Generating femtosecond coherent X-ray pulses in a diffractionlimited storage ring with the echo-enabled harmonic generation scheme

To study ultrafast processes at the sub-picosecond level, novel methods based on coherent harmonic generation technologies have been proposed to generate ultrashort radiation pulses in existing ring-based light sources. Using the High Energy Photon Source as an example, we numerically test the feasibility of implementing one coherent harmonic generation technology, i.e.,the echo-enabled harmonic generation(EEHG) scheme, in a diffraction-limited storage ring(DLSR). Two different EEHG element layouts are considered, and the effect of the EEHG process on the electron beam quality is also analyzed. Studies suggest that soft X-ray pulses, with pulse lengths of a few femtoseconds and peak powers of up to1 MW, can be generated by using the EEHG scheme, while causing little perturbation to the regular operation of a DLSR.

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.

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.

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.

Effect of laser focus in two-color synthesized waveform on generation of soft x-ray high harmonics

Synthesis of multi-color laser pulses has been developed as a promising way to improve low conversion efficiency of high-order harmonic generation(HHG). Here we systematically study the effect of laser focus in a two-color waveform on generation of macroscopic HHG in soft x-rays. We find that the dependence of HHG yields on laser focus at low or high gas pressure is sensitive to the characteristics of single-atom harmonic response, in which “short”-or “long”-trajectory emissions can be selectively controlled by changing the waveform of two-color synthesized laser pulse. We uncover the phase-matching mechanism of HHG in the gas medium by examining the propagation of the two-color waveform and the evolution of time-frequency emissions of high-harmonic field. We further reveal that the nonlinear effects, such as geometric phase, atomic dispersion, and plasma defocusing, are responsible for modification of two-color waveform upon propagation. This work can be used to find better macroscopic conditions for generating soft x-ray HHG by employing two-color optimized waveforms.

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.

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.

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.

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.

Generation of Higher Terahertz Harmonics in Nonlinear Paraelectrics under Focusing in a Wide Temperature Range

It is theoretically investigated the generation of higher harmonics of two-dimensional and three-dimensional terahertz electromagnetic beams in nonlinear crystals. The attention is paid to crystalline paraelectrics like SrTiO3 under the temperatures 60 - 200 K, these crystals possess the cubic nonlinearity. The bias electric field is applied to provide the dominating quadratic nonlinearity. The initial focusing of the beams not only increases the efficiency of generation of higher harmonics, but alto makes possible to select maxima of different higher harmonics at some distances from the input. At lower temperatures the nonlinearity behaves at smaller input amplitudes, whereas at higher temperatures the harmonic generation can be observed at higher frequencies up to 1.5 THz. In three-dimensional beams the peak amplitudes of higher harmonics can be bigger than in two-dimensional beams, but the ratios of these peak values to the maximum values of the focused first harmonic are smaller than in two-dimensional beams.

Role of the dressed and bound states on below-threshold harmonic generation of He atom

High-order harmonic generation below ionization threshold of He atom in the laser field is investigated by solving the three-dimensional time-dependent Schrodinger equation. An angular momentum-dependent model potential of He atom was used for getting the accurate energy levels of singlet states. The satellite-peak structures of the below-threshold harmonic generation(BTHG) of He are observed. We analyze the emission properties of the BTHG by employing a synchrosqueezing transform technique. We find that the satellite-peak structures have two types related to two kinds of transitions. One is the transition of the dressed states of the excited states, the other is the transition between the excited states and the ground state in the field-free case. Furthermore, our results show that the maximum Stark shift of the 2 p state is about 0.9 Up(penderomotive energy), and that of the 4 p state is about 1.0 Up. It indicates that the energy difference between some satellite-and main-peaks of the BTHG can be used to measure the maximum Stark shift of the excited states of He atom in the laser field.

Extension of high-order harmonics and generation of an isolated attosecond pulse in the chirped laser field

This paper theoretically investigates the high-order harmonic generation cutoff extension using intense few-cycle linearly chirped laser pulses. It shows that the cutoff of the harmonic can be extended remarkably by optimising the chirping parameters. The time-frequency characteristics of high-order harmonics with different chirping parameters are analysed by means of wavelet transform of the dipole acceleration. It also gives out the classical three-step model pictures of electron. By superposing a properly selected range of the harmonic spectrum, it obtains an isolated 65as pulse.

Effect of laser intensity on quantum trajectories in the macroscopic high-order harmonic generation

We macroscopically investigate the effect of the laser intensity and gas density on quantum trajectories in the highorder harmonic generation of Ne atoms irradiated by few-cycle, 800-nm laser pulses. The time–frequency profile of the harmonics shows that the long quantum trajectory is dominant at both lower and higher gas densities for a low laser intensity. At high laser intensities, the long quantum trajectory plays an important role for lower gas densities, while the short quantum trajectory is dominant at higher gas densities. An analysis of the phase mismatch for high-order harmonic generation shows that the primary emission of the quantum trajectories is determined by dynamic changes in the laser electric field during the propagation process.

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.

Selection of quantum path in high-order harmonics and isolated sub-100 attosecond generation in few-cycle spatially inhomogeneous laser fields

We theoretically study the selection of the quantum path in high-order harmonics（HHG） and isolated attosecond pulse generation from a one-dimensional（1D） model of a H_2~＋ molecule in few-cycle inhomogeneous laser fields.We show that the inhomogeneity of the laser fields play an important role in the HHG process.The cutoff of the harmonics can be extended remarkably,and the harmonic spectrum becomes smooth and has fewer modulations.We investigate the time-frequency profile of the time-dependent dipole,which shows that the short quantum path is enhanced and the long quantum path disappears in spatially inhomogeneous fields.The semi-classical three-step model is also applied to illustrate the physical mechanism of HHG.The influence of driving field carrier-envelop phase（CEP） on HHG is also discussed.By superposing a series of properly selected harmonics,an isolated attosecond pulse（IAP） with duration 53 as can be obtained by a 15-fs,1600-nm laser pulse with the parameter ε = 0.0013（e is the parameter that determines the order of inhomogeneity of the laser field）.

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.

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.