Optimization of extreme ultraviolet vortex beam based on high harmonic generation

In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as microscopy and spectroscopy.An experimental study on the HHG driven by vortex and Gaussian beams is conducted in this work.It is found that the intensity of vortex harmonics is positively correlated with the laser energy and gas pressure.The structure and intensity distribution of the vortex harmonics exhibit significant dependence on the relative position between the gas jet and the laser focus.The ring-like structures observed in the vortex harmonics,and the interference of quantum paths provide an explanation for the distinct structural characteristics.Moreover,by adjusting the relative position between the jet and laser focus,it is possible to discern the contributions from different quantum paths.The optimization of the HH vortex field is applicable to the XUV,which opens up a new way for exploiting the potential in optical spin or manipulating electrons by using the photon with tunable orbital angular momentum.

High-order harmonic generation of ZnO crystals in chirped and static electric fields

High harmonic generation in ZnO crystals under chirped single-color field and static electric field are investigated by solving the semiconductor Bloch equation(SBE). It is found that when the chirp pulse is introduced, the interference structure becomes obvious while the harmonic cutoff is not extended. Furthermore, the harmonic efficiency is improved when the static electric field is included. These phenomena are demonstrated by the classical recollision model in real space affected by the waveform of laser field and inversion symmetry. Specifically, the electron motion in k-space shows that the change of waveform and the destruction of the symmetry of the laser field lead to the incomplete X-structure of the crystal-momentum-resolved(k-resolved) inter-band harmonic spectrum. Furthermore, a pre-acceleration process in the solid four-step model is confirmed.

Elliptically polarized high-order harmonic generation of Ar atom in an intense laser field

High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(ε) in the lower-order harmonics is observed,specifically in the 13rd-order,which displays a maximal harmonic intensity at ε ≈ 0.1,rather than at ε = 0 as expected.This contradicts the general trend of harmonic yield,which typically decreases with the increase of laser ellipticity.In this study,we attribute this phenomenon to the disruption of the symmetry of the wave function by the Coulomb effect,leading to the generation of a harmonic with high ellipticity.This finding provides valuable insights into the behavior of elliptically polarized harmonics and opens up a potential way for exploring new applications in ultrafast spectroscopy and light–matter interactions.

Wavelength Dependent Nonlinear Spectroscopic Study of Third Harmonic Generation Probed by Rotational Maker Fringes Method

Efficient third-order nonlinearities of the Zinc Oxide and Al-doped Zinc Oxide were studied by Third Harmonic Generation (Third Harmonic Generation) Maker fringes to establish the effect Aluminum of Aluminum doping (Al-doping) on the cubic nonlinearities. Adding the Al-dopant to the Zinc Oxide crystal structure results in changes that affect the optical and nonlinear characteristics. Presented results indicate that the magnitude of X(3) was enhanced at single experimental wavelengths;however, across the broadband experimental spectrum, the effect of Al-doping remained relatively constant. The observed enhancement of third-order nonlinearity was purely from the bound electronic response. The observation is attributed to increased charge carriers and spontaneous polarization in the Zinc Oxide and Al-doped Zinc Oxide crystal structure.

Calibration of quantitative rescattering model for simulating vortex high-order harmonic generation driven by Laguerre–Gaussian beam with nonzero orbital angular momentum

We calibrate the macroscopic vortex high-order harmonic generation(HHG)obtained by the quantitative rescattering(QRS)model to compute single-atom induced dipoles against that by solving the time-dependent Schr?dinger equation(TDSE).We show that the QRS perfectly agrees with the TDSE under the favorable phase-matching condition,and the QRS can accurately predict the main features in the spatial profiles of vortex HHG if the phase-matching condition is not good.We uncover that harmonic emissions from short and long trajectories are adjusted by the phase-matching condition through the time-frequency analysis and the QRS can simulate the vortex HHG accurately only when the interference between two trajectories is absent.This work confirms that it is an efficient way to employ the QRS model in the single-atom response for precisely simulating the macroscopic vortex HHG.

Tailoring OAM spectrum of high-order harmonic generation driven by two mixed Laguerre–Gaussian beams with nonzero radial nodes

The extreme ultraviolet(XUV)light beam carrying orbital angular momentum(OAM)can be produced via high-order harmonic generation(HHG)due to the interaction of an intense vortex infrared laser and a gas medium.Here we show that the OAM spectrum of vortex HHG can be readily tailored by varying the radial node(from 0 to 2)in the driving laser consisting of two mixed Laguerre-Gaussian(LG)beams.We find that due to the change in spatial profile of HHG,the distribution range of the OAM spectrum can be broadened and its shape can be modified by increasing the radial node.We also show that the OAM mode range becomes much wider and its distribution shape becomes more symmetric when the harmonic order is increased from the plateau to the cutoff when the driving laser has the nonzero radial nodes.Through the map of coherence length and the evolution of harmonic field in the medium,we reveal that the favorable off-axis phase-matching conditions are greatly modified due to the change of intensity and phase distributions of driving laser with the radial node.We anticipate this work to stimulate some interests in generating the XUV vortex beam with tunable OAM spectrum through the gaseous HHG process achieved by manipulating the mode properties of the driving laser beam.

Phase-coherence dynamics of frequency-comb emission via high-order harmonic generation in few-cycle pulse trains

Frequency-comb emission via high-order harmonic generation(HHG)provides an alternative method for the coherent vacuum ultraviolet(VUV)and extreme ultraviolet(XUV)radiation at ultrahigh repetition rates.In particular,the temporal and spectral features of the HHG were shown to carry profound insight into frequency-comb emission dynamics.Here we present an ab initio investigation of the temporal and spectral coherence of the frequency comb emitted in HHG of He atom driven by few-cycle pulse trains.We find that the emission of frequency combs features a destructive and constructive coherences caused by the phase interference of HHG,leading to suppression and enhancement of frequency-comb emission.The results reveal intriguing and substantially different nonlinear optical response behaviors for frequency-comb emission via HHG.The dynamical origin of frequency-comb emission is clarified by analyzing the phase coherence in HHG processes in detail.Our results provide fresh insight into the experimental realization of selective enhancement of frequency comb in the VUV–XUV regimes.

Elliptically polarized high-order harmonic generation in nitrogen molecules with cross-linearly polarized two-color laser fields

Circularly and elliptically polarized high-order harmonics have unique advantages when used in studying the chiral and magnetic features of matter.Here,we studied the polarization properties of high-order harmonics generated from alignment nitrogen molecules driven by cross-linearly polarized two-color laser fields.Through adjusting various laser parameters and targets,such as the relative phase,the crossing angle,the intensity ratio of the driving fields,and the molecular alignment angle,we obtained highly elliptically polarized high-order harmonics with the same helicity in a wide spectral range.This provides a possible effective way to generate elliptically polarized attosecond pulses.Finally,we showed the probability of controlling the spectral range of elliptically polarized harmonics.

Role of excited states in helium-like ions on high-order harmonic generation

We theoretically investigate high-order harmonic generation(HHG) of helium(He), lithium cation(Li+), and beryllium dication(Be2+) using the time-dependent Hartree–Fock method to solve the three-dimensional time-dependent Schr ¨odinger equation. It is found that the intensity of the HHG increases significantly from a certain harmonic order below the ionization threshold, and the initial position of the enhancement does not depend on the intensity or the wavelength of the driving laser field. Further analysis shows that excited states play an important role on this enhancement,consistent with the excited-state tunneling mechanism [Phys. Rev. Lett. 116 123901(2016)]. Our results unambiguously show that excited-state tunneling is essential for understanding the enhancement of HHG. Accordingly, a four-step model is herein proposed to illustrate the multiphoton excitation effect in helium-like ions, which enriches the physics of HHG enhancement.

High-order harmonic generation of the cyclo[18]carbon molecule irradiated by circularly polarized laser pulse

High-order harmonic generation of the cyclo[18]carbon(C_(18) ) molecule under few-cycle circularly polarized laser pulse is studied by time-dependent density functional theory. Compared with the harmonic emission of the ring molecule C_(6)H_(6) having similar ionization potential, the C_(18) molecule has higher efficiency and cutoff energy than C_(6)H_(6) with the same laser field parameters. Further researches indicate that the harmonic efficiency and cutoff energy of the C_(18) molecule increase gradually with the increase of the laser intensity of the driving laser or decrease of the wavelength, both are larger than those of the C_(6)H_(6) molecule. Through the analysis of the time-dependent evolution of the electronic wave packets, it is also found that the higher efficiency of harmonic generation can be attributed to the larger spatial scale of the C_(18) molecule,which leads to a greater chance for the ionized electrons from one atom to recombine with others of the parent molecule.Selecting the suitable driving laser pulse, it is demonstrated that high-order harmonic generation in the C_(18) molecule has a wide range of applications in producing circularly polarized isolated attosecond pulse.

Second Harmonic Generation of Lamb Wave in Numerical Perspective

The influences of phase and group velocity matching on cumulative second harmonic generation of Lamb waves are investigated in numerical perspective. Finite element simulations of nonlinear Lamb wave propagation are performed for Lamb wave mode pairs with exact and approximate phase velocity matching, with and without group velocity matching, respectively. The evolution of time-domain second harmonic Lamb waves is analyzed with the propagation distance. The amplitudes of primary and second harmonic waves are calculated to characterize the acoustic nonlinearity. The results verify that phase velocity matching is necessary for generation of the cumulative second harmonic Lamb wave in numerical perspective, while group velocity matching is demonstrated to not be a necessary condition.

Photoinduced Second Harmonic Generation of Bi_2S_3 Microcrystallite Doped Silica Glass

Silica glasses doped with Bi2S3 microcystallite was prepared by the sol-gel process. Photoinduced second harmonic generation (SHG) was observed in the glass when it was irradiated with intense 1.06 μm and frequency doubled laser beams from a mode-locked Nd: YAG laser. It was found that the signal intensity increased with the irradiating time and approached a saturation gradually. The effect may be explained reasonably by the DC field model.

Dual bound states in the continuum enhanced second harmonic generation with transition metal dichalcogenides monolayer

The emergence of two dimensional(2D)materials has opened new possibilities for exhibiting second harmonic genera-tion(SHG)at the nanoscale,due to their remarkable optical response related to stable excitons at room temperature.However,the ultimate atomic-scale interaction length with light makes the SHG of Transition Metal Dichalcogenides(TM-Ds)monolayers naturally weak.Here,we propose coupling a monolayer of TMDs with a photonic grating slab that works with doubly resonant bound states in the continuum(BIC).The BIC slabs are designed to exhibit a pair of BICs,reson-ant with both the fundamental wave(FW)and the second harmonic wave(SHW).Firstly,the spatial mode matching can be fulfilled by tilting FW's incident angle.We theoretically demonstrate that this strategy leads to more than four orders of magnitude enhancement of SHG efficiency than a sole monolayer of TMDs,under a pump light intensity of 0.1 GW/cm^(2).Moreover,we demonstrate that patterning the TMDs monolayer can further enhance the spatial overlap coefficient,which leads to an extra three orders of magnitude enhancement of SHG efficiency.These results demonstrate remarkable pos-sibilities for enhancing SHG with nonlinear 2D materials,opening many opportunities for chip-based light sources,nano-lasers,imaging,and biochemical sensing.

Tunable second harmonic generation from a Kerr-lens mode-locked Yb:YCa4O(BO3)3 femtosecond laser

We experimentally demonstrated a diode-pumped Kerr-lens mode-locked femtosecond（fs） laser with a self-frequency doubling Yb：YCa_4O（BO_3）_3 crystal.Sub-40 fs laser pulses were directly generated from the oscillator without extracavity compression.The central wavelength was tunable from 1039 nm to 1049 nm with a typical bandwidth of 35 nm and an average output power of 53 mW.For the first time,a self-frequency doubled second harmonic green laser with tunable range from 519 nm to 525 nm was observed.

Restraint of spatial distribution in high-order harmonic generation from a model of hydrogen molecular ion

The spatial distribution in high-order harmonic generation（HHG） is theoretically investigated by using a few-cycle laser pulse from a two-dimensional model of a hydrogen molecular ion. The spatial distribution in HHG demonstrates that the harmonic spectra are sensitive to the carrier envelope phase and the duration of the laser pulse. The HHG can be restrained by a pulse with the duration of 5 fs in the region from the 90 th to 320th order. This characteristic is illustrated by the probability density of electron wave packet distribution. The electron is mainly located near the nucleus along the positive-x direction from 3.0 o.c. to 3.2 o.c., which is an important time to generate the HHG in the plateau area. We also demonstrate the time-frequency distribution in the region of the positive-and negative-x direction to explain the physical mechanism.

Role of excited states in the elliptically polarized harmonic generation

We theoretically investigate the contribution of the excited state to the ellipticity of the harmonics from H＋ at different orientation angles irradiated by a linearly polarized laser pulse. It is found that the first excited state has a significant influence to the ellipticity of the harmonics, and the contribution of higher excited states to the ellipticity can be neglected. Moreover, the conclusion is not dependent on the laser intensity.

Carrier envelope phase effect on the spatial distribution of high-order harmonic generation in asymmetric molecule

The spatial distribution in high-order harmonic generation（HHG） from the asymmetric diatomic molecule He H^（2＋） is investigated by numerically solving the non-Born–Oppenheimer time-dependent Schr？dinger equation（TDSE）. The spatial distribution of the HHG spectra shows that there is little contribution in HHG around the geometric center of two nuclei（z = 1.17 a.u.） and the equilibrium internuclear position of the H nucleus（z = 3.11 a.u.）. We demonstrate the carrier envelope phase（CEP） effect on the spatial distribution of HHG in a few-cycle laser pulse. The HHG process is investigated by the time evolution of the electronic density distribution. The time–frequency analysis of HHG from two nuclei in HeH^（2＋） is presented to further explain the underlying physical mechanism.

A scaling law of high-order harmonic generation

Using a nonperturbative quantum electrodynamics theory of high-order harmonic generation （HHG）, a scaling law of HHG is established. The scaling law states that when the atomic binding energy Eb, the wavelength ）, and the intensity I of the laser field change simultaneously to kEb, λ/k, and k3I, respectively. The characteristics of the HHG spectrum remain unchanged, while the harmonic yield is enhanced k3 times. That HHG obeys the same scaling law with above-threshold ionization is a solid proof of the fact that the two physical processes have similar physical mechanisms. The variation of integrated harmonic yields is also discussed.

Low-order harmonic generation of hydrogen molecular ion in laser field studied by the two-state model

The low-order harmonic generation of hydrogen molecular ion interacting with a linearly polarized laser field has been investigated theoretically by using a simple two-state model. The validity of the two-state model is carefully examined by comparing the harmonic spectra of hydrogen molecular ion obtained from this model with those from the three-dimensional time-dependent Schr¨odinger equation. When combined with the Morlet transform of quantum time-frequency spectrum,the two-state model can be used to study the dynamical origin of the low-order harmonic generation of hydrogen molecular ion driven by low-frequency pulses. In addition, some interesting structures of the time profiles for low order harmonics are obtained.

High-order harmonic generation of N2molecule in two-color circularly polarized laser fields

The generation of high-order harmonics and the attosecond pulse of the N2 molecule in two-color circularly polarized laser fields are investigated by the strong-field Lewenstein model. We show that the plateau of spectra is dramatically extended and a continuous harmonic spectrum with the bandwidth of 113 eV is obtained. When a static field is added to the x direction, the quantum path control is realized and a supercontinuum spectrum can be obtained, which is beneficial to obtain a shorter attosecond pulse. The underlying physical mechanism is well explained by the time-frequency analysis and the semi-classical three-step model with a finite initial transverse velocity. By superposing several orders of harmonics in the combination of two-color circularly polarized laser fields and a static field, an isolated attosecond pulse with a duration of 30 as can be generated.