential double ionized electron dynamics. Here, we propose a novel attoclock scheme with a polarization-gated few-cycle laser pulse and demonstrate its application in timing the correlated-electron emission in strong field double ionization of argon. Our experimental measurements reveal that the correlated-electron emission occurs mainly through two channels with time differences of 234±22 as and 1043±73 as, respectively. Classical model calculations well reproduce the experimental results and deepen our understanding of ultrafast electron correlation dynamics.

We present theoretically obtained photoelectron momentum distributions (PMDs) for the strong field ionization of argon in an elliptically polarized laser field at a central wavelength of 400 nm. Three different theoretical approaches, namely, a numerical solution of the time-dependent Schrödinger equation (TDSE), a nonadiabatic model, and a classical-trajectory Monte Carlo (CTMC) model are adopted in our calculations. From the TDSE calculations, it is found that the attoclock offset angle (most probable electron emission angles with respect to the minor axis of the laser's polarization ellipse) in the PMD increases with rising ATI order. While this result cannot be reproduced by the CTMC model, the nonadiabatic model achieves good agreement with the TDSE result. Analysis shows that the nonadiabatic corrections of the photoelectron initial momentum distribution (in both longitudinal and transverse directions with respect to the tunneling direction) and nonadiabatic correction of the tunneling exit are responsible for the ATI order-dependent angular shift.

We report a novel, to the best of our knowledge, double-quantum-zero-quantum two-dimensional coherent spectroscopy (2DCS) that allows direct detection of the quantum coherence between multiparticle collective states. Through correlating the double-quantum coherence and the zero-quantum coherence, signatures for coherence between collective states can be well isolated as side peaks and readily identified in the 2D spectrum. The experiment is implemented in a vapor of rubidium atoms in a collinear 2DCS setup. Good agreement with a theoretical simulation using density matrix confirms the essential role of the interatomic correlation effect in generating the side peak signals. This 2D spectrum technique paves a new avenue for studying the coherent coupling of highly excited states and many-body properties.

We report on an experimental and theoretical study of the ionization-fragmentation dynamics of argon dimers in intense few-cycle laser pulses with a tagged carrier-envelope phase. We find that a field-driven electron transfer process from one argon atom across the system boundary to the other argon atom triggers subcycle electron-electron interaction dynamics in the neighboring atom. This attosecond electron-transfer process between distant entities and its implications manifests itself as a distinct phase-shift between the measured asymmetry of electron emission curves of the Ar^{+}+Ar^{2+} and Ar^{2+}+Ar^{2+} fragmentation channels. This letter discloses a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving intermolecular electron-transfer processes.

Optical double-quantum two-dimensional coherent spectroscopy (2DCS) was implemented to probe interatomic dipole-dipole interactions in both potassium and rubidium atomic vapors. The dipole-dipole interaction was detected at densities of 4.81×10 8 cm -3 and 8.40×10 9 cm -3 for potassium and rubidium, respectively, corresponding to a mean interatomic separation of 15.8 μ m or 3.0×10 5 a 0 for potassium and 6.1 μ m or 1.2×10 5 a 0 for rubidium, where a 0 is the Bohr radius. The experimental results confirm the long range nature of the dipole-dipole interaction, which is critical for understanding many-body physics in atoms/molecules. The long range interaction also has implications in atom-based applications involving many-body interactions. Additionally, we demonstrated that double-quantum 2DCS is sufficiently sensitive to probe dipole-dipole interaction at densities that can be achieved with cold atom in a magneto-optical trap, paving the way for double-quantum 2DCS studies of cold atoms and molecules. The method can also open a new avenue to study long-range interactions in solid state systems such as quantum dots and color centers in diamonds.

We experimentally investigate the two-dimensional photoelectron momentum spectra of aligned diatomic molecules in an intense laser field. Our results reveal a novel prominent valley structure in the molecular alignment dependence of the high-energy photoelectron spectra along the laser polarization. Resorting to the molecular strong-field approximation and a simple semiclassical analysis, we show that this valley structure stems from the destructive two-center interference of the laser-driven rescattered electrons in diatomic molecules. Based on this two-center interference with aligned diatomic molecules, we demonstrate for the first time a tomographic method to extract the molecular internuclear separation, providing a more straightforward approach of molecular imaging, in comparison with, e.g., laser-induced electron diffraction and fixed-angle broadband laser-driven electron scattering.

We use orthogonally polarized two-color (OTC) laser pulses to separate quantum paths in the multiphoton ionization of Ar atoms. Our OTC pulses consist of 400 and 800 nm light at a relative intensity ratio of 10∶1. We find a hitherto unobserved interference in the photoelectron momentum distribution, which exhibits a strong dependence on the relative phase of the OTC pulse. Analysis of model calculations reveals that the interference is caused by quantum pathways from nonadjacent quarter cycles.

In this Letter, we propose a novel laser-induced inelastic diffraction (LIID) scheme based on the intense-field-driven atomic nonsequential double ionization (NSDI) process and demonstrate that, with this LIID approach, the doubly differential cross sections (DDCSs) of the target ions, e.g., Ar^{+} and Xe^{+}, can be accurately extracted from the two-dimensional photoelectron momentum distributions in the NSDI process of the corresponding atoms. The extracted DDCSs exhibit a strong dependence on both the target and the laser intensity, in good agreement with calculated DDCSs from the scattering of free electrons. The LIID scheme may be extended to molecular systems and provides a promising approach for imaging of the gas-phase molecular dynamics induced by a strong laser field with unprecedented spatial and temporal resolution.

We conceive an improved procedure to determine the laser intensity with the momentum distributions from nonadiabatic tunneling ionization of atoms in the close-to-circularly polarized laser fields. The measurements for several noble gas atoms are in accordance with the semiclassical calculations, where the nonadiabatic effect and the influence of Coulomb potential are included. Furthermore, the high-order above-threshold ionization spectrum in linearly polarized laser fields for Ar is measured and compared with the numerical calculation of the time-dependent Schrödinger equation in the single-active-electron approximation to test the accuracy of the calibrated laser intensity.