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Light-induced deprotonation of molecules is an important process in photochemical reactions. Here, we theoretically investigate the tunneling deprotonation of H 2 + and its asymmetric isotopologues driven by circularly polarized THz laser pulses. The quasi-static picture shows that the field-dressed potential barrier is significantly lowered for the deprotonation channel when the mass asymmetry of the diatomic molecule increases. Our numerical simulations demonstrate that when the mass symmetry breaks, the tunneling deprotonation is significantly enhanced and the proton tunneling becomes the dominant dissociation channel in the THz driving fields. In addition, the simulated nuclear momentum distributions show that the emission of the proton is directed by the effective vector potential for the deprotonation channel and, meanwhile, the angular distribution of the emitting proton is affected by the alignment and rotation of the molecule induced by the rotating field. [ABSTRACT FROM AUTHOR]

We experimentally study two-body Coulomb explosions of CO2, O2, and CH3Cl molecules in intense femtosecond laser pulses. We observe an obvious variation in the ionic angular distribution of the fragments with respect to the kinetic energy releases (KERs). Using a classical model based on ab initio potential energy curves, we find that the dependence of the ionic angular distribution on the KER is relevant to the fact that the accurate potential energy deviates significantly from the value determined by applying the Coulomb interaction approximation at a relatively small internuclear distance of the molecule. We show that the KER-dependent ionic angular distribution provides an effective way to determine the critical internuclear distance at which the Coulomb interaction approximation holds or breaks down without relying on the knowledge of the accurate potential energy curves. [ABSTRACT FROM AUTHOR]

Background: Renal cell carcinoma (RCC) is presently recognized as the most prevalent kidney tumor. However, the role and underlying mechanism of action of the conversion factor-inducible protein (TGFBI), an extracellular matrix protein, in RCC remain poorly understood. Methods: In this study, we employed Western blot, quantitative real-time polymerase chain reaction (qRT-PCR), and immunohistochemistry techniques to assess the expression of TGFBI in RCC tissues or cells. Furthermore, we analyzed the proliferation and migration of RCC cells using CCK8, cloning, scratching, and migration assays. Additionally, we examined apoptosis and cell cycle progression through flow cytometry, analysis. Lastly, we employed gene set enrichment analysis (GSEA) to investigate the biological processes associated with TGFBI, which were subsequently validated. Results: The findings indicate that TGFBI exhibits significantly elevated expression levels in both renal cell carcinoma (RCC) tissues and cells. Furthermore, the knockdown of TGFBI in SiRNA transfected cells resulted in the inhibition of RCC cell proliferation, migration, invasiveness, apoptosis, and alteration of the cell cycle. Additionally, TGFBI was found to impede the epithelial-mesenchymal transition (EMT) process in RCC cells. Bioinformatics analysis suggests that TGFBI may exert its influence on various biological processes in RCC through the tumor immune microenvironment. Moreover, our study demonstrates that TGFBI promotes RCC progression by activating the PI3K/AKT/mTOR/HIF-1α. Conclusions: Our research indicates that TGFBI exhibits high expression in RCC and facilitate RCC progression and metastasis through various molecular mechanisms. Hence, TGFBI has the potential to be a novel therapeutic target for the diagnosis and treatment of RCC in the future. [ABSTRACT FROM AUTHOR]

The momentum distribution of photoelectrons in H2+ molecules subjected to an attosecond pulse is theoretically investigated. To better understand the laser–molecule interaction, we develop an in-line photoelectron holography approach that is analogous to optical holography. This approach is specifically suitable for extracting the amplitude and phase of the forward-scattered electron wave packet in a dissociating molecule with atomic precision. We also extend this approach to imaging the transient scattering cross-section of a molecule dressed by a near infrared laser field. This attosecond photoelectron holography sheds light on structural microscopy of dissociating molecules with high spatial-temporal resolution. [ABSTRACT FROM AUTHOR]

Refraction is a basic beam bending effect at two media's interface. While traditional studies focus on stationary boundaries, moving boundaries or potentials could enable new laws of refractions. Meanwhile, media's discretization plays a pivotal role in refraction owing to Galilean invariance breaking principle in discrete-wave mechanics, making refraction highly moving-speed dependent. Here, by harnessing a synthetic temporal lattice in a fiber-loop circuit, we observe discrete time refraction by a moving gauge-potential barrier. We unveil the selection rules for the potential moving speed, which can only take an integer v = 1 or fractional v = 1/q (odd q) value to guarantee a well-defined refraction. We observe reflectionless/reflective refractions for v = 1 and v = 1/3 speeds, transparent potentials with vanishing refraction/reflection, refraction of dynamic moving potential and refraction for relativistic Zitterbewegung effect. Our findings may feature applications in versatile time control and measurement for optical communications and signal processing. Here, authors construct a moving potential barrier in a synthetic temporal lattice. They unveil the selection rules for choosing potential moving speed as well as the conditions to achieve transparent moving potentials and refraction. [ABSTRACT FROM AUTHOR]

Light–matter interactions are usually described within the electric-dipole approximation, where the magnetic-field component and the spatial variation of the light electric field over the relevant electronic length scales are both ignored. Non-dipole effects in photoionization were revealed to be tiny from the infrared to the soft X-ray domains, and all non-dipole observations reported so far were limited to single-pulse, single-colour measurements. Here we advance attosecond time-resolved spectroscopy into the non-dipole interaction regime. Using a self-referenced attosecond photoelectron interferometry on helium atoms, we resolve the electron subcycle motion along the light propagation direction in the 15 pm range driven by the magnetic component of a near-infrared laser field. Furthermore, we measure a time delay of 15 ± 10 as between the electric-dipole and electric-quadrupole transitions by resolving the asymmetry of the photoelectron forward–backward yields with attosecond resolution. These fundamental findings are supported by ab initio calculations based on the non-dipole time-dependent Schrödinger equation. Using a self-referenced attosecond photoelectron interferometry on helium atoms, the electron subcycle motion along the light propagation direction is observed in the 15 pm range. A time delay of 15 ± 10 as between the electric-dipole and electric-quadrupole transitions is also revealed. [ABSTRACT FROM AUTHOR]

Parity‐time (PT) and anti‐parity‐time (anti‐PT) symmetries have provided important guiding principles in the research of non‐Hermitian physics. However, realizations of anti‐PT symmetry in photonic systems usually rely on optical nonlinearities and indirect‐coupling approaches. Here, they apply the channel interference principle mediated by synthetic gauge‐flux biasing in open‐cavity systems to construct anti‐PT symmetries. It is shown that a specific π‐flux biasing into a looped‐resonator array can force a frequency degeneracy between pairwise Bloch modes therein. By further coupling the array into two external waveguides with tailored positions of ports, the system near the degeneracy point can be described by an anti‐PT‐symmetric Hamiltonian. When a real gauge‐flux detuning is introduced, the system undergoes a spontaneous transition between anti‐PT and anti‐PT‐broken phases, through which the two extreme cases of complete channel‐drop tunneling and complete tunneling suppression can be switched. Finally, by superimposing a PT‐symmetric term onto the anti‐PT‐symmetric Hamiltonian via applying an imaginary gauge‐flux biasing, extreme channel‐drop amplifying effects can be further realized by exciting the "lasing" mode under the critical‐coupling condition. The work bridges the physical connection between synthetic gauge field and anti‐PT symmetry. This paradigm may also find many applications from optical routing, and switching to buffering and amplifying on a chip–scale platform. [ABSTRACT FROM AUTHOR]

Mode selecting plays a vital role in the field of optoelectronics, such as optical communication, signal processing, on-chip light manipulation, mode conversion, and frequency synthesis. In this work, flexible selection and enhancement of the frequency modes in an unidirectional coupled Su–Schrieffer–Heeger (SSH) frequency lattice are obtained with Floquet exceptional points (EPs) and chiral Zener tunneling (ZT). The unidirectional coupled non-Hermitian SSH frequency lattices are synthesized by a double-ring system with complex dynamical modulations. Under an effective direct current (dc) force induced by the phase-mismatching of the modulations, the two Floquet bands of the non-Hermitian frequency lattices are degenerated and the Floquet EPs arise. Therefore, the unidirectional and irreversible frequency mode conversion takes place, which is the chiral ZT. Moreover, through perturbation analysis and numerical simulations, we prove that the frequency modes of the two-band system can be selected and enhanced by a multi-photon resonance dc force. [ABSTRACT FROM AUTHOR]

A novel method is proposed to directly characterize the exciton‐plasmon coupling in a photosensitive nanoparticle‐on‐mirror (NPoM) nanocavity. Under the illumination of UV light, the localized surface plasmon resonance (LSPR) peaks of the nanocavity can be continuously tuned over a wide range (≈65 nm), enabling precise determination of the energy dispersion relationship of plexcitons in the nanocavity. The results indicate that the energy of Rabi splitting can be actively tuned from 65 meV (weak coupling) to 170 meV (strong coupling) by adjusting the LSPR peak of a specific nanocavity (particle size L≈55‐92 nm) to the exciton wavelength (the zero detuning). In addition, the criterion of strong coupling is optimized by introducing single‐particle absorption spectroscopy. The work offers an intuitive method for the strong coupling characterization in nanocavity, paving the way for the real‐time tuning of coupling strength over a wide range (100 meV) from weak to strong coupling regimes. [ABSTRACT FROM AUTHOR]

An ultrafast fiber laser system comprising two coherently combined amplifier channels is reported. Within this system, each channel incorporates a rod-type fiber power amplifier, with individual operations reaching approximately 233 W. The active-locking of these coherently combined channels, followed by compression using gratings, yields an output with a pulse energy of 504 μJ and an average power of 403 W. Exceptional stability is maintained, with a 0.3% root mean square (RMS) deviation and a beam quality factor M2 < 1.2. Notably, precise dispersion management of the front-end seed light effectively compensates for the accumulated high-order dispersion in subsequent amplification stages. This strategic approach results in a significant reduction in the final output pulse duration for the coherently combined laser beam, reducing it from 488 to 260 fs after the gratings compressor, while concurrently enhancing the energy of the primary peak from 65% to 92%. [ABSTRACT FROM AUTHOR]

Dynamic localization (DL) refers to a wavefunction confinement effect of electrons in periodic lattices under an ac electric field driving. Recent studies have transplanted DLs from electronic to photonic systems using periodically curved waveguide lattices, where the ac electric field is mimicked by the waveguide's bending curvature. However, due to the severe limitations of bending losses and poor tunability for highly curved, arbitrarily shaped waveguides, present studies mainly focus on DL under the simplest sinusoidal‐wave driving; its extension to an arbitrary‐wave driving remains challenging. Here, by constructing a synthetic temporal lattice with a coupled fiber‐loop circuit, the limitations of spatially curved waveguides are circumvented and generalized DLs are experimentally demonstrated under arbitrary‐wave driving. First, by applying band‐collapse criteria, the general conditions for the driving field's symmetry to achieve DLs are revealed. Then, two representative even‐function driving fields of square‐ and triangle‐waveforms are chosen, and wave‐packet revivals are observed as signatures of DLs. As a counter‐example, the breakdown of DL is also verified using odd‐function driving field of sawtooth‐waveform. The work reveals the conditions for realizing generalized DLs and experimentally verifies them using synthetic lattice schemes. This paradigm may find potential applications in versatile temporal‐waveform reshaping, pulse manipulations for optical communications, and signal processing. [ABSTRACT FROM AUTHOR]

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]

The electron response of nanoplasmon and nanoplasma in the laser field is greatly important for improving the functionality and efficiency of many potential applications. However, how and under what conditions the nanoplasmon‐nanoplasma transition works remains poorly understood due to radiation damage and charge buildup. Utilizing the combined aerodynamic lens and velocity map imaging spectrometer, this transition mediated by different mechanisms are demonstrated, as verified by the distinct photoelectron momentum distributions from Cu nanoparticles. Initially the polarization‐dependent distributions emphasize the domination of surface emission driven by the plasmonic field. Subsequently the transition starts and the competition of volume‐multiphoton and thermionic emission plays the intermediate state dominating the transition process. Finally, a complete plasma is generated with the leading role of thermionic emission, which is confirmed by first observing the correlated electronic decay in metal nanoparticles. These findings bridge the gap between electron emission in nanoplasmonic and nanoplasma states and identify the mechanism‐specific contributions, which will offer general principles for designing nanostructure and laser fields to control electron excitation and emission in practice. [ABSTRACT FROM AUTHOR]

The laser‐irradiated aerosolized nanostructures with complex geometries offer unique opportunities to steer orientation‐dependent photoion emission for multiple applications of directional ion sources and photocatalysis. The orientation‐dependent photoion emission is characterized by measuring the distribution and probability on differently oriented nanostructures. This unique capability is achieved by introducing momentum‐to‐space orientation discrimination in the single‐shot velocity map imaging technique with the aerodynamic lens. The effect of geometry, polarization, and concentration to control the photoion emission from differently oriented nanostructures is introduced for optimizing the potential applications of photoion emission including directional tunable nanoanode and optical sensors. The mechanism behind controlling the photoion emission is visualized by the variations in the regions of high laser intensity inside the nanostructures responding to the orientation, geometry, and polarization. This work represents an advance in characterizing the photoion emission from the randomly oriented aerosolized nanostructures and facilitates the potential for combining with the pump–probe methods to provide an intuitive understanding of their real‐time ionization dynamics. [ABSTRACT FROM AUTHOR]

Dynamic localization (DL) of photons, i.e., the light-motion cancellation effect arising from lattice's quasi-energy band collapse under a synthetic ac-electric-field, provides a powerful and alternative mechanism to Anderson localization for coherent light confinement. So far only low-order DLs, corresponding to weak ac-fields, have been demonstrated using curved-waveguide lattices where the waveguide's bending curvature plays the role of ac-field as required in original Dunlap-Kenkre model of DL. However, the inevitable bending losses pose a severe limitation for the observation of high-order DL. Here, we break the weak-field limitation by transferring lattice concepts from spatial to synthetic time dimensions using fiber-loop circuits and observe up to fifth-order DL. We find that high-order DLs possess superior localization and robustness against random noise over lower-order ones. As an exciting application, by judiciously combining low- and high-order DLs, we demonstrate a temporal cloaking scheme with flexible tunability both for cloak's window size and opening time. Our work pushes DL towards high-order regimes using synthetic-lattice schemes, which may find potential applications in robust signal transmission, protection, processing, and cloaking. Dynamic localization is a method of confining light. Here the authors demonstrate higher-order dynamic localization of photons in a synthetic temporal mesh lattice and discuss the idea of tunable temporal cloaking by combining different-order localizations. [ABSTRACT FROM AUTHOR]

Dynamically encircling the exceptional point (EP) of an anti‐parity‐time (anti‐PT) symmetric system can achieve chiral mode switching between symmetry‐broken eigenmodes, which is especially important for developing nanophotonic devices. However, the realization of anti‐PT‐symmetric systems on a chip still remains significantly challenging as precisely controlling the parameters of nanophotonic structures is difficult. Herein, a novel anti‐PT‐symmetric system is designed and constructed on a silicon‐on‐insulator chip by taking advantage of subwavelength gratings to help engineer nanophotonic structures. Consequently, on‐chip chiral switching between symmetry‐broken eigenmodes is experimentally realized by dynamically encircling the EP in parametric space of the proposed anti‐PT‐symmetric system. Moreover, the achieved chiral mode switching exhibits high output power ratios (≥ 6.4 dB) at 1550 nm, wide‐band response that covers C‐band completely, and great thermal stability up to 90 °C, which indicate desirable performance features for practical applications in optical communication. This study paves an avenue for realizing on‐chip chiral switching between symmetry‐broken modes, which shows great promise for developing nanophotonic devices, such as optical switching, logic gates, and isolators, in optical telecommunication bands. [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]

Electron migration in molecules is the progenitor of chemical reactions and biological functions after light-matter interaction. Following this ultrafast dynamics, however, has been an enduring endeavor. Here we demonstrate that, by using machine learning algorithm to analyze high-order harmonics generated by two-color laser pulses, we are able to retrieve the complex amplitudes and phases of harmonics of single fixed-in-space molecules. These complex dipoles enable us to construct movies of laser-driven electron migration after tunnel ionization of N2 and CO2 molecules at time steps of 50 attoseconds. Moreover, the angular dependence of the migration dynamics is fully resolved. By examining the movies, we observe that electron holes do not just migrate along the laser polarization direction, but may swirl around the atom centers. Our result establishes a general scheme for studying ultrafast electron dynamics in molecules, paving a way for further advance in tracing and controlling photochemical reactions by femtosecond lasers. Seeing molecules in action under the influence of very short pulses is interesting. Here the authors demonstrate charge migration dynamics in molecules by using high harmonic spectroscopy and machine learning algorithm. [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]

We demonstrate a double Rabi splitting totaling 348 meV in an Ag nanocavity embedding of methylene blue (MB) dye layer, which is ascribed to the equilibrium state of monomer and dimer coexistence in MB dye. At low dye concentration, the single-mode strong coupling between the monomer exciton in MB dye and the Ag nanocavity is observed. As the dye concentration is increased, three hybridized plexciton states are observed, indicating a double Rabi splitting (178 and 170 meV). Furthermore, the double anti-crossing behavior of the three hybrid states is observed by tuning the Ag nanocube size, which validates the multi-mode strong coupling regime. It shows clear evidence on the diverse exciton forms of dye molecules, both of which can interact with plasmonic nanocavity, effectively. Therefore, it provides a good candidate for realizing the multi-mode strong coupling. [ABSTRACT FROM AUTHOR]

We demonstrate a double Rabi splitting totaling 348 meV in an Ag nanocavity embedding of methylene blue (MB) dye layer, which is ascribed to the equilibrium state of monomer and dimer coexistence in MB dye. At low dye concentration, the single-mode strong coupling between the monomer exciton in MB dye and the Ag nanocavity is observed. As the dye concentration is increased, three hybridized plexciton states are observed, indicating a double Rabi splitting (178 and 170 meV). Furthermore, the double anti-crossing behavior of the three hybrid states is observed by tuning the Ag nanocube size, which validates the multi-mode strong coupling regime. It shows clear evidence on the diverse exciton forms of dye molecules, both of which can interact with plasmonic nanocavity, effectively. Therefore, it provides a good candidate for realizing the multi-mode strong coupling. [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]

Interferometry, a key technique in modern precision measurements, has been used for length measurement in engineering metrology and astronomy. An analogous time-domain interferometric technique would represent a significant complement to spatial domain applications and require the manipulation of interference on extreme time and energy scales. Here, we report an all-optical interferometer using laser-driven high order harmonics as attosecond temporal slits. By controlling the phase of the temporal slits with an external field, a time domain interferometer that preserves both attosecond temporal resolution and hundreds of meV energy resolution is implemented. We apply this exceptional temporal resolution to reconstruct the waveform of an arbitrarily polarized optical pulse, and utilize the provided energy resolution to interrogate the abnormal character of the transition dipole near the Cooper minimum in argon. This novel attosecond interferometry paves the way for high precision measurements in the time-energy domain using all-optical approaches. [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]

The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields. Up to now, to directly image the onset of Jahn-Teller symmetry breaking remains unreached. Here we employ ultrafast ion-coincidence Coulomb explosion imaging with sub-10 fs resolution and unambiguously image the ultrafast dynamics of Jahn-Teller deformations of CH 4 + cation in symmetry space. It is unraveled that the Jahn-Teller deformation from C3v to C2v geometries takes a characteristic time of 20 ± 7 fs for this system. Classical and quantum molecular dynamics simulations agree well with the measurement, and reveal dynamics for the build-up of the C2v structure involving complex revival process of multiple vibrational pathways of the CH 4 + cation. The Jahn-Teller effect is the spontaneous symmetry breaking of the molecular structure caused by the coupling of electrons and nuclei. Here the authors use ultrafast Coulomb explosion imaging to map the evolution of the fundamental symmetry lowering process in photoionized methane within around 20fs. [ABSTRACT FROM AUTHOR]

Nonlinear metasurfaces provide a promising platform for integrated nonlinear photonic devices owing to their unprecedented capability of nonlinear wavefront manipulation. However, the previously reported second‐harmonic (SH) metasurfaces are mainly based on the nonlinear Pancharatnam–Berry phase modulation. While this method is quite convenient and robust, it shows limitations of modulation efficiency and the difficulty in extending to multidimensional combined modulations. Here, the resonant nonlinear synthetic metasurface is proposed and experimentally demonstrated for independent phase and amplitude modulations of the SH beam. A high SH modulation efficiency of 75% (with a theoretical limit of 90%) is achieved in the polarization‐dependent SH metalens. Moreover, SH holographic imaging with phase and amplitude (at 2 and 4 levels) combined modulation is realized experimentally. Compared with the pure‐phase modulation, the signal‐to‐noise ratios are increased by 2 and 3 times when 2‐ and 4‐level amplitude controls are introduced. This is not only an important step in the improvement and innovation of holographic display technology, but also paves a distinct avenue toward multifunctional, higher efficiency, and ultracompact nonlinear optical devices. [ABSTRACT FROM AUTHOR]

Strong-field tunneling ionization is the first step for a broad class of phenomena in intense laser-atom/molecule interactions. Accurate information about the electron wave packet from strong-field tunneling ionization of atoms and molecules is of essential importance for understanding various tunneling ionization triggered processes. Here, we survey the property of the electron wave packet in tunneling ionization of molecules with a method based on strong-field photoelectron holography. By solving the time-dependent Schrödinger equation, it is shown that the holographic interference in the photoelectron momentum distribution exhibits the asymmetric behavior with respect to the laser polarization direction, when the molecule is aligned with a nonzero angle to the linearly polarized laser field. We demonstrate that this asymmetry is due to the nonzero initial transverse displacement of the electron wave packet at tunneling. By analyzing the holographic interference, this transverse displacement for the launching of electron wave packet tunneling from the molecules is accurately retrieved. This displacement is directly related to the electron density distribution in molecules, and thus our work developed a novel concept for probing electronic structure in molecules. [ABSTRACT FROM AUTHOR]

We use an interferometic scheme to extract the phase distribution of the electron wave packet from above-threshold ionization in elliptically polarized laser fields. In this scheme, an electron wave packet released from a circularly polarized laser pulse acts as a reference wave and interferes with the electron wave packet ionized by a time-delayed counter-rotating elliptically polarized laser field. The generated vortex-shaped interference pattern in the photoelectron momentum distribution enables us to extract the phase distribution of the electron wave packet in the elliptically polarized laser pulse with high precision. By artificially screening the ionic potential at different ranges when solving the time-dependent Schördinger equation, we find that the angle-dependent phase distribution of the electron wave packet in the elliptically polarized laser field shows an obvious angular shift as compared to the strong-field approximation, whose value is the same as the attoclock shift. We also show that the amplitude of the angle-dependent phase distribution is sensitive to the ellipticity of the laser pulse, providing an alternative way to precisely calibrate the laser ellipticity in the attoclock measurement. [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]

We report an experimental measurement of nonlinear absorption by using the near-infrared femtosecond laser and a crystalline MgO sample. We show that the nonlinear absorption inside MgO presents a four-fold modulation as a function of the crystal alignment to the laser polarization. In different intensities and wavelengths, we observe that the modulation amplitude is changed. We introduce a model based on the calculation of the carrier density to explain the phenomenon. It shows that the varied modulation is due to the variation of effective electron mass, which is related to the crystal structure. Our work makes a step forward in the application of nonlinear absorption in exploring solid structure. [ABSTRACT FROM AUTHOR]

An inline fiber sensor for simultaneous measurement of curvature and temperature based on anti-resonant (AR) effect combined with multimode interference (MMI) is proposed and experimentally demonstrated. The sensing structure is simply formed by embedding a section of multimode fiber (MMF) and glass capillary between single-mode fibers (SMF). Thence the multimode interference (MMI) pattern with dips and the AR effect spectrum with the loss valleys at the resonance wavelengths can be observed on the optical spectrum analyzer (OSA). A curvature sensitivity of −9.25 dB/ $\text{m}^{-1}$ with almost unchanged wavelength can be achieved by intensity demodulation at an AR valley. And a temperature sensitivity of 30 pm/°C with a tiny intensity sensitivity −0.079 dB/°C is obtained by wavelength demodulation at a MMI dip. Different demodulation mechanisms enable our sensors to discriminate curvature and temperature. Moreover, the advantages such as repeatability of fabrication, robust structure and cost-effectiveness, further benefit its practical sensing applications. [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 investigate the topological edge modes in a rhombic waveguide array with imaginary coupling, which is realized by incorporating auxiliary waveguide between the coupled waveguides. By suitably tuning both real and imaginary couplings to generate an effective π flux, a non-Hermitian analog of Aharonov-Bohm (AB) cage is formed as the band structures become flat and coalesce into third-order exceptional points (EPs). We show the array can support gapped topological edge modes, which can be explained by mapping the system Hamiltonian into the square root of an anti-parity-time (PT) -symmetric waveguide array. In contrast to the linear power increase of bulk modes, the propagation of edge modes can be conserved or exponentially amplified depending on which termination is initially excited. Our study provides a promising way to realizing robust light propagation. [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]

We investigate the excitation of surface plasmon polaritons (SPPs) using a metallic nanoaperture array illuminated by circularly polarized Laguerre-Gaussian (LG) vortex beams. The direction of SPP excitation is tunable by changing the circular polarization and topological charge of LG beams. The left- or right-handed circular polarization determines SPP propagation on either side of the nanoaperture array. Furthermore, varying the topological charge of LG beam will result in beam splitting of SPPs. We also utilize a composite nanoaperture array with different periods to achieve unidirectional excitation of SPPs. The study provides an interesting approach to control the excitation direction of SPPs and may find great applications in SPP generators and optical switches. [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]

A method to produce circularly polarized attosecond pulses with tunable helicity from CO molecule by using an unidirectionally rotating laser field is proposed. It is found that broadband harmonic supercontinuum with circular polarization can be generated from the oriented CO molecule. This enables the production sub‐100 attosecond isolated pulse with the ellipticity as high as 0.9 at the macroscopic level. Moreover, the helicity of the generated high‐order harmonics and the attosecond pulse can be tuned by adjusting the orientation of the CO molecule. This method will be beneficial for the studies on chiral‐specific dynamics and magnetic circular dichroism on an attosecond time scale. [ABSTRACT FROM AUTHOR]

We study the temporal imaging with a gradient-index (GRIN) time lens in which both dispersion and time-varying quadratic phase modulation are introduced. The lens is built by using cross-phase modulation between a signal and a parabolic pump pulse in the nonlinear optical fiber with group velocity dispersion. A general theoretical analysis of temporal imaging by the GRIN time lens is performed in detail. Compared to thin lens in previous studies, the introduction of dispersion, benefits periodic self-imaging of both time waveform and frequency spectrum for optical pulses. Interestingly, the temporal and spectral profiles of the input can be exchanged with each other periodically in the GRIN time lens. By combining the GRIN time lens with dispersive elements on both sides, the temporal waveforms of incident optical pulses can be stretched and compressed. For an input signal composed of multiple pulses experiencing different dispersions, the temporal depth imaging of the signal is realized by scanning the timing of the pump pulse applied on the lens. The study may find great applications in ultrafast optical signal processing and measurement. [ABSTRACT FROM AUTHOR]

2D organic–inorganic hybrid perovskites are promising materials for next‐generation optoelectronic devices. Nevertheless, 2D perovskites still suffer from performance‐limiting trap states and possess fundamental photophysical effects that remain poorly understood. Herein, a photoinduced trap passivation for enhanced photoluminescence (PL) in 2D hybrid perovskites is reported. Under two‐photon excitation, the PL emission of the 2D hybrid perovskites exhibits a gradual increase in intensity and lifetime, due to the photoinduced trap passivation by interacting with oxygen in ambient environment. Interestingly, the PL increase shows distinct features at the surface and in the bulk of the 2D perovskites, which can be well revealed by a photoinduced oxygen‐diffused trap‐passivation model. Moreover, the PL increase and relaxation can recycle for several times, which suggests an excellent repeatability of the photoinduced trap passivation. The photoinduced trap passivation is critical for fundamental study of light–matter interaction in 2D perovskites, and shows great promise for improving the optoelectronic responses for functional devices. [ABSTRACT FROM AUTHOR]