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.

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.

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.

Interference of harmonics emitted by different tunneling momentum channels in laser fields

By numerically solving the semiconductor Bloch equation(SBEs),we theoretically study the high-harmonic generation of ZnO crystals driven by one-color and two-color intense laser pulses.The results show the enhancement of harmonics and the cut-off remains the same in the two-color field,which can be explained by the recollision trajectories and electron excitation from multi-channels.Based on the quantum path analysis,we investigate contribution of different ranges of the crystal momentum k of ZnO to the harmonic yield,and find that in two-color laser fields,the intensity of the harmonic yield of different ranges from the crystal momentum makes a big difference and the harmonic intensity is depressed from all k channels,which is related to the interferences between harmonics from symmetric k channels.

Analysis of third and one-third harmonic generation in lossy waveguides

A comprehensive study on the requirements for the highly efficient third harmonic generation(THG) and its inverse process, one-third harmonic generation(OTHG), in lossy waveguides is proposed. The field intensity restrictions for both THG and OTHG caused by loss are demonstrated. The effective relative phase ranges, supporting the positive growth of signal fields of THG and OTHG are shrunken by the loss. Furthermore, it turns out that the effective relative phase ranges depend on the intensities of the interacting fields. At last, a modified definition of coherent length in loss situation, which evaluates the phase matching degree more precisely, is proposed by incorporating the shrunken relative phase range and the nonlinear phase mismatch. These theoretical analysis are valuable for guiding the experimental designs for highly efficient THG and OTHG.

Cavity-Enhanced Third Harmonic Generation

We derive the analytical expression of microcavity-enhanced factor for third harmonic generation in terms of detunings, linewidths, and the Purcell factors of the relevant microcavity modes. It is suitable for microcavities with any dimensions and arbitrary geometric shapes.

Nonlinear Cascaded Femtosecond Third Harmonic Generation by Multi-grating Periodically Poled MgO-doped Lithium Niobate

Nonlinear cascaded femtosecond third harmonic generation was experimentally investigated pumped by 100 fs pulses at optical communication band 1550 nm using a multi-grating 5 mol. % MgO-doped periodically poled lithium niobate crystal. The optimized efficiency of 10.8% was achieved with the simultaneous phase-matching of the second harmonic and sum frequency process. And the third harmonic spectrum reached as broad as 8.7 nm because of the choosing of a small group velocity mismatching between the fundamental and second harmonic pulses. Nonlinear cascaded method will provide a reference for the efficient frequency conversion in the high intensity range.

Enhanced wide-angle third-harmonic generation in flat-band-engineered quasi-BIC metagratings

Nonlinear metasurfaces and photonic crystals provide a significant way to generate and manipulate nonlinear signals owing to the resonance-and symmetry-based light-matter interactions supported by the artificial structures.However,the nonlinear conversion efficiency is generally limited by the angular dispersion of optical resonances especially in nonparaxial photonics.Here,we propose a metagrating realizing a quasi-bound-state in the continuum in a flat band to dramatically improve the third harmonic generation(THG)efficiency.A superior operating angular range is achieved based on the interlayer and intralayer couplings,which are introduced by breaking the mirror symmetry of the metagrating.We demonstrate the relation of angular dispersion between the nonlinear and linear responses at different incident angles.We also elucidate the mechanism of these offaxis flat-band-based nonlinear conversions through different mode decomposition.Our scheme provides a robust and analytical way for nonparaxial nonlinear generation and paves the way for further applications such as wide-angle nonlinear information transmission and enhanced nonlinear generation under tight focusing.

Optical third-harmonic generation of spherical quantum dots under inversely quadratic Hellmann plus inversely quadratic potential

The third-harmonic generation(THG)coefficient for a spherical quantum dot system with inversely quadratic Hellmann plus inversely quadratic potential is investigated theoretically,considering the regulation of quantum size,confinement potential depth and the external environment.The numerical simulation results indicate that the THG coefficient can reach the order of 10~(-12)m~2V~(-2),which strongly relies on the tunable factor,with its resonant peak experiencing a redshift or blueshift.Interestingly,the effect of temperature on the THG coefficient in terms of peak location and size is consistent with the quantum dot radius but contrasts with the hydrostatic pressure.Thus,it is crucial to focus on the influence of internal and external parameters on nonlinear optical effects,and to implement the theory in practical experiments and the manufacture of optoelectronic devices.

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.

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.