Directly imaging excited state-resolved transient structures of water induced by valence and inner-shell ionisation.

Real-time imaging of transient structure of the electronic excited state is fundamentally critical to understand and control ultrafast molecular dynamics. The ejection of electrons from the inner-shell and valence level can lead to the population of different excited states, which trigger manifold ultrafast relaxation processes, however, the accurate imaging of such electronic state-dependent structural evolutions is still lacking. Here, by developing the laser-induced electron recollision-assisted Coulomb explosion imaging approach and molecular dynamics simulations, snapshots of the vibrational wave-packets of the excited (A) and ground states (X) of D2O+ are captured simultaneously with sub-10 picometre and few-femtosecond precision. We visualise that θDOD and ROD are significantly increased by around 50∘ and 10 pm, respectively, within approximately 8 fs after initial ionisation for the A state, and the ROD further extends 9 pm within 2 fs along the ground state of the dication in the present condition. Moreover, the ROD can stretch more than 50 pm within 5 fs along autoionisation state of dication. The accuracies of the results are limited by the simulations. These results provide comprehensive structural information for studying the fascinating molecular dynamics of water, and pave the way towards to make a movie of excited state-resolved ultrafast molecular dynamics and light-induced chemical reaction.

Triple ionization and fragmentation of benzene trimers following ultrafast intermolecular Coulombic decay.

Intermolecular interactions involving aromatic rings are ubiquitous in biochemistry and they govern the properties of many organic materials. Nevertheless, our understanding of the structures and dynamics of aromatic clusters remains incomplete, in particular for systems beyond the dimers, despite their high presence in many macromolecular systems such as DNA and proteins. Here, we study the fragmentation dynamics of benzene trimer that represents a prototype of higher-order aromatic clusters. The trimers are initially ionized by electron-collision with the creation of a deep-lying carbon 2s-1 state or one outer-valence and one inner-valence vacancies at two separate molecules. The system can thus relax via ultrafast intermolecular decay mechanisms, leading to the formation of C[Formula: see text]C[Formula: see text]C[Formula: see text] trications and followed by a concerted three-body Coulomb explosion. Triple-coincidence ion momentum spectroscopy, accompanied by ab-initio calculations and further supported by strong-field laser experiments, allows us to elucidate the details on the fragmentation dynamics of benzene trimers.

Femtosecond Time-Resolved Neighbor Roles in the Fragmentation Dynamics of Molecules in a Dimer.

How the neighbor effect plays its role in the fragmentation of molecular clusters attracts great attention for physicists and chemists. Here, we study this effect in the fragmentation of N_{2}O dimer by performing three-body coincidence measurements on the femtosecond timescale. Rotations of bound N_{2}O^{+} triggered by neutral or ionic neighbors are tracked. The forbidden dissociation path between B^{2}Π and ^{4}Π is opened by the spin-exchange effect due to the existence of neighbor ions, leading to a new channel of N_{2}O^{+}→NO+N^{+} originating from B^{2}Π. The formation and dissociation of the metastable product N_{3}O_{2}^{+} from two ion-molecule reaction channels are tracked in real time, and the corresponding trajectories are captured. Our results demonstrate a significant and promising step towards the understanding of neighbor roles in the reactions within clusters.

Research Progress of Photo-/Electro-Driven Thermochromic Smart Windows.

Thermochromic smart windows can automatically control solar radiation according to the ambient temperature. Compared with photochromic and electrochromic smart windows, they have a stronger applicability and lower energy consumption, and have a wide range of application prospects in the field of building energy efficiency. At present, aiming at the challenge of the high transition temperature of thermochromic smart windows, a large amount of innovative research has been carried out via the principle that thermochromic materials can be driven to change their optical performance by photothermal or electrothermal effects at room temperature. Based on this, the research progress of photo- and electro-driven thermochromic smart windows is summarized from VO2-based composites, hydrogels and liquid crystals, and it is pointed out that there are two main development trends of photo-/electro-driven thermochromic smart windows. One is exploring the diversified combination methods of photothermal materials and thermochromic materials, and the other is developing low-cost large-area heating electrodes.

Revealing Molecular Strong Field Autoionization Dynamics.

The novel strong field autoionization (SFAI) dynamics is identified and investigated by channel-resolved angular streaking measurements of two electrons and two ions for the double-ionized CO. Comparing with the laser-assisted autoionization calculations, we demonstrate the electrons from SFAI are generated from the field-induced decay of the autoionizing state with a following acceleration in the laser fields. The energy-dependent photoelectron angular distributions further reveal that the subcycle ac-Stark effect modulates the lifetime of the autoionizing state and controls the emission of SFAI electrons in molecular frame. Our results pave the way to control the emission of resonant high-harmonic generation and trace the electron-electron correlation and electron-nuclear coupling by strong laser fields. The lifetime modulation of quantum systems in the strong laser field has great potential for quantum manipulation of chemical reactions and beyond.

Accurate in situ Measurement of Ellipticity Based on Subcycle Ionization Dynamics.

Elliptically polarized laser pulses (EPLPs) are widely applied in many fields of ultrafast sciences, but the ellipticity (ϵ) has never been in situ measured in the interaction zone of the laser focus. In this Letter, we propose and realize a robust scheme to retrieve the ϵ by temporally overlapping two identical counterrotating EPLPs. The combined linearly electric field is coherently controlled to ionize Xe atoms by varying the phase delay between the two EPLPs. The electron spectra of the above-threshold ionization and the ion yield are sensitively modulated by the phase delay. We demonstrate that these modulations can be used to accurately determine ϵ of the EPLP. We show that the present method is highly reliable and is applicable in a wide range of laser parameters. The accurate retrieval of ϵ offers a better characterization of a laser pulse, promising a more delicate and quantitative control of the subcycle dynamics in many strong field processes.

Ultrafast proton migration and Coulomb explosion of methyl chloride in intense laser fields.

We investigated the ultrafast proton migration and the Coulomb explosion (CE) dynamics of methyl chloride (CH3Cl) in intense femtosecond laser fields at the wavelengths of 800 nm (5.5 × 1014 W/cm2) and 400 nm (4 × 1014 W/cm2), respectively. Various fragment channels from molecular dication and trication were observed by coincidence momentum imaging through the measurement of their kinetic energy releases (KERs). The proton migration from different charged parent ions was analyzed from the obtained KER distributions. For the direct CE channel of CH3+ + Cl+ and CH3+ + Cl2+, the contribution of multiply excited electronic states and multicharged states is identified. In addition, the measurements of relative yields of the fragmentation channel at different laser wavelengths provide a selective control of proton migration for CH3Cl molecules in intense laser fields.