Probing H_{2} Double Ionization with Bicircular Laser Fields.

We present a kinematically complete study on strong-field double ionization of H_{2} molecules in two-color bicircular laser fields. The releasing times of electrons and protons are recorded with the double-hand attoclock. We observe the relative emission angles of two electrons oscillate with the kinetic energy release of protons, indicating the internal concerted four-body fragmentation. Using a three-dimensional molecular semiclassical ensemble model, we have disentangled the attosecond correlated electron emission in H_{2} double ionization. This work reveals the strong electron-nuclear coupling in the molecular bond breaking and may open up a new approach to experimentally accessing the intramolecular electron and bond dynamics with bicircular fields.

Ultrafast Imaging of Jahn-Teller Distortion and the Correlated Proton Migration in Photoionized Cyclopropane.

The Jahn-Teller (JT) distortion is one of the fundamental processes in molecules and condensed phase matters. For photoionized organic molecules with high symmetry, the JT effect leads to geometric instability in certain electron configurations and thus has a significant effect on the subsequent isomerization and proton migration processes. Utilizing the femtosecond pump-probe Coulomb explosion method, we probe the isomerization dynamics process of a monovalent cyclopropane cation (C3H6+) caused by proton migration and reveal the relationship between proton migration and JT distortion. We found that the C3H6+ cation evolves from the D3h symmetric equilateral triangle geometry either to the acute triangle via two elongated C-C bonds (JT1) or to the obtuse triangle via a single elongated C-C bond (JT2). The JT1 pathway does not involve proton migration, while the JT2 pathway drives proton migration and can be mapped into the indirect dissociation channel of Coulomb explosion. The time-resolved experiment indicates that the delay time between those two JT pathways can be as large as ∼600 fs. After the JT distortion, the cyclopropane cation undergoes a subsequent structural evolution, which brings a greater variety of dissociation channels.

Enhanced arsenic removal by graphene oxide chitosan composites through FeOx decoration: Influences and mechanism.

Iron decoration has been recognized as one of the most important paths to enhance contaminant adsorption by carbon-based composites. In this study, varying amounts of Fe (II) are used for the modification of graphene oxide chitosan (GOCS) materials to assess the impact of iron oxide (FeOx) morphology on the composites and their efficiency in arsenic (As) removal. Results show that incorporating 0.08 mol Fe(II) into GOCS yields better As removal performance, leading to a remarkable enhancement by 5 times for As(V) and 6 times for As(III). The iron minerals in the material consist of goethite (FeO(OH)) and magnetite (Fe3O4), with FeO(OH) playing a predominant role in As removal through the complexation and electrostatic attraction of -OH and Fe - O groups. The adsorption capacity for As (Qe) decreases with the increasing pH and the mass and volume ratio (m/v) but increases with the increasing initial concentration (C0). Besides, the presence of SO42- and HPO42- can significantly reduce As removal by the FeOx-modified GOCS. Under the conditions of pH = 3, m/v = 1.0 g/L, and C0 = 10 mg/L, a maximum Qe value reaches 61.94 mg/g. The adsorption is well-fitted to a pseudo-second-order kinetic model and is an endothermic, spontaneous, and monolayer adsorption process.

Topologically Protected Strong-Interaction of Photonics with Free Electrons.

We propose a robust scheme of studying the strong interactions between free electrons and photons using topological photonics. Our study reveals that the topological corner state can be used to enhance the interaction between light and a free electron significantly. The quality factor of the topological cavity can exceed 20 000 and the corner state has a very long lifetime even after the pump pulse is off. And thus, the platform enables us to achieve a strong interaction without the need for zero delay and phase matching as in traditional photon-induced near-field electron microscopy (PINEM). This work provides the new perspective that the topological photonic structures can be utilized as a platform to shape free electron wave packets, which facilitates the control of quantum electrodynamical (QED) processes and quantum optics with free electrons in the future.

Probing Conical Intersection in the Multipathway Isomerization of CH3Cl Using Coulomb Explosion.

Ubiquitous ultrafast isomerization is paramount in photoexcited molecules, in which non-adiabatic coupling among multiple electronic states can occur. We use the pump-probe Coulomb explosion imaging method to study the isomerization of CH3Cl molecules. We find that the isomerization under our strong field pump-probe scheme proceeds along multiple pathways, which are encoded in several distinct branches of the time-resolved kinetic energy release spectra for the CH2++HCl+ Coulomb explosion channel. Apart from the isomerized dissociative pathway in neutral and cationic excited states, the pump laser can also induce coherent vibrational dynamics in two coupled intermediate states and set up the initial conditions for the two concurrently proceeding isomerization pathways. The isomerization of CH3Cl provides an intriguing example of a chemical reaction consisting of multiple pathways and non-adiabatic dynamics.

Spatiotemporal imaging and shaping of electron wave functions using novel attoclock interferometry.

Electrons detached from atoms by photoionization carry valuable information about light-atom interactions. Characterizing and shaping the electron wave function on its natural timescale is of paramount importance for understanding and controlling ultrafast electron dynamics in atoms, molecules and condensed matter. Here we propose a novel attoclock interferometry to shape and image the electron wave function in atomic photoionization. Using a combination of a strong circularly polarized second harmonic and a weak linearly polarized fundamental field, we spatiotemporally modulate the atomic potential barrier and shape the electron wave functions, which are mapped into a temporal interferometry. By analyzing the two-color phase-resolved and angle-resolved photoelectron interference, we are able to reconstruct the spatiotemporal evolution of the shaping on the amplitude and phase of electron wave function in momentum space within the optical cycle, from which we identify the quantum nature of strong-field ionization and reveal the effect of the spatiotemporal properties of atomic potential on the departing electron. This study provides a new approach for spatiotemporal shaping and imaging of electron wave function in intense light-matter interactions and holds great potential for resolving ultrafast electronic dynamics in molecules, solids, and liquids.

Amplification of light pulses with orbital angular momentum (OAM) in nitrogen ions lasing.

Nitrogen ions pumped by intense femtosecond laser pulses give rise to optical amplification in the ultraviolet range. Here, we demonstrated that a seed light pulse carrying orbital angular momentum (OAM) can be significantly amplified in nitrogen plasma excited by a Gaussian femtosecond laser pulse. With the topological charge of ℓ = ±1, we observed an energy amplification of the seed light pulse by two orders of magnitude, while the amplified pulse carries the same OAM as the incident seed pulse. Moreover, we show that a spatial misalignment of the plasma amplifier with the OAM seed beam leads to an amplified emission of Gaussian mode without OAM, due to the special spatial profile of the OAM seed pulse that presents a donut-shaped intensity distribution. Utilizing this misalignment, we can implement an optical switch that toggles the output signal between Gaussian mode and OAM mode. This work not only certifies the phase transfer from the seed light to the amplified signal, but also highlights the important role of spatial overlap of the donut-shaped seed beam with the gain region of the nitrogen plasma for the achievement of OAM beam amplification.

Ultrafast Electronic Dynamics in Anisotropic Indirect Interlayer Excitonic States of Monolayer WSe2/ReS2 Heterojunctions.

Understanding ultrafast electronic dynamics of the interlayer excitonic states in atomically thin transition metal dichalcogenides is of importance in engineering valleytronics and developing excitonic integrated circuits. In this work, we experimentally explored the ultrafast dynamics of indirect interlayer excitonic states in monolayer type II WSe2/ReS2 heterojunctions using time-resolved photoemission electron microscopy, which reveals its anisotropic behavior. The ultrafast cooling and decay of excited-state electrons exhibit significant linear dichroism. The ab initio theoretical calculations provide unambiguous evidence that this linear dichroism result is primarily associated with the anisotropic nonradiative recombination of indirect interlayer excitonic states. Measuring time-resolved photoemission energy spectra, we have further revealed the ultrafast evolution of excited-state electrons in anisotropic indirect interlayer excitonic states. The findings have important implications for controlling the interlayer moiré excitonic effects and designing anisotropic optoelectronic devices.

Imaging and Controlling Ultrafast Electron Pulses Emitted from Plasmonic Nanostructures.

We experimentally study photoemission from gold nanodisk arrays using space-, time-, and energy-resolved photoemission electron microscopy. When excited by a plasmonic resonant infrared (IR) laser pulse, plasmonic hotspots are generated owing to local surface plasmon resonance. Photoelectrons emitted from each plasmonic hotspot form a nanoscale and ultrashort electron pulse. When the system is excited by an extreme ultraviolet (EUV) laser pulse, a uniformly distributed photoelectron cloud is formed across the sample surface. When excited by the IR and EUV laser pulses together, both the photoemission image and kinetic energy vary significantly for the IR laser-generated electrons depending on the time delay between the two laser pulses. These observations are well explained by the Coulomb interaction with the EUV laser-generated electron cloud. Our study offers a feasible approach to manipulate the energy of electron pulse emitted from a plasmonic nanostructure on an ultrafast time scale.

Strong-Field Ionization of Hydrogen Atoms with Quantum Light.

We study the strong-field ionization driven by quantum lights. Developing a quantum-optical-corrected strong-field approximation model, we simulate the photoelectron momentum distribution with squeezed-state light, which manifests as notably different interference structures from that with coherent-state (classical) light. With the saddle-point method, we analyze the electron dynamics and reveal that the photon statistics of squeezed-state light fields endows the tunneling electron wave packets with a time-varying phase uncertainty and modulates the photoelectron intracycle and intercycle interferences. Moreover, it is found the fluctuation of quantum light imprints significant influence on the propagation of tunneling electron wave packets, in which the ionization probability of electrons is considerably modified in time domain.

Generating optical cat states via quantum interference of multi-path free-electron-photons interactions.

The novel quantum effects induced by the free-electron-photons interaction have attracted increasing interest due to their potential applications in ultrafast quantum information processing. Here, we propose a scheme to generate optical cat states based on the quantum interference of multi-path free-electron-photons interactions that take place simultaneously with strong coupling strength. By performing a projection measurement on the electron, the state of light changes significantly from a coherent state into a non-Gaussian state with either Wigner negativity or squeezing property, both possess metrological power to achieve quantum advantage. More importantly, we show that the Wigner negativity oscillates with the coupling strength, and the optical cat states are successfully generated with high fidelity at all the oscillation peaks. This oscillation reveals the quantum interference effect of the multiple quantum pathways in the interaction of the electron with photons, by that various nonclassical states of light are promising to be fast prepared and manipulated. These findings inspire further exploration of emergent quantum phenomena and advanced quantum technologies with free electrons.

Geometric Phase Effect in Attosecond Stimulated X-ray Raman Spectroscopy.

Conical intersections (CIs) are diabolical points in the potential energy surfaces generally caused by point-wise degeneracy of different electronic states, and give rise to the geometric phases (GPs) of molecular wave functions. Here we theoretically propose and demonstrate that the transient redistribution of ultrafast electronic coherence in attosecond Raman signal (TRUECARS) spectroscopy is capable of detecting the GP effect in excited state molecules by applying two probe pulses including an attosecond and a femtosecond X-ray pulse. The mechanism is based on a set of symmetry selection rules in the presence of nontrivial GPs. The model of this work can be realized for probing the geometric phase effect in the excited state dynamics of complex molecules with appropriate symmetries, using attosecond light sources such as free-electron X-ray lasers.

As(III) removal by a recyclable granular adsorbent through dopping Fe-Mn binary oxides into graphene oxide chitosan.

Graphene oxide chitosan composite (GOCS) is recognized as an environmentally friendly composite adsorbent because of its stability and abundant functional groups to adsorb heavy metals, and Fe-Mn binary oxides (FMBO) have attracted increasing interest due to their high removal capacity of As(III). However, GOCS is often inefficient for heavy metal adsorption and FMBO suffers poor regeneration for As(III) removal. In this study, we have proposed a method of dopping FMBO into GOCS to obtain a recyclable granular adsorbent (Fe/MnGOCS) for achieving As(III) removal from aqueous solutions. Characterization of BET, SEM-EDS, XRD, FTIR, and XPS are carried out to confirm the formation of Fe/MnGOCS and As(III) removal mechanism. Batch experiments are conducted to investigate the effects of operational factors (pH, dosage, coexisting ions, etc.), as well as kinetic, isothermal, and thermodynamic processes. Results show that the removal efficiency (Re) of As(III) by Fe/MnGOCS is about 96 %, which is much higher than those of FeGOCS (66 %), MnGOCS (42 %), and GOCS (8 %), and it increases slightly with the increasing molar ratio of Mn and Fe. This is because amorphous Fe (hydro)oxides (mainly in the form of ferrihydrite) complexation with As(III) is the major mechanism to remove As(III) from aqueous solutions, and it is accompanied by As(III) oxidation mediated by Mn oxides and the complexation of As(III) with oxygen-containing functional groups of GOCS. Charge interaction plays a weaker role in As(III) adsorption, therefore Re is persistently high over a wide range of pH values of 3-10. But the coexisting PO43- can greatly decrease Re by 24.11 %. As(III) adsorption on Fe/MnGOCS is endothermic and its kinetic process is controlled by pseudo-second-order with a determination coefficient of 0.95. Fitted by the Langmuir isotherm, the maximum adsorption capacity is 108.89 mg/g at 25 °C. After four times regeneration, there is only a slight decrease of <10 % for the Re value. Column adsorption experiments show that Fe/MnGOCS can effectively reduce As(III) concentration from 10 mg/L to <10 µg/L. This study provides new insights into binary polymer composite modified by binary metal oxides to efficiently remove heavy metals from aquatic environments.

Trajectory-controlled high-order harmonic generation in ZnO crystals.

We experimentally and theoretically study high-order harmonic generation in zinc oxide crystals irradiated by mid-infrared lasers. The trajectories are mapped to the far field spatial distribution of harmonics. The divergence angles of on-axis and off-axis parts exhibit different dependences on the order of the harmonics. This observation can be theoretically reproduced by the coherent interference between the short and long trajectories with dephasing time longer than 0.5 optical cycle. Further, the relative contribution of the short and long trajectories is demonstrated to be accurately controlled by a one-color or two-color laser on the attosecond time scale. This work provides a reliable method to determine the electron dephasing time and demonstrates a versatile control of trajectory interference in the solid high-order harmonic generation.

Iron modified chitosan/coconut shell activated carbon composite beads for Cr(VI) removal from aqueous solution.

Iron modified chitosan/coconut shell activated carbon (Fe/CSCC) composite bead is synthesized to remove Cr(VI) and is characterized to reveal the influencing factors and reaction mechanism. Results show that the adsorption capacity (Qe) of Cr(VI) increases with the increase of iron loading, contact time (t), Cr(VI) initial concentration (C0), and temperature (T), but decreases with the increase of pH, and mass and volume ratio (m/v). After 0.1 mol FeCl3 modification, the removal efficiency of Cr(VI) by Fe/CSCC reaches as high as 97.25 % at pH = 3, m/v = 1.0 g/L, t = 2880 min, C0 = 25 mg/L, and T = 25 °C. The coexisting ions of SO42-, HPO4-, and Ca2+ lead to the decrease of Qe by 7.82, 5.05, and 5.50 mg/g, respectively, and the inhibition effect increases with their increasing concentrations. Fe/CSCC adsorption for Cr(VI) is an endothermic spontaneous process, and a chemical and monolayer adsorption, which is better fitted to a pseudo-second-order kinetic. The fitted maximum Qe is 64.49 mg/g by using the Langmuir model. Moreover, after five cycles of regeneration, the Qe value only drops about 3.46 mg/g. Characterization analysis of BET, XRD, FTIR, XPS, and SEM-EDS indicates that Cr(VI) is mainly adsorbed by Fe/CSCC through electrostatic attraction and complexation, which is related to the -COOH and - NH2 groups, and Fe - O groups, respectively.

On As(III) Adsorption Characteristics of Innovative Magnetite Graphene Oxide Chitosan Microsphere.

A magnetite graphene oxide chitosan (MGOCS) composite microsphere was specifically prepared to efficiently adsorb As(III) from aqueous solutions. The characterization analysis of BET, XRD, VSM, TG, FTIR, XPS, and SEM-EDS was used to identify the characteristics and adsorption mechanism. Batch experiments were carried out to determine the effects of the operational parameters and to evaluate the adsorption kinetic and equilibrium isotherm. The results show that the MGOCS composite microsphere with a particle size of about 1.5 mm can be prepared by a straightforward method of dropping FeCl2, graphene oxide (GO), and chitosan (CS) mixtures into NaOH solutions and then drying the mixed solutions at 45 °C. The produced MGOCS had a strong thermal stability with a mass loss of <30% below 620 °C. The specific surface area and saturation magnetization of the produced MGOCS was 66.85 m2/g and 24.35 emu/g, respectively. The As(III) adsorption capacity (Qe) and removal efficiency (Re) was only 0.25 mg/g and 5.81% for GOCS, respectively. After 0.08 mol of Fe3O4 modification, more than 53% of As(III) was efficiently removed by the formed MGOCS from aqueous solutions over a wide pH range of 5−10, and this was almost unaffected by temperature. The coexisting ion of PO43− decreased Qe from 3.81 mg/g to 1.32 mg/g, but Mn2+ increased Qe from 3.50 mg/g to 4.19 mg/g. The As(III) adsorption fitted the best to the pseudo-second-order kinetic model, and the maximum Qe was 20.72 mg/g as fitted by the Sips model. After four times regeneration, the Re value of As(III) slightly decreased from 76.2% to 73.8%, and no secondary pollution of Fe happened. Chemisorption is the major mechanism for As(III) adsorption, and As(III) was adsorbed on the surface and interior of the MGOCS, while the adsorbed As(III) was partially oxidized to As(V) accompanied by the reduction of Fe(III) to Fe(II). The produced As(V) was further adsorbed through ligand exchange (by forming Fe−O−As complexes) and electrostatic attraction, enhancing the As(III) removal. As an easily prepared and environmental-friendly composite, MGOCS not only greatly adsorbs As(III) but also effectively removes Cr(VI) and As(V) (Re > 60%) and other metals, showing a great advantage in the treatment of heavy metal-contaminated water.

Removal of Cr(VI) from Wastewater Using Graphene Oxide Chitosan Microspheres Modified with α-FeO(OH).

Graphene oxide and chitosan microspheres modified with α−FeO(OH) (α−FeO(OH)/GOCS) are prepared and utilized to investigate the performance and mechanism for Cr(VI) removal from aqueous solutions and the possibility of Fe secondary pollution. Batch experiments were carried out to identify the effects of pH, mass, and volume ratio (m/v), coexisting ions, time (t), temperature (T), and Cr(VI) initial concentration (C0) on Cr(VI) removal, and to evaluate adsorption kinetics, equilibrium isotherm, and thermodynamics, as well as the possibility of Fe secondary pollution. The results showed that Cr(VI) adsorption increased with C0, t, and T but decreased with increasing pH and m/v. Coexisting ions inhibited Cr(VI) adsorption, and this inhibition increased with increasing concentration. The influence degrees of anions and cations on the Cr(VI) adsorption in descending order were SO42− > PO42− > NO3− > Cl− and Ca2+ > Mg2+ > Mn2+, respectively. The equilibrium adsorption capacity of Cr(VI) was the highest at 24.16 mg/g, and the removal rate was 97.69% under pH = 3, m/v = 1.0 g/L, T = 298.15 K, and C0 = 25 mg/L. Cr(VI) adsorption was well fitted to a pseudo-second-order kinetic model and was spontaneous and endothermic. The best fit of Cr(VI) adsorption with the Langmuir and Sips models indicated that it was a monolayer and heterogeneous adsorption. The fitted maximum adsorption capacity was 63.19 mg/g using the Sips model under 308.15 K. Cr(VI) removal mainly included electrostatic attraction between Cr(VI) oxyanions with surface Fe−OH2+, and the adsorbed Cr(VI) was partially reduced to Cr(III) and then precipitated on the surface. In addition, there was no Fe secondary pollution during Cr(VI) adsorption.

Probing the orbital angular momentum of intense vortex pulses with strong-field ionization.

With the rapid development of femtosecond lasers, the generation and application of optical vortices have been extended to the regime of intense-light-matter interaction. The characterization of the orbital angular momentum (OAM) of intense vortex pulses is very critical. Here, we propose and demonstrate a novel photoelectron-based scheme that can in situ distinguish the OAM of the focused intense femtosecond optical vortices without the modification of light helical phase. We employ two-color co-rotating intense circular fields in the strong-field photoionization experiment, in which one color light field is a plane wave serving as the probing pulses and the other one is the vortex pulses whose OAM needs to be characterized. We show that by controlling the spatial profile of the probing pulses, the OAM of the vortex pulses can be clearly identified by measuring the corresponding photoelectron momentum distributions or angle-resolved yields. This work provides a novel in situ detection scenario for the light pulse vorticity and has implications for the studies of ultrafast and intense complex light fields with optical OAM.

Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Lasers, and Electron Pulses.

The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, X-ray, and electron sources have enabled the direct imaging of evolving molecular structures in chemical processes, and recent experimental advances in preparing ultrafast laser and electron pulses resulted in molecular imaging with femtosecond time resolution. This Perspective presents an overview of the versatile imaging methods of molecular dynamics. High-order harmonic generation imaging and photoelectron diffraction imaging are based on laser-induced ionization and rescattering processes. Coulomb explosion imaging retrieves molecular structural information by detecting the momentum vectors of fragmented ions. Diffraction imaging encodes molecular structural and electronic information in reciprocal space. We also present various applications of these ultrafast imaging methods in resolving laser-induced nuclear and electronic dynamics.

miR-181a Ameliorates the Progression of Myasthenia Gravis by Regulating TRIM9.

Abnormally activated CD4+ T cells are considered to be an important factor in the pathogenesis of myasthenia gravis (MG). In the pathogenesis of MG, the imbalance of proinflammatory cytokines and immune cells maintains the imbalance of immune response and inflammatory microenvironment. Studies have shown that miRNA is involved in the pathogenesis of MG. In our experiment, we extracted peripheral blood mononuclear cells (PBMCs) from MG patients and detected the expression of miR-181a and TRIM9 in PBMCs by qRT-PCR. In vitro experiments were conducted to explore the regulatory mechanism of miR-181a on target genes and its influence on inflammatory factors related to MG disease. Experimental autoimmune myasthenia gravis (EAMG) model mice are established, and the effects of miR-181a on EAMG symptoms and inflammatory factors are explored through in vivo experiments. According to a total of 40 EAMG mice that were successfully modeled, all EAMG mice showed symptoms of muscle weakness; their diet was reduced; their weight gain was slow; and even weight loss occurred. In MG patients and EAMG mice, the expression of miR-181a was low and TRIM9 was highly expressed. Bioinformatics website and dual-luciferase report analysis of miR-181a had a targeting relationship with TRIM9, and miR-181a could target the expression of TRIM9. After upregulating miR-181a or interfering with TRIM9, serum miR-181a in EAMG mice was significantly upregulated; TRIM9 was significantly downregulated; its clinical symptoms were reduced; and the expression of inflammatory factors was reduced. The study finally learned that miR-181a can reduce the level of MG inflammatory factors by targeting the expression of TRIM9 and has the effect of improving the symptoms of MG.