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.

Electron correlation in two-electron atoms:A Bohmian analysis of high-order harmonic generation in high-frequency domain

In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics(BM),we have theoretically explored the two-electron correlation characteristics while generating high-order harmonics in xenon atoms subjected to intense laser fields.We initially employed Bohmian trajectories to reproduce the dynamics of the electrons and subsequently utilized time-frequency analysis spectra to ascertain the emission time windows for high-order harmonics.Within these time windows,we classified the nuclear region Bohmian trajectories and observed that intense high-order harmonics are solely generated when paired Bohmian particles(BPs)concurrently appear in the nuclear region and reside there for a duration within a re-collision time window.Furthermore,our analysis of characteristic trajectories producing high-order harmonics led us to propose a two-electron re-collision model to elucidate this phenomenon.The study demonstrates that intense high-order harmonics are only generated when both electrons are in the ground state within the re-collision time window.This work discusses the implications of correlation effects between two electrons and offers valuable insights for studying correlation in multi-electron high-order harmonic generation.

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.

Modulation of High-Order Harmonic Generation from a Monolayer ZnO by Co-rotating Two-Color Circularly Polarized Laser Fields

By numerically solving the two-dimensional semiconductor Bloch equation,we study the high-order harmonic emission of a monolayer ZnO under the driving of co-rotating two-color circularly polarized laser pulses.By changing the relative phase between the fundamental frequency field and the second one,it is found that the harmonic intensity in the platform region can be significantly modulated.In the higher order,the harmonic intensity can be increased by about one order of magnitude.Through time-frequency analysis,it is demonstrated that the emission trajectory of monolayer ZnO can be controlled by the relative phase,and the harmonic enhancement is caused by the second quantum trajectory with the higher emission probability.In addition,near-circularly polarized harmonics can be generated in the co-rotating two-color circularly polarized fields.With the change of the relative phase,the harmonics in the platform region can be altered from left-handed near-circularly polarization to right-handed one.Our results can obtain high-intensity harmonic radiation with an adjustable ellipticity,which provides an opportunity for syntheses of circularly polarized attosecond pulses.

EVOLUTION ANALYSIS OF TS WAVE AND HIGH-ORDER HARMONIC WAVES IN BOUNDARY LAYERS

Linear and nonlinear evolutions of TS wave and high-order harmonic waves in boundary layers are studied based on the parabolic stability equation （PSE）. Initial conditions are derived by the local method with the Landau expansion. The evolution process and characteristics of the disturbance amplitude and the velocity profile, etc. , especially stronger nonlinear effects, are computed by an efficient numerical method. Effects and regulations of different initial amplitudes, frequencies and pressure gradients on the evolution of disturbances are explored, which are directly relative to the stability and the transition in boundary layers. Simulation results are in good agreement with the data of the accuracy direct numerical simulation （DNS） using full Navier-Stokes equations.

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.

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.

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.

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.

Role of Bloch oscillation in high-order harmonic generation from periodic structure

The high-order harmonic generation from a model solid structure driven by an intense laser pulse is investigated using the semiconductor Bloch equations(SBEs). The main features of harmonic spectrum from SBEs agree well with the result of the time-dependent Schro¨dinger equation(TDSE), and the cut-off energy can be precisely estimated by the recollision model. With increasing the field strength, the harmonic spectrum shows an extra plateau. Based on the temporal population of electron and the time–frequency analysis, the harmonics in the extra plateau are generated by the Bloch oscillation. Due to the ultrafast time response of the Bloch electron, the generated harmonics provide a potential source of shorter isolated attosecond pulse.

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.

Extension of high-order harmonic cutoff frequency by synthesizing the waveform of a laser field via the optimization of classical electron trajectory in the laser field

We theoretically investigate high-order harmonic generation by employing strong-field approximation （SFA） and present a new approach to the extension of the high-order harmonic cutoff frequency via an exploration of the dependence of high-order harmonic generation on the waveform of laser fields. The dependence is investigated via detailed analysis of the classical trajectories of the ionized electron moving in the continuum in the velocity-position plane. The classical trajectory consists of three sections （Acceleration Away, Deceleration Away, and Acceleration Back）, and their relationship with the electron recollision energy is investigated. The analysis of classical trajectories indicates that, besides the final （Acceleration Back） section, the electron recollision energy also relies on the previous two sections. We simultaneously optimize the waveform in all three sections to increase the electron recollision energy, and an extension of the cutoff frequency up to Ip ＋ 20.26Up is presented with a theoretically synthesized waveform of the laser field.

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.

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.

Controlling the contributions to high-order harmonic generation from different nuclei of N_2 with an orthogonally polarized two-color laser field

The generation of high-order harmonic and the attosecond pulse of the N2 molecule with an orthogonally polarized two-color laser field are investigated by the strong-field Lewenstein model.We show that the control of contributions to high-order harmonic generation（HHG） from different nuclei is realized by properly selecting the relative phase.When the relative phase is chosen to be φ= 0.4π,the contribution to HHG from one nucleus is much more than that from another.Interference between two nuclei can be suppressed greatly; a supercontinuum spectrum of HHG appears from 40 e V to125 e V.The underlying physical mechanism is well explained by the time–frequency analysis and the semi-classical threestep model with a finite initial transverse velocity.By superposing several orders of harmonics,an isolated attosecond pulse with a duration of 80 as can be generated.

High-order harmonic generation in a two-color strong laser field with Bohmian trajectory theory

We theoretically study the high-order harmonic generation （HHG） in a two-color laser field using the Bohmian mechanics. Our results show that, for tile case of a weak second-color laser field, the simulation of the HHG with only one central Bohmian trajectory is in a good agreement with the ab initio time-dependent Schrodinger equation （TDSE） results. In contrast, with the increase of the amplitude of the second-color laser field, the HHG spectra from the single central Bohmian trajectory deviate from the TDSE results more and more significantly. By analyzing the Bohmian trajectories, we find that the significant deviation is due to the fact that the central Bohmian trajectory leaves the core quickly in the two-color laser field with the breaking of inversion symmetry. Interestingly, we find that another Bohmian trajectory with different initial position, which keeps oscillating around the core, could qualitatively well reproduce the TDSE results. Furthermore, we study the HHG spectrum in a two-color laser field with inversion symmetry and find that the HHG spectrum in TDSE can be still well simulated with the central Bohmian trajectory. These results indicate that, similar to the case of one color laser field, the HHG spectra in a two-color laser field can be also reproduced with a single Bohmian trajectory, although the initial position of the trajectory is dependent on the symmetry of the laser field. Our work thus demonstrates that Bohmian trajectory theory can be used as a promising tool in investigating the HHG process in a two-color laser field.

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.