Abstract: The time delay of photoelectron emission serves as a fundamental building block to understand the ultrafast electron emission dynamics in strong-field physics. Here, we study the photoelectron angular streaking of CO molecules by using two-color ( 400+800nm) corotating circularly polarized fields. By coincidently measuring photoelectrons with the dissociative ions, we present molecular frame photoelectron angular distributions with respect to the instantaneous driving electric field signatures. We develop a semiclassical nonadiabatic molecular quantum-trajectory Monte Carlo (MO-QTMC) model that fully captures the experimental observations and further ab initio simulations. We disentangle the orientation-resolved contribution of the anisotropic ionic potential and the molecular orbital structure on the measured photoelectron angular distributions. Furthermore, by analyzing the photoelectron interference patterns, we extract the sub-Coulomb-barrier phase distribution of the photoelectron wavepacket and reconstruct the orientation- and energy-resolved Wigner time delay in the molecular frame. Holographic angular streaking with bicircular fields can be used for probing polyatomic molecules in the future.
Abstract: More than ten years ago, the observation of the low-energy structure in the photoelectron energy spectrum, regarded as an “ionization surprise,” has overthrown our understanding of strong-field physics. However, the similar low-energy nuclear fragment generation from dissociating molecules upon the photon energy absorption, one of the well-observed phenomena in light-molecule interaction, still lacks an unambiguous mechanism and remains mysterious. Here, we introduce a time-energy-resolved manner using a multicycle near-infrared femtosecond laser pulse to identify the physical origin of the light-induced ultrafast dynamics of molecules. By simultaneously measuring the bond-stretching times and photon numbers involved in the dissociation of H2+ driven by a polarization-skewed laser pulse, we reveal that the low-energy protons (below 0.7 eV) are produced via dipole-transitions at large bond lengths. The observed low-energy protons originate from strong-field dissociation of high vibrational states rather than the low ones of H2+ cation, which is distinct from the well-accepted bond-softening picture. Further numerical simulation of the time-dependent Schrödinger equation unveils that the electronic states are periodically distorted by the strong laser field, and the energy gap between the field-dressed transient electronic states may favor the one- or three-photon transitions at the internuclear distance larger than 5 a.u. The time-dependent scenario and our time-energy-resolved approach presented here can be extended to other molecules to understand the complex ultrafast dynamics.
Abstract: Remote or standoff detection of greenhouse gases, air pollutants, and biological agents with innovative ultrafast laser technology attracts growing interests in recent years. Hybrid femtosecond/picosecond coherent Raman spectroscopy is considered as one of the most versatile techniques due to its great advantages in terms of detection sensitivity and chemical specificity. However, the simultaneous requirement for the femtosecond pump and the picosecond probe increases the complexity of optical system. Herein, we demonstrate that air lasing naturally created inside a filament can serve as an ideal light source to probe Raman coherence excited by the femtosecond pump, producing coherent Raman signal with molecular vibrational signatures. The combination of pulse self-compression effect and air lasing action during filamentation improves Raman excitation efficiency and greatly simplifies the experimental setup. The air-lasing-assisted Raman spectroscopy was applied to quantitatively detect greenhouse gases mixed in air, and it was found that the minimum detectable concentrations of CO2 and SF6 can reach 0.1% and 0.03%, respectively. The ingenious designs, especially the optimization of pump-seed delay and the choice of perpendicular polarization, ensure a high detection sensitivity and signal stability. Moreover, it is demonstrated that this method can be used for simultaneously measuring CO2 and SF6 gases and distinguishing 12CO2 and 13CO2. The developed scheme provides a new route for high-sensitivity standoff detection and combustion diagnosis.