Tunable spectral continuous shift of high-order harmonic generation in atoms by a plasmon-assisted shaping pulse

We delve into the phenomenon of high-order harmonic generation within a helium atom under the influence of a plasmon-assisted shaping pulse.Our findings reveal an intriguing manipulation of the frequency peak position in the harmonic emission by adjusting the absolute phase parameter within the frequency domain of the shaping pulse.This phenomenon holds potential significance for experimental setups necessitating precisely tuned single harmonics.Notably,we observe a modulated shift in the created harmonic photon energy,spanning an impressive range of 1.2 eV.This frequency peak shift is rooted in the asymmetry exhibited by the rising and falling edges of the laser pulse,directly influencing the position of the peak frequency emission.Our study quantifies the dependence of this tuning range and the asymmetry of the laser pulse,offering valuable insights into the underlying mechanisms driving this phenomenon.Furthermore,our investigation uncovers the emergence of semi-integer order harmonics as the phase parameter is altered.We attribute this discovery to the intricate interference between harmonics generated by the primary and secondary return cores.This observation introduces an innovative approach for generating semi-integer order harmonics,thus expanding our understanding of high-order harmonic generation.Ultimately,our work contributes to the broader comprehension of complex phenomena in laser-matter interactions and provides a foundation for harnessing these effects in various applications,particularly those involving precise spectral control and the generation of unique harmonic patterns.

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.

Spectral shift of solid high-order harmonics from different channels in a combined laser field

We investigate theoretically the spectral shift of the high-order harmonic generation(HHG)in ZnO driven by a combined laser field by solving the two-band semiconductor Bloch equations(SBEs)in the velocity gauge.The combined laser field is synthesized by a fundamental laser pulse and its seventh-frequency laser pulse.When the seventh-frequency laser pulse is added to the rising or falling parts of the fundamental laser field,we find that the spectral blueshift or redshift appears,which is due to the unequal contribution of the rising and falling parts in the fundamental laser field to the harmonics.By analyzing the time-dependent conduction band population in k space,we found that,in addition to the tunneling ionization channel,there is also the resonant electron injection channels which is induced by the seventh-frequency laser pulse.The harmonics generated by the different channels show the spectral redshift or the spectral blueshift,respectively.Through analyzing the k-integrated transient conduction band population of the electrons from different channels,we found that if there is a certain delay in the process of the electron excitation,it will lead to the delay in the harmonic emission,which results in the spectral redshift of the harmonics.

Hybrid simulation of q=1 high-order harmonics driven by passing energetic particles in tokamak plasmas

High-order harmonics q(ψ_(s))=1 energetic particle modes(EPMs)have been observed in toroidal plasmas experiments with neutral beam injection.To investigate these phenomena,linear properties and nonlinear dynamics of these EPMs driven by passing energetic particles(EPs)are studied via the global hybrid kinetic-magnetohydrodynamic code M3D-K.Simulation results demonstrate that passing EPs'effects on high mode-number harmonics(q(ψ_(s))=m/n=2/2,3/3,4/4)instability are more obvious than the q(ψ_(s))=1/1 mode,especially when q-profile is sufficiently flat in the core region.Furthermore,the effects of the pitch angleΛ_0 and beam ion pressure P_(hot)/P_(total)on the features of high n components are also analyzed specifically.It is found that there exists only one resonant condition for these EPMs.In the nonlinear phase,these high mode-number harmonics can induce significant energetic ions redistribution and chirping up phenomena,which differs from the classical fishbone excited by passing EPs.These discoveries are conducive to better apprehend the underlying physical mechanisms of the highorder harmonics driven by passing EPs.

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.

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.

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.

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.

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.

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）.

Quantitative Measurement of the Proportions of High-Order Harmonics for the 4B7B Soft-X-Ray Source at Beijing Synchrotron Radiation Facility

A transmission grating coupled with an X-ray charge coupled device （CCD） is used to quantitatively measure the proportion of high-order harmonics of the soft-X-ray source of beam line 4B7B. The results show that the monochromatic X-ray has third-order and second-order harmonics. The proportion of second-order harmonic of 4B7B is less than 9.0% and the third- order harmonic is below 0.7% when no suppressing method is applied. When suppression methods are used, the proportion of second-order harmonic is less than 1.7% and the third-order harmonic is ignorable.

Retrieval of Electron Return Time from High-order Harmonics Generated in a Mixture of He and Ne Gases

In terms of single-atom induced dipole moment by Lewenstein model, we present the macroscopic high-order harmonic generation from mixed He and Ne gases with different mixture ratios by solving three-dimensional Maxwell＇s equation of harmonic field. And then we show the validity of mixture formulation by Wagner et al. [Phys. Rev. A 76 （2007） 061403（R）] in macroscopic response level. Finally, using/east squares fitting we retrieve the electron return time of short trajectory by formulation in Kanai et al. [Phys. Rev. Lett. 98 （2007） 153904] when the gas jet is put after the laser focus.

Generation of non-integer high-order harmonics and significant enhancement of harmonic intensity

High-order harmonics from helium atom in the orthogonally two-color(OTC) laser field are investigated by solving the two-dimensional time-dependent Schrodinger equation.Non-integer high-order harmonics are obtained in some ratio of frequencies of two components.Pure odd and even harmonics from atoms could be separated in two components by adjusting the ratio of frequencies in OTC scheme,and the resolution of harmonics is improved at the same time.The physical mechanism is explained by the periodicity of dipole.With the same intensity of the incident laser,the intensity of the high-order harmonics from the OTC field scheme is improved by three orders of magnitude compared to the monochromatic laser field scheme.A theoretical scheme is provided for experimentally achieving improving energy resolution and separation of pure odd and even harmonics in atoms.Also,we provide a means for improving harmonic intensity.

At wavelength coherent scatterometry microscope using high-order harmonics for EUV mask inspection

In this review,we describe our research on the development of the 13.5 nm coherent microscope using high-order harmonics for the mask inspection of extreme ultraviolet(EUV)lithography.EUV lithography is a game-changing piece of technology for high-volume manufacturing of commercial semiconductors.Many top manufacturers apply EUV technology for fabricating the most critical layers of 7 nm chips.Fabrication and inspection of defect-free masks,however,still remain critical issues in EUV technology.Thus,in our pursuit for a resolution,we have developed the coherent EUV scatterometry microscope(CSM)system with a synchrotron radiation(SR)source to establish the actinic metrology,along with inspection algorithms.The intensity and phase images of patterned EUV masks were reconstructed from diffraction patterns using ptychography algorithms.To expedite the practical application of the CSM,we have also developed a standalone CSM,based on high-order harmonic generation,as an alternative to the SR-CSM.Since the application of a coherent 13.5 nm harmonic enabled the production of a high contrast diffraction pattern,diffraction patterns of sub-100 ns size defects in a 2D periodic pattern mask could be observed.Reconstruction of intensity and phase images from diffraction patterns were also performed for a periodic line-and-space structure,an aperiodic angle edge structure,as well as a cross pattern in an EUV mask.

Spectral redshift of high-order harmonics by adding a weak pulse in the falling part of the trapezoidal laser pulse

We investigate the spectral redshift of high-order harmonics of the H_2~＋（D_2~＋） molecule by numerically solving the non-Born–Oppenheimer time-dependent Schr ¨odinger equation（TDSE）. The results show that the spectral redshift of highorder harmonics can be observed by adding a weak pulse in the falling part of the trapezoidal laser pulses. Comparing with the H_2~＋ molecule, the shift of high-order harmonic generation（HHG） spectrum for the D_2~＋ molecule is more obvious.We employ the spatial distribution in HHG and time-frequency analysis to illustrate the physical mechanism of the spectral redshift of high-order harmonics.

Generation-channel interference of high-order harmonics of an anharmonic oscillator driven by bi-chrime laser fields and its mechanism

A method to describe the generation channels of high-order harmonics is proposed. According to this method, the mechanism of generation-channel interference of high-order harmonics is revealed clearly. We take the anharmonic oscillator driven by bi-chrome fields as an example to illustrate that this method can be used to understand the effect of generation-channel interference.