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Enlarging bandwidth capacity of the integrated photonic systems demands efficient and broadband light coupling among optical elements, which has been a vital issue in integrated photonics. Here, we have developed a compact ultra-broadband light coupling strategy based on nonadiabatic pumping in coupled optical waveguides, and experimentally demonstrated the designs in thin-film lithium niobate on insulator (LNOI) platform. We found that nonadiabatic transition would produce a decreased dispersion of the phases related to eigenstates in the waveguides. As a consequence, we realized high-efficiency directional transfer between edgestates for various wavelengths covering a 1-dB bandwidth of ~320 nm in experiment (>400 nm in simulation), with a coupling length (~50 {\mu}m) approximately 1/10 of that required in the adiabatic regime. Furthermore, we have constructed complex functional devices including beamsplitter and multiple-level cascaded networks for broadband light routing and splitting. Our work preserves significant advantages simultaneously in extending the operation bandwidth and minimizing the footprint, which demonstrates great potential for large-scale and compact photonic integration on chip.

We have demonstrated the capability of spectral multiplexing in multi-distance diffractive imaging, enabling the reconstruction of samples with diverse spectral responses. While previous methods like ptychography utilize redundancy in radial diffraction data to achieve information multiplexing, they typically require capturing a substantial amount of diffraction data. In contrast, our approach effectively harnesses the redundancy information in axial diffraction data. This significantly reduces the amount of diffraction data required and relaxes the stringent requirements on optical path stability., Comment: 4 pages, 5 figures

High-energy, few-cycle laser pulses are essential for numerous applications in the fields of ultrafast optics and strong-field physics, due to their ultrafast temporal resolution and high peak intensity. In this work, different from the traditional hollow-core fibers and multiple thin solid plates, we represent the first demonstration of the octave-spanning supercontinuum broadening by utilizing multiple ultrathin liquid films (MTLFs) as the nonlinear media. The continuum covers a range from 380 to 1050 nm, corresponding to a Fourier transform limit pulse width of 2.5 fs, when 35 fs Ti:sapphire laser pulse is applied on the MTLFs. The output pulses are compressed to 3.9 fs by employing chirped mirrors. Furthermore, a continuous high-order harmonic spectrum up to the 33rd order is realized by subjecting the compressed laser pulses to interact with Kr gas. The utilization of flowing water films eliminates permanent optical damage and enables wider and stronger spectrum broadening. Therefore, this MTLFs scheme provides new solutions for the generation of highly efficient femtosecond supercontinuum and nonlinear pulse compression, with potential applications in the fields of strong-field physics and attosecond science., Comment: 9 pages, 5 figures

High harmonic generation (HHG) from gas phase atoms (or molecules) has opened up a new frontier in ultrafast optics, where attosecond time resolution and Angstrom spatial resolution are accessible. The fundamental physical pictures of HHG are always explained by the laser-induced recollision of particle-like electron motion, which lay the foundation of attosecond spectroscopy. In recent years, HHG has also been observed in solids. One can expect the extension of attosecond spectroscopy to the condensed matter if a description capable of resolving ultrafast dynamics is provided. Thus, a large number of theoretical studies have been proposed to understand the underlying physics of HHG. Here, we revisit the recollision picture in solid HHG and show some challenges of current methods with particle perspective, and present the recently developed wave perspective Huygens-Fresnel picture in understanding dynamical systems within the ambit of strong-field physics.

Characterizing an isolated attosecond pulse (IAP) is essential for its potential applications. A complete characterization of an IAP ultimately requires the determination of its electric field in both time and space domains. However, previous methods, like the widely-used RABBITT and attosecond streaking, only measure the temporal profile of the attosecond pulse. Here we demonstrate an all-optical method for the measurement of the space-time properties of an IAP. By introducing a non-collinear perturbing pulse to the driving field, the process of IAP generation is modified both spatially and temporally, manifesting as a spatial and a frequency modulation in the harmonic spectrum. By using a FROG-like retrieval method, the spatio-spectral phases of the harmonic spectrum are faithfully extracted from the induced spatio-spectral modulations, which allows a thoroughgoing characterization of the IAP in both time and space. With this method, the spatio-temporal structures of the IAP generated in a two-color driving field in both the near- and far-field are fully reconstructed, from which a weak spatio-temporal coupling in the IAP generation is revealed. Our approach overcomes the limitation in the temporal measurement in conventional in situ scheme, providing a reliable and holistic metrology for IAP characterization., Comment: 18 pages, 5 figures

The double-slit interference in single-photon ionization of the diatomic molecular ion $\mathrm{H}_2^+$ is theoretically studied beyond the dipole approximation. Via simulating and comparing the interactions of the prealigned $\mathrm{H}_2^+$ and the hydrogen atom with the xuv pulses propagating in different directions, we illustrate two kinds of effects that are encoded in the interference patterns of the photoelectrons from $\mathrm{H}_2^+$: (i) the photon-momentum transfer and (ii) the finite speed of light. While both effects could modify the maxima of the interference fringes, we show that the former one hardly affects the interference minima. Our results and analysis show that the interference minima rule out the influences of the photon-momentum transfer and, potentially, the multielectron effect, thus performing a better role in decoding the zeptosecond time delay for the pulse hitting one and the other atomic centers of the molecule.

We experimentally explore the fingerprint of the microscopic electron dynamics in second-order harmonic generation (SHG). It is shown that the interbond electron hopping induces a novel source of nonlinear polarization and plays an important role even when the driving laser intensity is 2 orders of magnitude lower than the characteristic atomic field. Our model predicts anomalous anisotropic structures of the SHG yield contributed by the interbond electron hopping, which is identified in our experiments with ZnO crystals. Moreover, a generalized second-order susceptibility with an explicit form is proposed, which provides a unified description in both the weak and strong field regimes. Our work reveals the nonlinear responses of materials at the electron scale and extends the nonlinear optics to a previously unexplored regime, where the nonlinearity related to the interbond electron hopping becomes dominant. It paves the way for realizing controllable nonlinearity on an ultrafast time scale.

In strong laser fields, the electron density in solids can show up tidal motions caused by the laser ``pulling'' on the electrons, which forms an electron density tide (EDT). However, the strong field processes in solids are always explained by the single-active-electron (SAE) model and the fluctuation of background electrons is neglected previously. Here, we demonstrate the strong field induced EDT effect and propose a model for revealing its role in high harmoinc generation (HHG) from solids. We show that the EDT effect induces an additional polarization current beyond the SAE approximation. It gives a new mechanism for HHG and leads to new anisotropic structures, which are experimentally observed with MgO. Our experiment indicates that the EDT effect becomes more obvious with increasing the laser intensity. Our work establishes the bridge between the HHG and the microscopic EDT in solids induced by the strong laser field, which paves the way to probe the ultrafast electron dynamics.

In a non-Hermitian optical system with loss and gain, an exceptional point (EP) will arise under specific parameters where the eigenvalues and eigenstates exhibit simultaneous coalescence. Here we report a dynamical switching of lasing behavior in a non-Hermitian system composed of coupled microcavities by modulating the EPs. Utilizing the effect of gain, loss and coupling on the eigenstates of coupled microcavities, the evolution path of the eigenvalues related to the laser emission characteristics can be modulated. As a result, the lasing emission property of the coupled cavities exhibits an dynamical switching behavior, which can also be effectively controlled by tuning the gain and loss of the cavities. Moreover, the evolution behavior in a more complicated system composed of three coupled microcavities is investigated, which shows a better tunability compared with the two-microcavity system. Our results have correlated the EPs in non-Hermitian system with lasing emission in complex microcavity systems, which shows great potential for realizing dynamical, ultrafast and multifunctional optoelectronic devices for on-chip integrations.

Interferometry, as the key technique in modern precision measurements, has been used for length diagnosis in the fields of engineering metrology and astronomy. Analogous interferometric technique for time domain precision measurement is a significant complement to the spatial domain applications and requires the manipulation of the interference on the extreme time and energy scale. Here we present an all-optical interferometry for high precision measurement with attosecond temporal and hundreds of meV energy resolution. The interferometer is based on laser driven high order harmonics which provide a robust sequence of attosecond temporal slits. As applications, we reconstruct the waveform of an arbitrarily polarized optical pulse using the time resolving capability, and capture the abnormal character of the transition dipole near a Cooper minimum in argon using the energy resolution provided. This novel attosecond interferometry opens the possibility for high precision measurement in time energy domain using an all-optical approach., Comment: 12 pages, 5 figures in main text and 9 pages, 7 figures in supplementary material

We demonstrate an all-optical approach for precise characterization of attosecond extreme ultraviolet pulses. Isolated attosecond pulse is produced from high order harmonics using intense driving pulse with proper gating technique. When a weak field is synchronized with the driver, it perturbs the harmonics generation process via altering the accumulated phase of the electron trajectories. The perturbed harmonic spectrum can be formulated as a convolution of the unperturbed dipole and a phase gate, implying the validity of complete reconstruction of isolated attosecond pulses using conventional frequency resolved optical gating method. This in situ measurement avoids the central momentum approximation assumed in the widely used attosecond streaking measurement, providing a simple and reliable metrology for isolated attosecond pulse., Comment: 5 pages, 4 figures

An all-optical measurement of high-order fractional molecular echoes is demonstrated by using high-order harmonic generation (HHG). Excited by a pair of time-delayed short laser pulses, the signatures of full and high order fractional (1/2 and 1/3) alignment echoes are observed in the HHG signals measured from CO2 molecules at various time delays of the probe pulse. By increasing the time delay of the pump pulses, much higher order fractional (1/4) alignment echo is also observed in N2O molecules. With an analytic model based on the impulsive approximation, the spatiotemporal dynamics of the echo process are retrieved from the experiment. Compared to the typical molecular alignment revivals, high-order fractional molecular echoes are demonstrated to dephase more rapidly, which will open a new route towards the ultrashort-time measurement. The proposed HHG method paves an efficient way for accessing the high-order fractional echoes in molecules., Comment: 8 pages, 4 figures

We propose an all-optical method to directly reconstruct the band structure of semiconductors. Our scheme is based on the temporal Young's interferometer realized by high harmonic generation (HHG) with a few-cycle laser pulse. As a time-energy domain interferometric device, temporal interferometer encodes the band structure into the fringe in the energy domain. The relation between the band structure and the emitted harmonic frequencies is established. This enables us to retrieve the band structure from the HHG spectrum with a single-shot measurement. Our scheme paves the way to study matters under ambient conditions and to track the ultrafast modification of band structures.

Although TMDC monolayers offer giant optical nonlinearity within few-angstrom thickness, it is still elusive to modulate and engineer the wavefront of nonlinear emissions. The grain size of high-quality monolayers also restricts possibilities of imparting inhomogeneous or gradient profiles of phases and amplitudes by classical light sources. Plasmonic nanosieves can support huge field enhancement and precise nonlinear phase control with hundred-nanometer pixel-level resolution, however they suffer from intrinsically weak nonlinear susceptibility. In nature, epoxy represents a strong glue whose magic adhesion comes from the bonding of two intrinsic loose and nonsticky resins. Inspired by the nature of epoxy, we report a multifunctional and powerful nonlinear interfaces via integrating transition-metal dichalcogenide (TMDC) monolayers with linear plasmonic nanosieves, which cannot be accessed by either constituents. We experimentally demonstrate orbital angular momentum (OAM) generation, beam steering, versatile polarization control and holograms and of SH emission, with the proposed nonlinear interfaces. In addition, an effective second-harmonic (SH) nonlinearity \c{hi}(2) of ~25 nm/V is obtained for such systems. This designer platform synergizes the complementary advantages of TMDC monolayer, plasmonic nanosieves, geometric phases, and field enhancement, paving a distinct avenue toward designer, multi-functional, and ultra-compact nonlinear optical devices.

Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding information from the harmonic signals is usually painstaking due to the coherent nature of high-harmonic generation (HHG). Here we show that this obstacle can be effectively overcome by exploiting machine learning in HHS. Combining the machine learning with an angle-resolved HHS method, we demonstrate that the rich dynamics of molecular rotational wave packet is fully reconstructed from the angular distributions of HHG measured at various time delays of the probe pulse. The experimental retrievals are in good agreement with the numerical simulations. These findings provide a comprehensive picture of molecular rotation in space and time which will facilitate the development of related researches on molecular dynamics imaging., Comment: 8 pages, 6 figures

We revisit the mechanism of high harmonic generation (HHG) from solids by comparing HHG in laser fields with different ellipticities but constant maximum amplitude. It is shown that the cutoff of HHG is strongly extended in a circularly polarized field. Moreover, the harmonic yield with large ellipticity is comparable to or even higher than that in the linearly polarized field. To understand the underlying physics, we develop a reciprocal-space-trajectory method, which explains HHG in solids by a trajectory ensemble from different ionization times and different initial states in the reciprocal space. We show that the cutoff extension is related to an additional pre-acceleration step prior to ionization, which has been overlooked in solids. By analyzing the trajectories and the time-frequency spectrogram, we show that the HHG in solids cannot be interpreted in terms of the classical re-collision picture alone. Instead, the radiation should be described by the electronhole interband polarization, which leads to the unusual ellipticity dependence. We propose a new four-step model to understand the mechanism of HHG in solids., Comment: arXiv admin note: text overlap with arXiv:1805.12370

We investigate the high harmonic generation (HHG) in solids driven by laser fields with different ellipticities. The HHG spectra show a two-plateau structure within the energy gap between the valence band and the first conduction band. These two plateaus depend distinctly on the laser ellipticity. The first plateau is decreased while the second plateau is enhanced with increasing the laser ellipticity. To understand these phenomena, we develop an intuitive Reciprocal-Space- Trajectory (RST) method, with which HHG in solids is explained by a trajectory-ensemble from different initial states and different ionization times in the reciprocal space. In the framework of RST, we can not only quantitatively reproduce the HHG spectra, but also well understand the underlying physics of these phenomena, providing a deep insight into the mechanism of HHG in solids.

We demonstrate to image asymmetric molecular orbitals via high-order harmonic generation in a one-color inhomogeneous field. Due to the broken inversion symmetry of the inhomogeneous field in space, the returning electrons with energy in a broad range can be forced to recollide from only one direction for all the orientation angles of molecules, which therefore can be used to reconstruct asymmetric molecular orbitals. Following the procedure of molecular orbital tomography, the highest occupied molecular orbital of CO is satisfactorily reconstructed with high-order harmonic spectra driven by the inhomogeneous field. This scheme is helpful to relax the requirement of laser conditions and also applicable to other asymmetric molecules., Comment: 11 pages, 3 figures

We investigate the high-order harmonic generation (HHG) in doped semiconductors. The HHG is simulated with the single-electron time-dependent Schr\"{o}dinger equation (TDSE). The results show that the high-order harmonics in the second plateau generated from the doped semiconductors is about 1 to 3 orders of magnitude higher than those from the undoped semiconductor. The results are explained based on the analysis of the energy band structure and the time-dependent population imaging. Our work indicates that doping can effectively control the HHG in semiconductor.

Recently, nonlinear hybrid metasurface comes into an attractive new concept in the research of nanophotonics and nanotechnology. It is composed of semiconductors with an intrinsically large nonlinear susceptibility and traditional plasmonic metasurfaces, offering opportunities for efficiently generating and manipulating nonlinear optical responses. A high second-harmonic generation (SHG) conversion efficiency has been demonstrated in the mid-infrared region by using multi-quantum-well (MQW) based plasmonic metasurfaces. However, it has yet to be demonstrated in the visible region. Here we present a new type of nonlinear hybrid metasurfaces for the visible region, which consists of a single layer of tungsten disulfide (WS2) and a phased gold nanohole array. The results indicate that a large SHG susceptibility of ~0.1 nm/V at 810 nm is achieved, which is 2~3 orders of magnitude larger than that of typical plasmonic metasurfaces. Nonlinear metalenses with the focal lengths of 30 {\mu}m, 50 {\mu}m and 100 {\mu}m are demonstrated experimentally, providing a direct evidence for both generating and manipulating SH signals based on the nonlinear hybrid metasurfaces. It shows great potential applications in designing of integrated, ultra-thin, compacted and efficient nonlinear optical devices, such as frequency converters, nonlinear holography and generation of nonlinear optical vortex beam.

The ability to manipulate the frequency of light is of great importance in both fundamental quantum sciences and practical applications. Traditional method for frequency conversion relies on nonlinear optical processes, which are faced with the obstacles of low efficiency and limited bandwidth. Recent developments of topological photonics introduce the concepts of gauge potentials and magnetic fields to the realm of photons. Here, we demonstrate versatile frequency manipulation of light via photonic gauge potentials in a fiber-optic communication system. The gauge potential of frequency dimension is realized by controlling the initial phase of electro-optic phase modulation. A maximum 50 GHz frequency shift and three-fold bandwidth expansion for frequency combs are achieved by choosing different gauge potentials. By adopting two cascaded phase modulators with different gauge potentials, we also realize "negative refraction" for frequency combs and frequency "perfect imaging"for arbitrarily input spectra. These results may pave the way towards versatile frequency management in quantum optics and classical optical communications., Comment: 14 pages,5 figures

High harmonic generation in the interaction of femtosecond lasers with atoms and molecules opens the path to molecular orbital tomography and to probe the electronic dynamics with attosecond-{\AA}ngstr\"{o}m resolutions. Molecular orbital tomography requires both the amplitude and phase of the high harmonics. Yet the measurement of phases requires sophisticated techniques and represents formidable challenges at present. Here we report a novel scheme, called diffractive molecular orbital tomography, to retrieve the molecular orbital solely from the amplitude of high harmonics without measuring any phase information. We have applied this method to image the molecular orbitals of N$_2$, CO$_2$ and C$_2$H$_2$. The retrieved orbital is further improved by taking account the correction of Coulomb potential. The diffractive molecular orbital tomography scheme, removing the roadblock of phase measurement, significantly simplifies the molecular orbital tomography procedure and paves an efficient and robust way to the imaging of more complex molecules., Comment: 10 pages, 11 figures

We investigate the surface plasmonic lattice solitons (PLSs) in semi-infinite graphene sheet arrays. The surface soliton is formed as the SPPs tunneling is inhibited by the graphene nonlinearity, and meanwhile the incident power should be above a threshold value. Thanks to the strong confinement of surface plasmon polaritons (SPPs) on graphene, the effective width of surface PLSs can be squeezed into deep-subwavelength scale of ~ 0.001{\lambda}. Based on the stable propagation of surface PLSs, we find that the light propagation can be switched from the array boundary to the inner graphene sheets by reducing the incident power or increasing the chemical potential of graphene. The study may find promising application in optical switches on deep-subwavelength scale., Comment: 5 pages, 5 figures

We investigate the exceptional points (EPs) in a non-Hermitian system composed of a pair of graphene sheets with different losses. There are two surface plasmon polaritons (SPP) modes in the graphene waveguide. By varying the distance between two graphene sheets and chemical potential of graphene, the EPs appear as the eigenvalues, that is, the wave vectors of the two modes coalesce. The cross conversion of eigenmodes and variation of geometric phase can be observed by encircling the EP in the parametric space formed by the geometric parameters and chemical potential of graphene. At the same time, a certain input SPP mode may lead to completely different output. The study paves a way to the development of nanoscale sensitive optical switches and sensors.

Nanogenerators based on ZnO nanowires (NWs) realize the energy conversion at nanoscale, which are ascribed to the piezoelectric property caused by the lattice distortion of the ZnO NWs. The lattice distortion can significantly tune the electronic and optical properties, and requires a sensitive and convenient measurement. However, high-resolution transmission electron microscopy (HRTEM) technique provides a limited sensitivity of 0.01 nm on the variation of the lattice spacing and requires vacuum conditions. Here we demonstrate a highly-sensitive detection of the lattice distortion in single bent ZnO NWs by second-harmonic generation (SHG) microscopy. As the curvature of the single bent ZnO NW increases to 21 mm-1 (<4% bending distortion), it shows a significant decrease (~70%) in the SHG intensity ratio between perpendicular and parallel excitation polarization with respect to c-axis of ZnO NWs. Importantly, the extraordinary non-axisymmetrical SHG polarimetric patterns are also observed, indicating the twisting distortion around c-axis of ZnO NWs. Thus, SHG microscopy provides a sensitive all-optical and non-invasive method for in situ detecting the lattice distortion under various circumstances.