We demonstrate a deep-learning neural network (DNN) method for the measurement of molecular alignment by using the molecular-alignment-based cross-correlation polarization-gating frequency resolved optical gating (M-XFROG) technique. Our network has the capacity for direct measurement of molecular alignment from the FROG traces. In a proof-of-principle experiment, we have demonstrated our method in O2 molecules. With our method, the molecular alignment factor ⟨cos2θ⟩(t) of O2, impulsively excited by a pump pulse, was directly reconstructed. The accuracy and validity of the reconstruction have been verified by comparison with the simulations based on experimental parameters.

In quantum mechanics, when an electron is quickly ripped off from a molecule, a superposition of new eigenstates of the cation creates an electron wave packet that governs the charge flow inside, which has been called charge migration (CM). Experimentally, extracting such dynamics at its natural (attosecond) timescale is quite difficult. We report the first such experiment in a linear carbon-chain molecule, butadiyne (C₄H₂), via high-harmonic spectroscopy (HHS). By employing advanced theoretical and computational tools, we showed that the wave packet and the CM of a single molecule are reconstructed from the harmonic spectra for each fixed-in-space angle of the molecule. For this one-dimensional molecule, we calculate the center of charge ⟨ x ⟩ ( t ) to obtain v_cm, to quantify the migration speed and how it depends on the orientation angle. The findings also uncover how the electron dynamics at the first few tens to hundreds of attoseconds depends on molecular structure. The method can be extended to other molecules where the HHS technique can be employed.

We propose and numerically demonstrate a simple and background-free all-optical chiral spectroscopy technique for gas molecules. Our approach is based on high harmonic generation driven by a new type of laser beam that is produced by one linearly polarized single-color beam passing through a lens and a prism. It is shown that chiral and achiral signals are completely separated in frequency, indicating strong background-free and highly sensitive chirality detection. We believe this all-optical method can open new opportunities for ultrafast detection for chiral dynamics in the femtoseond to attosecond time scale.

台式阿秒相干光源在过去20多年取得了飞速的发展，其研究重心已经从早期的产生与测量机理的探索逐渐过渡到了极端时间尺度超快过程的追踪及操控上。目前阿秒时间分辨的谱学技术不仅能实现简单的原子分子体系瞬态过程的直接追踪，还被逐步应用到化学分子、生物分子、固体材料等复杂体系的测量中。本文回顾了基于阿秒光源的超快测量技术的发展，介绍了相关技术的原理及其在物理、化学、信息科学领域的应用研究。

Tunneling ionization of atoms and molecules induced by intense laser pulses contains the contributions of numerous quantum orbits. Identifying the contributions of these orbits is crucial for exploring the application of tunneling and for understanding various tunneling-triggered strong-field phenomena. We perform a combined experimental and theoretical study to identify the relative contributions of the quantum orbits corresponding to the electrons tunneling ionized during the adjacent rising and falling quarter cycles of the electric field of the laser pulse. In our scheme, a perturbative second-harmonic field is added to the fundamental driving field. By analyzing the relative phase dependence of the signal in the photoelectron momentum distribution, the relative contributions of these two orbits are unambiguously determined. Our results show that their relative contributions sensitively depend on the longitudinal momentum and modulate with the transverse momentum of the photoelectron, which is attributed to the interference of the electron wave packets of the long orbit. The relative contributions of these orbits resolved here are important for the application of strong-field tunneling ionization as a photoelectron spectroscopy for attosecond time-resolved measurements.

The nonlinear Talbot effect is a near-field nonlinear diffraction phenomenon in which the self-imaging of periodic objects is formed by the second harmonics of the incident laser beam. We demonstrate the first, to the best of our knowledge, example of nonlinear Talbot self-healing, i.e., the capability of creating defect-free images from faulty nonlinear optical structures. In particular, we employ the tightly focused femtosecond infrared optical pulses to fabricate LiNbO3 nonlinear photonic crystals and show that the defects in the form of the missing points of two-dimensional square and hexagonal periodic structures are restored in the second harmonic images at the first nonlinear Talbot plane. The observed nonlinear Talbot self-healing opens up new possibilities for defect-tolerant optical lithography and printing.

We investigate the Airy–Talbot effect of an Airy pulse train in time-dependent linear potentials. The parabolic trajectory of self-imaging depends on both the dispersion sign and the linear potential gradient. By imposing linear phase modulations on the pulse train, the Airy–Talbot effects accompanied with positive and negative refractions are realized. For an input composed of stationary Airy pulses, the self-imaging follows straight lines, and the Airy–Talbot distance can be engineered by varying the linear potential gradient. The effect is also achieved in symmetric linear potentials. The study provides opportunities to control the self-imaging of aperiodic optical fields in time dimension.

Using the classical-trajectory Monte Carlo model, we have theoretically studied the angular momentum distribution of frustrated tunneling ionization (FTI) of atoms in strong laser fields. Our results show that the angular momentum distribution of the FTI events exhibits a double-hump structure. With this classical model, we back traced the tunneling coordinates, i.e., the tunneling time and initial transverse momentum at tunneling ionization. It is shown that for the events tunneling ionized at the rising edge of the electric field, the final angular momentum exhibits a strong dependence on the initial transverse momentum at tunneling. While for the events ionized at the falling edge, there is a relatively harder recollision between the returning electron and the parent ion, leading to the angular momentum losing the correlation with the initial transverse momentum. Our study suggests that the angular momentum of the FTI events could be manipulated by controlling the initial coordinates of the tunneling ionization.