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We theoretically investigate nonadiabatic effects in tunneling ionization of a hydrogen atom induced by a few-cycle elliptically polarized laser pulse. We find a deflection angle between the maximum of the photoelectron momentum distribution and the direction of the negative vector potential corresponding to the electric-field peak. This deflection angle mainly originates from the fact that the instant of the maximal ionization rate does not exactly correspond to the instant of the electric-field peak in the few-cycle elliptically polarized laser pulse, revealing an ionization time shift between those two instants. The ionization time shift is a result of the nonadiabatic effect induced by the envelope of the few-cycle elliptically polarized laser pulse, which disappears in a long-pulsed laser. Our study is useful for understanding attoclock experiments using few-cycle elliptically polarized laser pulses. [ABSTRACT FROM AUTHOR]

We report an unexplored observation of multi-orbital contribution in the below- and near-threshold harmonic generation of aligned molecules. A typical pump–probe configuration is used in our experiments. By scanning the time delay and crossing angle of polarization directions between the pump and probe pulses, we find that the harmonic yield in this region exhibits abnormal intensity-dependent modulation patterns. Further comparison and analysis show that this observation can be interpreted as due to the contribution of deeper-lying molecular orbitals, which are much more prominent than in the above-threshold region and can overall surpass the contribution of the highest occupied molecular orbital, leading to reversed modulation patterns. The particular importance of the deeper-lying orbitals in this regime is closely related to the multi-photon excitation pathways involved in the generation process. Our work will advance further investigations on the mechanism of below- and near-threshold harmonic generation. [ABSTRACT FROM AUTHOR]

Transition metal dichalcogenides (TMD) have attracted considerable attention in the field of photonic integrated circuits due to their giant optical anisotropy. However, on account of their inherent loss in the visible region and the difficulty of measuring high refractive index materials, near-field characterizations of the optical anisotropy of TMD in the visible region have inherent experimental difficulties. In this work, we present a systematical characterization of the optical anisotropy in tungsten disulfide (WS2) flakes by using scattering-type scanning near-field optical microscopy (s -SNOM) excited at 671 nm. Transverse-electric and transverse-magnetic (TM) waveguide modes can be excited in WS2 flakes with suitable thickness, respectively. With the assistance of the Au substrate, the contrast of the near-field fringes is enhanced in comparison with the SiO2 substrate. By combining waveguide mode near-field imaging and theoretical calculations, the in-plane and out-of-plane refractive indexes of WS2 are determined to be 4.96 and 3.01, respectively, indicating a high birefringence value up to 1.95. This work offers experimental evidence for the potential application of WS2 in optoelectronic integrated circuits in the visible region. [ABSTRACT FROM AUTHOR]

The sensitivity of strong-field ionization to atomic orbital helicity has attracted much attention from physicists, due to its potential application in attosecond spectroscopy and spintronics. In order to intuitively observe the physical mechanisms of helicity-dependent ionization rates during photoionization, the concept of the Wigner phase can be used to characterize the different interactions between the rotating electrons and the Coulomb potential. Here, we find that in both one- and three-photon ionization schemes, the electrons liberated more easily by the circularly polarized laser field suffer less influence of the Coulomb potential during the propagation and then accumulate less Winger phase. This result indicates that the strength of the interaction between the rotating electrons and the Coulomb potential can explain the helicity-dependent ionization for different ionization mechanisms universally, which is also supported by our classical ensemble analysis. Our work provides an intuitive perspective towards the physics picture of ionization propensity rules. [ABSTRACT FROM AUTHOR]

We propose a quantitative polarization-resolved quantum trajectory approach to analyse the solid high-order harmonic generation (HHG). By using this approach, we can distinguish the ionization channels of different polarization components in HHG. We take the HHG in hBN under two counter-rotating circularly polarized fields as an example. We find that the right and left circular polarized high harmonics are contributed by the electron trajectories with the ionization channel around the high symmetry points K and K ′ respectively. Furthermore, the intensity of the right and left circular polarization harmonics is determined by the interference between these electron trajectories. Our work offers a quantitatively polarization-resolved analysis to understand the underlying mechanism in HHG in the view of electron reciprocal space trajectory. [ABSTRACT FROM AUTHOR]

Coherent superposition of electronic states induces attosecond electron motion in molecules. We theoretically investigate the strong-field ionization of this superposition state by numerically solving the time-dependent Schrödinger equation. In the obtained photoelectron momentum distribution, an intriguing bifurcation structure appears in the strong-field holographic interference pattern. We demonstrate that this bifurcation structure directly provides complete information about the status of the transient wave function of the superposition state: the horizontal location of the bifurcation in the momentum distribution reveals the relative phase of the involved components of the superposition state and the vertical position indicates the relative coefficient. Thus, this bifurcation structure takes a snapshot of the transient electron wave packet of the superposition state and provides an intuitive way to monitor electron motion in molecules. [ABSTRACT FROM AUTHOR]

Charge migration during light–matter interaction is one of the most fundamental processes which plays a key role in chemical and biological processes of molecule. The measurement of this process requires the extreme temporal and subatomic spatial resolutions. Here, we show that a scheme based on infrared pump and short extreme ultraviolet probe technique enables us to trace the laser-controlled electron motion with high spatiotemporal resolution. By numerically solving the time-dependent Schrödinger equation for combined with a simple double-slit model, we demonstrate that the laser-controlled charge migration can be directly reconstructed from the interference patterns of the photoelectron spectrum. [ABSTRACT FROM AUTHOR]

We theoretically investigate the high-order harmonic generation (HHG) driven by dual-pulse lasers. The first pulse of 800 nm can create plasma in the high-density gas target. Then, the second pulse of 1800 nm is spatiotemporally reshaped by the plasma and generates soft x-ray high-order harmonics in the overdriven regime. The simulation results show that adding the first pulse can promote the phase matching of HHG in the cutoff region. As a result, a cutoff-extended HHG is achieved, which is one order of magnitude more intense than that in one pulse scheme reported previously. In dual-pulse driving lasers, the harmonic yield and the cutoff photon energy can be optimized effectively by increasing the gas pressure inside the water window region. [ABSTRACT FROM AUTHOR]

The high-resolution three-dimensional photoelectron momentum distributions via above-threshold ionization (ATI) of Xe atoms are measured in an intense near circularly polarized laser field using velocity map imaging and tomography reconstruction. Compared to the linearly polarized laser field, the employed near circularly polarized laser field imposes a more strict selection rule for the transition via resonant excitation, and therefore we can selectively enhance the resonant ATI through certain atomic Rydberg states. Our results show the self-reference ionization delay, which is determined from the difference between the measured streaking angles for nonadiabatic ATI via the 4f and 5f Rydberg states, is 45.6 as. Our method provides an accessible route to highlight the role of resonant transition between selected states, which will pave the way for fully understanding the ionization dynamics toward manipulating electron motion as well as reaction in an ultrafast time scale. [ABSTRACT FROM AUTHOR]

We discuss the non-dipole effect in high-order harmonic generation from atoms driving by a linearly polarized vortex beam. Different from the selection rule under the dipole approximation, where only odd high harmonics are allowed, both even and odd harmonics are generated in the vortex beam. Moreover, the polarization states of the harmonics are modulated. Elliptically polarized high harmonics can be directly generated with a linearly polarized vortex beam. We show that these non-dipole effects arise from the orbital angular momentum and spin angular momentum of the vortex beam. [ABSTRACT FROM AUTHOR]

2D organic-inorganic lead iodide perovskites hold great promise for functional optoelectronic devices. However, their performances have been seriously limited by poor long-term stability in ambient environment. Here, we perform a systematic study for the stability improvement of a typical 2D organic-inorganic lead iodide perovskite (PEA)2PbI4. The degradation of the (PEA)2PbI4 films can be attributed to the interaction with the humidity in environment, which leads to decomposition of the perovskite components. Then, we demonstrate that polymer passivation provides an effective approach for improving the crystal quality and stability of the (PEA)2PbI4 films. Correspondingly, the photoemission of the polymer-passivated (PEA)2PbI4 films has been enhanced due to the decreased trap states. More importantly, a hydrophobic polymer (Poly(4-Vinylpyridine), PVP) will protect the (PEA)2PbI4 films from humidity in ambient environment, which can greatly improve the physical and chemical stability of the 2D perovskite films. As a result, the PVP-passivated (PEA)2PbI4 films can produce a bright emission even after long-term (>15 d) exposure to ambient environment (25 °C, 80% RH) and continuous UV illumination. This work provides a convenient and effective approach for improving the long-term stability of 2D organic-inorganic lead iodide perovskites, which shows great promise for fabricating large-area and versatile optoelectronic devices. [ABSTRACT FROM AUTHOR]

By numerically solving the three-dimensional time-dependent Schrödinger equation, we theoretically investigate the dynamic interference of the hydrogen atom in intense arbitrarily polarized high-frequency XUV pulses with and without the non-dipole correction included. Our results show a clear shift of the dynamic-interference peaks in the photoelectron spectra from the linearly and circularly polarized XUV pulses, which can be attributed to the different AC Stark shifts of the ground state. The non-dipole correction for the electron–light interaction produces a similar peak shift along the propagation direction in the photoelectron momentum spectra for the linear and circular pulses. But no obvious non-dipole effect for the AC Stark shift of the ground state is identified for the light pulse with intensity around 1019 W cm−2. [ABSTRACT FROM AUTHOR]

Debris mitigation using an ambient gas is the easiest way for laser-produced plasma extreme ultraviolet light source. The debris mitigation power of hydrogen, helium and argon buffer gases against CO2 laser produced tin plasma plumes was quantitatively estimated by means of the visualization imaging system as well as the optical emission spectroscopy technique. The debris mitigation power of hydrogen buffer gas was assessed under ambient pressure ranging from 30 to 104 Pa. The debris mitigation power of the hydrogen buffer gas was determined as 150 eV mm−1 for energetic particles of 400 eV under a pressure of 104 Pa, which remained as high as 40 eV mm−1 at a pressure of 100 Pa. The maximum stopping power and collision scattering cross section of argon were measured to be almost three times larger in comparison with hydrogen and one and a half times larger than helium atmosphere at a pressure of 2000 Pa. Time-resolved optical emission spectroscopy showed that thermalizing collisions were responsible for slowing down the fast energetic ions and atoms towards a thermal equilibrium. [ABSTRACT FROM AUTHOR]