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Toroidal vortex is a kind of novel and exotic structured light with potential applications in photonic topology and quantum information. Here, we present the study on high harmonic generation (HHG) from the interaction of the intense toroidal vortices with atoms. We show that the spatial distribution of harmonic spectra reveal unique structures, which are kinds of high-order topological toroidal vortex because of the rotating of the driving fields with transverse orbital angular momentum. Then we show that, by synthesizing the toroidal vortices and optical vortices with longitudinal orbital angular momentum, it is able to generate the optical hopfions in extreme ultraviolet (EUV) range, which exhibit completely different topological property compared with both the driving fields. Harnessing the spin angular momentum selection rules, we further show that one can control the topological texture and channel each harmonic into a single mode of controllable Hopf invariant.

High harmonic generation (HHG) with longitudinal optical orbital angular momentum has attracted much attention over the past decade. Here, we present the first study on the HHG with transverse orbital angular momentum driven by the spatiotemporal optical vortex (STOV) pulses. We show that the produced spatial resolved harmonic spectra reveal unique structures, such as the spatially spectral tilt and the fine interference patterns. We show these spatio-spectral structures originate from both the macroscopic and microscopic effect of spatiotemporal optical singularity in HHG. Employing two-color counter-spin and counter-vorticity STOV pulses, we further discuss a robust method to control the spatiotemporal topological charge and spectral structure of high-order harmonics. The conservation rule of photon transverse orbital angular momentum in HHG process is also discussed when mixing with photon spin angular momenta., Comment: 15 pages, 5 figures

Optical skyrmion serves as a crucial interface between optics and topology. Recently, it has attracted great interest in linear optics. Here, we theoretically introduce a framework for the all-optical generation and control of freespace optical skyrmions in extreme ultraviolet regions via high harmonic generation. We show that by employing full Poincare beams, the created extreme ultraviolet fields manifest as skyrmionic structures in Stokes vector fields, whose skyrmion number is relevant to harmonic orders. We reveal that the generation of skyrmionics structure is attributed to spatial-resolved spin constraint of high harmonic generation. Through qualifying the geometrical parameters of full Poincar\'e beams, the topological texture of extreme ultraviolet fields can be completely manipulated, generating the Bloch-type, Neel-type, anti-type, and higher-order skyrmions, etc. This work promotes the investigation of topological optics in optical highly nonlinear processes, with potential applications towards ultrafast spintronics with structured light fields., Comment: 17 Pages, 4 figures

The interaction between a quantum particle's spin angular momentum and its orbital angular momentum is ubiquitous in nature. In optics, the spin-orbit optical phenomenon is closely related with the light-matter interaction and has been of great interest. With the development of laser technology, the high-power and ultrafast light sources now serve as a crucial tool in revealing the behaviour of matters under extreme conditions. The comprehensive knowledge of the spin-orbit interaction for the intense light is of utmost importance. Here, we achieve the in-situ modulation and visualization of the optical orbital-to-spin conversion in strong-field regime. We show that, through manipulating the morphology of femtosecond cylindrical vector vortex pulses by a slit, the photons' orbital angular momentum can be controllably transformed into spin after focusing. By employing strong-field ionization experiment, the orbital-to-spin conversion can be imaged and measured through the photoelectron momentum distributions. Such detection and consequent control of spin-orbit dynamics of intense laser fields have implications on controlling the photoelectron holography and coherent extreme ultraviolet radiation., Comment: 28 pages, 4 figures

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 +1 and -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., Comment: 10 pages, 7 figures

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.

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.

Nondipole effects are ubiquitous and crucial in light-matter interaction. However, they are too weak to be directly observed. In strong-field physics, motion of electrons is mainly confined in transverse plane of light fields, which suppresses the significance of nondipole effects. Here, we present a theoretical study on enhancing and controlling the nondipole effect by using the synthesized two perpendicularly propagating laser fields. We calculate the three-dimensional photoelectron momentum distributions of strong-field tunneling ionization of hydrogen atoms using the classical trajectory Monte Carlo model and show that the nondipole effects are noticeably enhanced in such laser fields due to their remarkable influences on the sub-cycle photoelectron dynamics. In particular, we reveal that the magnitudes of the magnetic and electric components of nondipole effects can be separately controlled by modulating the ellipticity and amplitude of driving laser fields. This novel scenario holds promising applications for future studies with ultrafast structured light fields., Comment: 14 pages, 4 figures, 49 references

Structured light has attracted great interest in scientific and technical fields. Here, we demonstrate the first generation of structured air lasing in N2+ driven by 800 nm femtosecond laser pulses. By focusing a vortex pump beam at 800 nm in N2 gas, we generate a vortex superfluorescent radiation of N2+ at 391 nm, which carries the same photon orbital angular momentum as the pump beam. With the injection of a Gaussian seed beam at 391 nm, the coherent radiation is amplified, but the vorticity is unchanged. A new physical mechanism is revealed in the vortex N2+ superfluorescent radiation: the vortex pump beam transfers the spatial spiral phase into the N2+ gain medium, and the Gaussian seed beam picks up the spatial spiral phase and is then amplified into a vortex beam. Moreover, when we employ a pump beam with a cylindrical vector mode, the Gaussian seed beam is correspondingly amplified into a cylindrical vector beam. Surprisingly, the spatial polarization state of the amplified radiation is identical to that of the vector pump beam regardless of whether the Gaussian seed beam is linearly, elliptically, or circularly polarized. Solving three-dimensional coupled wave equations, we show how a Gaussian beam becomes a cylindrical vector beam in a cylindrically symmetric gain medium. This study provides a novel approach to generating structured light via N2+ air lasing., Comment: 18 pages, 5 figures, 3 equations

Spatiotemporal sculpturing of light pulse with ultimately sophisticated structures represents the holy grail of the human everlasting pursue of ultrafast information transmission and processing as well as ultra-intense energy concentration and extraction. It also holds the key to unlock new extraordinary fundamental physical effects. Traditionally, spatiotemporal light pulses are always treated as spatiotemporally separable wave packet as solution of the Maxwell's equations. In the past decade, however, more generalized forms of spatiotemporally nonseparable solution started to emerge with growing importance for their striking physical effects. This roadmap intends to highlight the recent advances in the creation and control of increasingly complex spatiotemporally sculptured pulses, from spatiotemporally separable to complex nonseparable states, with diverse geometric and topological structures, presenting a bird's eye viewpoint on the zoology of spatiotemporal light fields and the outlook of future trends and open challenges., Comment: This is the version of the article before peer review or editing, as submitted by an author to Journal of Optics. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it

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 equipped molecular imaging with femtosecond time resolution. This Perspectives present an overview of 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.

We experimentally demonstrate spatiotemporal steering of photoelectron emission in multiphoton above-threshold single ionization of atoms exposed to a phase-controlled orthogonally polarized two-color (OTC) laser pulse. Spatial and energy resolved photoelectron angular distributions are measured as a function of the laser phase, allowing us to look into the fine structures and emission dynamics. The slow and fast photoelectrons, distinguished by the energy larger or smaller than 2Up with Up being the ponderomotive energy of a free electron in the laser field, have distinct spatiotemporal dependences of the laser waveform. The phase-of-phase of the slow electron oscillates as functions of both the energy and emission direction, however, the fast electron present rather flat phase structure which merely depends on its emission direction. Three-dimensional generalized quantum trajectory Monte Carlo simulations are performed to explore the sub-cycle dynamics of the electron emission in the phase-controlled OTC pulse., Comment: This paper has been withdrawn by the author due to a new analysis

We investigate electron momentum distributions from single ionization of Ar by two orthogonally polarized laser pulses of different color. The two-color scheme is used to experimentally control the interference between electron wave packets released at different times within one laser cycle. This intracycle interference pattern is typically hard to resolve in an experiment. With the two-color control scheme these features become the dominant contribution to the electron momentum distribution. Furthermore the second color can be used for streaking of the otherwise interfering wave packets establishing a which-way marker. Our investigation shows that the visibility of the interference fringes depends on the degree of the which-way information determined by the controllable phase between the two pulses., Comment: submitted to PRL