Attosecond Imaging of Electronic Wave Packets.

An electronic wave packet has significant spatial evolution besides its temporal evolution, due to the delocalized nature of composing electronic states. The spatial evolution was not previously accessible to experimental investigations at the attosecond timescale. A phase-resolved two-electron-angular-streaking method is developed to image the shape of the hole density of an ultrafast spin-orbit wave packet in the krypton cation. Furthermore, the motion of an even faster wave packet in the xenon cation is captured for the first time: An electronic hole is refilled 1.2 fs after it is produced, and the hole filling is observed on the opposite side where the hole is born.

Ellipticity controlled dissociative double ionization of ethane by strong fields.

The yields of all dissociation channels of ethane dications produced by strong field double ionization were measured. It was found that the branching ratios can be controlled by varying the ellipticity of laser pulses. The CH3+ formation and H+ formation channels show a clear competition, producing the highest and lowest branching ratios at ellipticity of ∼0.6, respectively. With the help of theoretical calculations, such a control was attributed to the ellipticity dependent yields of different sequential ionization pathways.

Developing a camera-based 3D momentum imaging system capable of 1 Mhits/s.

A camera-based three-dimensional (3D) imaging system with a superb time-of-flight (TOF) resolution and multi-hit capability was recently developed for electron/ion imaging [Lee et al. J. Chem. Phys. 141, 221101 (2014)]. In this work, we report further improvement of the event rate of the system by adopting an event-driven camera, Tpx3Cam, for detecting the 2D positions of electrons, while a high-speed digitizer provides highly accurate (∼30 ps) TOF information for each event at a rate approaching 1 Mhits/sec.

Direct in-situ single-shot measurements of the absolute carrier-envelope phases of ultrashort pulses.

Many important physical processes such as nonlinear optics and coherent control are highly sensitive to the absolute carrier-envelope phase (CEP) of driving ultrashort laser pulses. This makes the measurement of CEP immensely important in relevant fields. Even though relative CEPs can be measured with a few existing technologies, the estimate of the absolute CEP is not straightforward and always requires theoretical inputs. Here, we demonstrate a novel in-situ technique based on angular streaking that can achieve such a goal without complicated calibration procedures. Single-shot measurements of the absolute CEP have been achieved with an estimated precision of 0.19 radians.

Disentangling Strong-Field Multielectron Dynamics with Angular Streaking.

The study into the interaction between a strong laser field and atoms/molecules has led to significant advances in developing spectroscopic tools in the attosecond time-domain and methods for controlling chemical reactions. There has been great interest in understanding the complex electronic and nuclear dynamics of molecules in strong laser fields. However, it is still a formidable challenge to fully model such dynamics. Conventional experimental tools such as photoelectron spectroscopy encounter difficulties in revealing the involved states because the electron spectra are largely dictated by the property of the laser field. Here, with strong field angular streaking technique, we measure the angle-dependent ionization yields that directly reflect the symmetry of the ionizing orbitals of methyl iodide and thus reveal the ionization/dissociation dynamics. Moreover, kinematically complete measurements of momentum vectors of all fragments in dissociative double ionization processes allow access to electron-momentum correlations that reveal correlated multielectron dynamics.