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 m...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.展开更多
Optical skyrmion serves as a crucial interface between optics and topology.Recently,it has attracted great interest in linear optics.Here,we theoretically introduce a framework for the all-optical generation and contr...Optical skyrmion serves as a crucial interface between optics and topology.Recently,it has attracted great interest in linear optics.Here,we theoretically introduce a framework for the all-optical generation and control of free-space optical skyrmions in extreme ultraviolet regions via high harmonic generation(HHG).We show that by employing full Poincarébeams,the created extreme ultraviolet fields manifest as skyrmionic structures in Stokes vector fields,whose skyrmion number is relevant to harmonic orders.We reveal that the generation of the skyrmionics structure is attributed to spatial-resolved spin constraint of HHG.Through qualifying the geometrical parameters of full Poincarébeams,the topological texture of extreme ultraviolet fields can be completely manipulated,generating the Bloch-type,Néel-type,anti-type,and higher-order skyrmions.We promote the investigation of topological optics in optical highly nonlinear processes,with potential applications toward ultrafast spintronics with structured light fields.展开更多
We theoretically investigate the yield enhancement of elliptical high harmonics in the interaction of molecules with bicircular laser pulses by solving the time-dependent Schrodinger equation.It is shown that by adjus...We theoretically investigate the yield enhancement of elliptical high harmonics in the interaction of molecules with bicircular laser pulses by solving the time-dependent Schrodinger equation.It is shown that by adjusting the relative intensity ratio of the two bicircular field components in specific ranges the yield of the molecular high harmonics for the plateau and cutoff regions can be respectively enhanced.To analyze this enhancement phenomenon,we calculate the weights of the electron classical trajectories.Additionally,we also study the ellipticity distribution of harmonics for different intensity ratios.We find that these enhanced harmonics are elliptically polarized,which we mainly attribute to the recombination dipole moment of the major weighted trajectories.These enhanced elliptical extreme ultraviolet and soft x-ray radiations may serve as essential tools for exploring the ultrafast dynamics in magnetic materials and chiral media.展开更多
The symmetry of the target system plays a decisive role in the polarization of high harmonic generation(HHG).Molecules breaking the isotropic symmetry can be utilized to manipulate HHG polarization,but it has long bee...The symmetry of the target system plays a decisive role in the polarization of high harmonic generation(HHG).Molecules breaking the isotropic symmetry can be utilized to manipulate HHG polarization,but it has long been believed that prealignment is necessary to manifest the microscopic molecular structural effect within the macroscopic ensemble.In this work,we show that the molecular structural effect can be exploited in nonaligned molecular ensembles with appropriate 2-dimensional driving fields,despite the ensembles exhibiting isotropic macroscopic symmetry.The feasibility of this scheme is comprehensively elaborated with a multiscale theory from the perspective of symmetry breaking and is experimentally validated employing bichromatic counterrotating circularly polarized driving fields as an example.By varying the intensity ratio of the bichromatic components,substantially chiral high harmonics are generated from nonaligned molecules associated with the highest HHG efficiency,where,by contrast,the spectral chirality is nearly zero from the reference atom.Remarkably,we observe a simultaneous enhancement of both the chirality and yield of the harmonics from CO_(2),overcoming a commonly observed trade-off of the HHG efficiency for higher spectral chirality.Our findings hold the potential for a straightforward and robust pathway toward attosecond light sources with high brightness and large ellipticity.展开更多
Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and e...Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.展开更多
Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic hav...Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH.Based on this scheme,significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions.However,we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes.Using time-dependent density functional theory,we simulated the dynamics of HHG from NH2COOH and NH2COSH interacting with linearly polarized lasers.We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region.Our analysis indicates that this is due to the complex molecular configuration of NH_(2)COOH and NH_(2)COSH:while the NH_(2) group has C_(2v) symmetry,both COOH and COSH groups lack this symmetry.This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups,but not to NH_(2) group.Additionally,our results reveal a multi-plateau structure in HHG signal along laser polarization direction,a phenomenon arising from multi-electron and multiorbital effects during interaction between complex molecule and strong laser field.展开更多
Using nonperturbative quantum electrodynamics, we develop a scattering theory for high harmonic generation （HHG）. A transition rate formula for HHG is obtained. Applying this formula, we cal- culate the spectra of h...Using nonperturbative quantum electrodynamics, we develop a scattering theory for high harmonic generation （HHG）. A transition rate formula for HHG is obtained. Applying this formula, we cal- culate the spectra of high harmonics generated from different noble gases shined by strong laser light. We study the cutoff property of the spectra. The data show that the cutoff orders of high harmonics are greater than that predicted by the ＂3.17＂ cutoff law. As a numerical experiment, the data obtained from our repeated calculations support the newly derived theoretical expression of the cutoff law. The cutoff energy of high harmonics described by the new cutoff law, in terms of the ponderomotive energy Up and the ionization potential energy Ip, is 3.34Up 1.83Ip. The higher cutoff orders predicted by this theory are due to the absorption of the extra photons, which participate only the photon-mode up-conversion and do nothing in the photoionization process.展开更多
Efficient high harmonics generation(HHG) was demonstrated at 10 MHz repetition rate with an external femtosecond enhancement cavity, seeded by a ～70 fs post-compressed 10 MHz fiber chirped pulse amplifier(FCPA) laser...Efficient high harmonics generation(HHG) was demonstrated at 10 MHz repetition rate with an external femtosecond enhancement cavity, seeded by a ～70 fs post-compressed 10 MHz fiber chirped pulse amplifier(FCPA) laser. Operation lasting over 30 min with 0.1 m W outcoupled power at 149 nm was demonstrated. It was found that shorter pulse was beneficial for alleviating the nonlinear plasma effect and improving the efficiency of HHG. Low finesse cavity can relax the plasma nonlinearity clamped intra-cavity power and improve the cavity-locking stability. The pulse duration is expected to be below 100 fs for both 1040 nm and 149 nm outputs, making it ideal for applications such as time-resolved photoemission spectroscopy.展开更多
In atomic force microscopy(AFM), high-frequency components consisted in dynamic tip-sample interaction have been recently demonstrated as a promising technique for exploring more extensive material properties. Here we...In atomic force microscopy(AFM), high-frequency components consisted in dynamic tip-sample interaction have been recently demonstrated as a promising technique for exploring more extensive material properties. Here we present an exploratory study of high harmonic atomic force microscopy by force-spectroscopy and high harmonic imaging. Since these components are very weak compared to the fundamental response, we firstly designed a high harmonic cantilever by tuning the second order flexural resonance frequency to an integer 6 times of its fundamental mode(i.e. ω_2=6ω_1). Moreover, it is verified that high harmonic can discern extra features than topographies on different samples with amplitude/frequency modulation(AM/FM) dynamic AFM mode. In AM mode, the first resonance amplitude and 6 th harmonic amplitude were discussed. The 6 th harmonic is more sensitive than the first order response. In FM mode, it is noted that the decaying rate of the 6 th harmonic frequency is approximately 6 multiples to the slope of the fundamental frequency shift when the tip approaches to the surface of sample. This non-destructive method was also adopted to investigate the local interlayer coupling and intercalation in the two-dimensional graphene films tentatively.展开更多
We demonstrate the suppression of soft X-ray high harmonics generated by two-color laser pulses interacting with Ne gas in a gas cell. We show that harmonic suppression can occur at the proper combination of the propa...We demonstrate the suppression of soft X-ray high harmonics generated by two-color laser pulses interacting with Ne gas in a gas cell. We show that harmonic suppression can occur at the proper combination of the propagation distance and gas pressure. The physical mechanism behind is the phase mismatch between ＂short＂-trajectory harmonics generated at the early and later times through the interplay of geo- metric phase, dispersion, and plasma effects. In addition, we demonstrate that the position and depth of harmonic suppression can be tuned by increasing the gas pressure. Furthermore, the suppression can be extended to other laser focusing configurations by properly scaling macroscopic parameters. Our investigation reveals a simple controlling soft X-ray Laser Press and novel experimental scheme purely relying on the phase mismatch for selectively tabletop light sources without adopting the filters for applications.展开更多
The currently well accepted cutoff law for laser induced high harmonic spectra predicts the cutoff energy as a linear combination of two interaction energies, the ponderomotive energy Up and the atomic biding energy I...The currently well accepted cutoff law for laser induced high harmonic spectra predicts the cutoff energy as a linear combination of two interaction energies, the ponderomotive energy Up and the atomic biding energy Ip, with coefficients 3.17 and 1.32, respectively. Even though, this law has been there for twenty years or so, the background information for these two constants, such as how they relate to fundamental physics and mathematics constants, is still unknown. This simple fact, keeps this cutoff law remaining as an empirical one. Based on the cutoff property of Bessel functions and the Einstein photoelectric law in the multiphoton case, we show these two coefficients are algebraic constants, 9 - 4√2 ≈ 3.34 and 2√2-1≈1.83, respectively. A recent spectra calculation and an experimental measurement support the new cutoff law.展开更多
High-order harmonic generation（HHG） driven by two non-collinear beams including a fundamental and its weak second harmonic is numerically studied. The interference of harmonics from adjacent electron quantum paths i...High-order harmonic generation（HHG） driven by two non-collinear beams including a fundamental and its weak second harmonic is numerically studied. The interference of harmonics from adjacent electron quantum paths is found to be dependent on the relative delay of the driving pulse, and the dependences are different for different harmonic orders.This frequency dependence of the interference is attributed to the spatial frequency chirp in the HHG beam resulting from the harmonic dipole phase, which in turn provides a potential way to gain an insight into the generation of high-order harmonics. As an example, the intensity dependent dipole phase coefficient α is retrieved from the interference fringe.展开更多
We accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from int...We accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from intense laser driven high harmonic generation in gas phase. The time preserving for the selected harmonic radiation is achieved by a Czerny-Turner type monochromator designed with a conical diffraction grating mount for minimizing the time broadening caused by grating diffraction and keeping a relatively high diffraction efficiency. Our measurement shows that the photon flux of the 23-order harmonic（H23） centered at 35.7 eV is 1×10~9 photons/s approximately with a resolving power E/？E ≈ 36.This source provides an ultrashort tunable monochromatic XUV beam for ultrafast studies of electronic and structural dynamics in a large variety of matters.展开更多
This paper investigates experimentally high-order harmonic generation （HHG） of neon gas with 5-fs and 25-fs driving laser pulses. It has been demonstrated that the cutoff energy of the harmonic extreme ultraviolet p...This paper investigates experimentally high-order harmonic generation （HHG） of neon gas with 5-fs and 25-fs driving laser pulses. It has been demonstrated that the cutoff energy of the harmonic extreme ultraviolet photons is extended to 131 eV and the HHC spectrum near the cutoff region becomes continuum as the driving laser pulse duration is 5 fs; whereas much lower cutoff photon energy and discrete harmonic spectrum near the cutoff region are presented as the laser pulse duration is 25 fs. The results can be explained by the fact that neutral atoms can be exposed to more intense laser field before they are depleted by ionization because of the extremely short rising time of the few-cycle pulse. The 5-fs driving laser pulse paves the way of generation of coherent x-ray in the water window and single attosecond pulse.展开更多
High harmonic generation(HHG)delivering attosecond pulse duration with photon energy in the extreme ultraviolet spectral range has been demonstrated as a robust table-top coherent light source,allowing for the observa...High harmonic generation(HHG)delivering attosecond pulse duration with photon energy in the extreme ultraviolet spectral range has been demonstrated as a robust table-top coherent light source,allowing for the observation and manipulation of ultrafast process within the shortest time window ever made by humans.The past decade has witnessed the rapid progress of HHG from a variety of solid targets and its application for photoemission spectroscopy in condensed matter.In this article,we review the HHG in solids and the understanding of the underlying physics of HHG,which allows all-optical band structure reconstruction.We also introduce combinations of HHG source and photoemission spectroscopy,such as angular-resolved photoemission spectroscopy and photoemission electron microscopy.With the capacity of exploring a wide momentum space and high temporal resolution,the extension of attosecond science to the field of condensed matter physics will lead to new insights into the fundamental ultrafast dynamics in novel quantum materials.展开更多
We investigate high-order harmonic generations(HHGs)under comparison of Weyl cones in two types.Due to the hyperboloidal electron pocket structure,strong noncentrosymmetrical generations in high orders are observed ar...We investigate high-order harmonic generations(HHGs)under comparison of Weyl cones in two types.Due to the hyperboloidal electron pocket structure,strong noncentrosymmetrical generations in high orders are observed around a single type-ⅡWeyl point,especially at zero frequency.Such a remarkable DC signal is proved to have attributions from the intraband transition after spectral decomposition.Under weak pulse electric field,the linear optical response of a nontilted Weyl cone is consistent with the Kubo theory.With extensive numerical simulations,we conclude that the non-zero chemical potential can enhance the even-order generations,from the slightly tilted system to the over-tilted systems.In consideration of dynamical symmetries,type-Ⅰand type-ⅡWeyl cones also show different selective responses under the circularly polarized light.Finally,using a more realistic model containing two pairs of Weyl points,we demonstrate that paired Weyl points with opposite chirality can suppress the overall even-order generations.展开更多
Response of the wave packet of a one-dimensional Coulomb atom to an intense laser field is calculated using the symmetrized split operator fast Fourier method. The high-order harmonic generation （HHG） of the initial...Response of the wave packet of a one-dimensional Coulomb atom to an intense laser field is calculated using the symmetrized split operator fast Fourier method. The high-order harmonic generation （HHG） of the initial state separately being the ground and excited states is presented. When the hardness parameter a in the soft Coulomb potential V（x） =-1√x^2＋α is chosen to be small enough, the so-called hard Coulomb potential V（x）=1/｜x｜ can be obtained. It is well known that the hard one-dimensional Coulomb atom has an unstable ground state with an energy eigenvalue of - 0.5 and it has no states corresponding to physical states in the true atoms, and has the first and second excited states being degenerate. The parity effects on the HHG can be seen from the first and second excited states of the hard one-dimensional Coulomb atom. The HHG spectra of the excited states from both the soft and hard Coulomb atom models are shown to have more complex structures and to be much stronger than the corresponding HHG spectrum of the ground state of the soft Coulomb model with a = 2 in the same laser field. Laser-induced non-resonant one-photon emission is also observed.展开更多
Applying Fourier transform technique to deduction of background and noise on dE/dt-t curve, a new electrochemical method, high order harmonic oscillographic chronopotentiometry is proposed in this paper.
The high-order harmonic generation(HHG)in solids permits the exploration of the ultrafast electron dynamics in strong-field light–matter interaction.In particular,the laser ellipticity dependence of HHG provides insi...The high-order harmonic generation(HHG)in solids permits the exploration of the ultrafast electron dynamics in strong-field light–matter interaction.In particular,the laser ellipticity dependence of HHG provides insight into the energy band structure and the electron dynamics.Here,we report the harmonics up to the 10th order generated from monolayer MoS2in experiment.The perpendicular components of even harmonics display unreported enhanced yield at a finite ellipticity,which is sensitive to the crystal orientations.The abnormal ellipticity dependence indicates a novel mechanism that the Berry curvature distributed in a two-dimensional structure manipulates the subcycle electron dynamics during harmonics generation.So far,the research of the BC is limited to the theoretical configuration or one-dimensional experimental measurement,lacking a comprehensive characterization of the BC in the whole Brillouin zone.Our experiment provides a potential experimental scheme to characterize the complex BC structure in two-or three-dimensional materials and a new way to control the subcycle electron dynamics based on the Berry curvature field.展开更多
Generating Bessel-Gauss beams in the extreme ultraviolet(EUV)with attosecond pulse durations poses a significant challenge due to the limitations of conventional transmission optical components.Here,we propose a novel...Generating Bessel-Gauss beams in the extreme ultraviolet(EUV)with attosecond pulse durations poses a significant challenge due to the limitations of conventional transmission optical components.Here,we propose a novel approach to produce such beams by inducing an annular EUV source through high-order harmonic generation(HHG)under nonadiabatic phase-matching conditions.The resulting light pulse maintains temporal coherence and manifests attosecond pulse trains as confirmed by the reconstruction of attosecond beating by interference of two-photon transitions(RABBIT)measurements.Macroscopic HHG calculations reproduce the measured spatiotemporal structures,demonstrating the plasma-induced spatial modulation on the formation of an annular source.Propagation simulations further confirm the feasibility of this approach for generating attosecond Bessel-Gauss beams,presenting exciting prospects for various applications in EUV photonics and attosecond science.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974137,92250306,and 12304302)the National Key Program for Science and Technology Research and Development(Grant No.2019YFA0307700)+1 种基金the Natural Science Foundation of Jilin Province,China(Grant Nos.YDZJ202101ZYTS157 and YDZJ202201ZYTS314)the Scientific Research Foundation of Jilin Provincial Education Department,China(Grant No.JJKH20230283KJ)。
文摘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.
基金the National Key R&D Program(Grant No.2022YFA1604301)National Science Foundation of China(Grant Nos.92050201 and 92250306)for the financial support.
文摘Optical skyrmion serves as a crucial interface between optics and topology.Recently,it has attracted great interest in linear optics.Here,we theoretically introduce a framework for the all-optical generation and control of free-space optical skyrmions in extreme ultraviolet regions via high harmonic generation(HHG).We show that by employing full Poincarébeams,the created extreme ultraviolet fields manifest as skyrmionic structures in Stokes vector fields,whose skyrmion number is relevant to harmonic orders.We reveal that the generation of the skyrmionics structure is attributed to spatial-resolved spin constraint of HHG.Through qualifying the geometrical parameters of full Poincarébeams,the topological texture of extreme ultraviolet fields can be completely manipulated,generating the Bloch-type,Néel-type,anti-type,and higher-order skyrmions.We promote the investigation of topological optics in optical highly nonlinear processes,with potential applications toward ultrafast spintronics with structured light fields.
基金Project supported by the National Natural Science Foundation of China(Grant No.11904269)the Natural Science Foundation of Hubei Province,China(Grant Nos.2021CFB300 and 2020CFB362)Scientific Research Program of Hubei Provincial Department of Education(Grant No.B2020176)。
文摘We theoretically investigate the yield enhancement of elliptical high harmonics in the interaction of molecules with bicircular laser pulses by solving the time-dependent Schrodinger equation.It is shown that by adjusting the relative intensity ratio of the two bicircular field components in specific ranges the yield of the molecular high harmonics for the plateau and cutoff regions can be respectively enhanced.To analyze this enhancement phenomenon,we calculate the weights of the electron classical trajectories.Additionally,we also study the ellipticity distribution of harmonics for different intensity ratios.We find that these enhanced harmonics are elliptically polarized,which we mainly attribute to the recombination dipole moment of the major weighted trajectories.These enhanced elliptical extreme ultraviolet and soft x-ray radiations may serve as essential tools for exploring the ultrafast dynamics in magnetic materials and chiral media.
基金supported by the National Key Research and Development Program(Grant No.2023YFA1406800)the National Natural Science Foundation of China(NSFC)(Grant Nos.12174134,12021004,12104389,and 12225406).
文摘The symmetry of the target system plays a decisive role in the polarization of high harmonic generation(HHG).Molecules breaking the isotropic symmetry can be utilized to manipulate HHG polarization,but it has long been believed that prealignment is necessary to manifest the microscopic molecular structural effect within the macroscopic ensemble.In this work,we show that the molecular structural effect can be exploited in nonaligned molecular ensembles with appropriate 2-dimensional driving fields,despite the ensembles exhibiting isotropic macroscopic symmetry.The feasibility of this scheme is comprehensively elaborated with a multiscale theory from the perspective of symmetry breaking and is experimentally validated employing bichromatic counterrotating circularly polarized driving fields as an example.By varying the intensity ratio of the bichromatic components,substantially chiral high harmonics are generated from nonaligned molecules associated with the highest HHG efficiency,where,by contrast,the spectral chirality is nearly zero from the reference atom.Remarkably,we observe a simultaneous enhancement of both the chirality and yield of the harmonics from CO_(2),overcoming a commonly observed trade-off of the HHG efficiency for higher spectral chirality.Our findings hold the potential for a straightforward and robust pathway toward attosecond light sources with high brightness and large ellipticity.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFE0134200)the National Natural Science Foundation of China(Grant No.12204214)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.GK202207012)QCYRCXM-2022-241。
文摘Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.
基金supported by the Fundamental Research Funds for the Central Universities(Grant Nos.GK202207012 and QCYRCXM-2022-241).
文摘Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH.Based on this scheme,significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions.However,we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes.Using time-dependent density functional theory,we simulated the dynamics of HHG from NH2COOH and NH2COSH interacting with linearly polarized lasers.We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region.Our analysis indicates that this is due to the complex molecular configuration of NH_(2)COOH and NH_(2)COSH:while the NH_(2) group has C_(2v) symmetry,both COOH and COSH groups lack this symmetry.This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups,but not to NH_(2) group.Additionally,our results reveal a multi-plateau structure in HHG signal along laser polarization direction,a phenomenon arising from multi-electron and multiorbital effects during interaction between complex molecule and strong laser field.
文摘Using nonperturbative quantum electrodynamics, we develop a scattering theory for high harmonic generation （HHG）. A transition rate formula for HHG is obtained. Applying this formula, we cal- culate the spectra of high harmonics generated from different noble gases shined by strong laser light. We study the cutoff property of the spectra. The data show that the cutoff orders of high harmonics are greater than that predicted by the ＂3.17＂ cutoff law. As a numerical experiment, the data obtained from our repeated calculations support the newly derived theoretical expression of the cutoff law. The cutoff energy of high harmonics described by the new cutoff law, in terms of the ponderomotive energy Up and the ionization potential energy Ip, is 3.34Up 1.83Ip. The higher cutoff orders predicted by this theory are due to the absorption of the extra photons, which participate only the photon-mode up-conversion and do nothing in the photoionization process.
基金support of the Photon Frontier Network Program of the Ministry of Education,Culture,Sports,Science and Technology(MEXT),Japan
文摘Efficient high harmonics generation(HHG) was demonstrated at 10 MHz repetition rate with an external femtosecond enhancement cavity, seeded by a ～70 fs post-compressed 10 MHz fiber chirped pulse amplifier(FCPA) laser. Operation lasting over 30 min with 0.1 m W outcoupled power at 149 nm was demonstrated. It was found that shorter pulse was beneficial for alleviating the nonlinear plasma effect and improving the efficiency of HHG. Low finesse cavity can relax the plasma nonlinearity clamped intra-cavity power and improve the cavity-locking stability. The pulse duration is expected to be below 100 fs for both 1040 nm and 149 nm outputs, making it ideal for applications such as time-resolved photoemission spectroscopy.
基金supported by the Ministry of Science and Technology(MOST)of China(Grant No.2016YFA0200700)the National Natural Science Foundation of China(Grant Nos.21622304,61674045,11604063)+2 种基金Key Research Program of Frontier Sciences,Chinese Academy of Sciences(Grant No.QYZDB-SSW-SYS031)Osaka University's International Joint Research Promotion Program(Grant Nos.J171013014,J171013007)Distinguished Technical Talents Project and Youth Innovation Promotion Association,Chinese Academy of Sciences
文摘In atomic force microscopy(AFM), high-frequency components consisted in dynamic tip-sample interaction have been recently demonstrated as a promising technique for exploring more extensive material properties. Here we present an exploratory study of high harmonic atomic force microscopy by force-spectroscopy and high harmonic imaging. Since these components are very weak compared to the fundamental response, we firstly designed a high harmonic cantilever by tuning the second order flexural resonance frequency to an integer 6 times of its fundamental mode(i.e. ω_2=6ω_1). Moreover, it is verified that high harmonic can discern extra features than topographies on different samples with amplitude/frequency modulation(AM/FM) dynamic AFM mode. In AM mode, the first resonance amplitude and 6 th harmonic amplitude were discussed. The 6 th harmonic is more sensitive than the first order response. In FM mode, it is noted that the decaying rate of the 6 th harmonic frequency is approximately 6 multiples to the slope of the fundamental frequency shift when the tip approaches to the surface of sample. This non-destructive method was also adopted to investigate the local interlayer coupling and intercalation in the two-dimensional graphene films tentatively.
基金Fundamental Research Funds for the Central Universities of China(30916011207)National Natural Science Foundation of China(NSFC)(11774175)+1 种基金U.S. Department of Energy(DOE)(DE-FG02-86ER13491)Air Force Office of Scientific Research(AFOSR)(FA9550-14-1-0255)
文摘We demonstrate the suppression of soft X-ray high harmonics generated by two-color laser pulses interacting with Ne gas in a gas cell. We show that harmonic suppression can occur at the proper combination of the propagation distance and gas pressure. The physical mechanism behind is the phase mismatch between ＂short＂-trajectory harmonics generated at the early and later times through the interplay of geo- metric phase, dispersion, and plasma effects. In addition, we demonstrate that the position and depth of harmonic suppression can be tuned by increasing the gas pressure. Furthermore, the suppression can be extended to other laser focusing configurations by properly scaling macroscopic parameters. Our investigation reveals a simple controlling soft X-ray Laser Press and novel experimental scheme purely relying on the phase mismatch for selectively tabletop light sources without adopting the filters for applications.
文摘The currently well accepted cutoff law for laser induced high harmonic spectra predicts the cutoff energy as a linear combination of two interaction energies, the ponderomotive energy Up and the atomic biding energy Ip, with coefficients 3.17 and 1.32, respectively. Even though, this law has been there for twenty years or so, the background information for these two constants, such as how they relate to fundamental physics and mathematics constants, is still unknown. This simple fact, keeps this cutoff law remaining as an empirical one. Based on the cutoff property of Bessel functions and the Einstein photoelectric law in the multiphoton case, we show these two coefficients are algebraic constants, 9 - 4√2 ≈ 3.34 and 2√2-1≈1.83, respectively. A recent spectra calculation and an experimental measurement support the new cutoff law.
基金Project supported by the National Key Basic Research Program of China(Grant Nos.2013CB922401 and 2013CB922402)the National Key Scientific Instrument and Equipment Development Projects,China(Grant No.2012YQ12004704)+1 种基金the National Natural Science Foundation of China(Grant No.11374356)the International Joint Research Program of National Natural Science Foundation of China(Grant No.61210017)
文摘High-order harmonic generation（HHG） driven by two non-collinear beams including a fundamental and its weak second harmonic is numerically studied. The interference of harmonics from adjacent electron quantum paths is found to be dependent on the relative delay of the driving pulse, and the dependences are different for different harmonic orders.This frequency dependence of the interference is attributed to the spatial frequency chirp in the HHG beam resulting from the harmonic dipole phase, which in turn provides a potential way to gain an insight into the generation of high-order harmonics. As an example, the intensity dependent dipole phase coefficient α is retrieved from the interference fringe.
基金Project supported by the National Natural Science Foundation of China(Grants Nos.11627807,11127403,and 11474130)the National Basic Research Program of China(Grant No.2013CB922200)the Natural Science Foundation of Jilin Province of China(Grant No.20160101332JC)
文摘We accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from intense laser driven high harmonic generation in gas phase. The time preserving for the selected harmonic radiation is achieved by a Czerny-Turner type monochromator designed with a conical diffraction grating mount for minimizing the time broadening caused by grating diffraction and keeping a relatively high diffraction efficiency. Our measurement shows that the photon flux of the 23-order harmonic（H23） centered at 35.7 eV is 1×10~9 photons/s approximately with a resolving power E/？E ≈ 36.This source provides an ultrashort tunable monochromatic XUV beam for ultrafast studies of electronic and structural dynamics in a large variety of matters.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 60608003,10874237 and 60808007)the National Basic Research Program of China (973 Program) (Grant No. 2007CB815104)
文摘This paper investigates experimentally high-order harmonic generation （HHG） of neon gas with 5-fs and 25-fs driving laser pulses. It has been demonstrated that the cutoff energy of the harmonic extreme ultraviolet photons is extended to 131 eV and the HHC spectrum near the cutoff region becomes continuum as the driving laser pulse duration is 5 fs; whereas much lower cutoff photon energy and discrete harmonic spectrum near the cutoff region are presented as the laser pulse duration is 25 fs. The results can be explained by the fact that neutral atoms can be exposed to more intense laser field before they are depleted by ionization because of the extremely short rising time of the few-cycle pulse. The 5-fs driving laser pulse paves the way of generation of coherent x-ray in the water window and single attosecond pulse.
基金supported by the National Natural Science Foundation of China(Grant Nos.91850209,12174435 and 12034020)the National Key Research and Development Program of China(2017YFB0405202,2018YFB1107200).
文摘High harmonic generation(HHG)delivering attosecond pulse duration with photon energy in the extreme ultraviolet spectral range has been demonstrated as a robust table-top coherent light source,allowing for the observation and manipulation of ultrafast process within the shortest time window ever made by humans.The past decade has witnessed the rapid progress of HHG from a variety of solid targets and its application for photoemission spectroscopy in condensed matter.In this article,we review the HHG in solids and the understanding of the underlying physics of HHG,which allows all-optical band structure reconstruction.We also introduce combinations of HHG source and photoemission spectroscopy,such as angular-resolved photoemission spectroscopy and photoemission electron microscopy.With the capacity of exploring a wide momentum space and high temporal resolution,the extension of attosecond science to the field of condensed matter physics will lead to new insights into the fundamental ultrafast dynamics in novel quantum materials.
基金performed at the Chinese Academy of Science Terahertz Science Centersupported by the National Natural Science Foundation of China(Grant No.61988102)
文摘We investigate high-order harmonic generations(HHGs)under comparison of Weyl cones in two types.Due to the hyperboloidal electron pocket structure,strong noncentrosymmetrical generations in high orders are observed around a single type-ⅡWeyl point,especially at zero frequency.Such a remarkable DC signal is proved to have attributions from the intraband transition after spectral decomposition.Under weak pulse electric field,the linear optical response of a nontilted Weyl cone is consistent with the Kubo theory.With extensive numerical simulations,we conclude that the non-zero chemical potential can enhance the even-order generations,from the slightly tilted system to the over-tilted systems.In consideration of dynamical symmetries,type-Ⅰand type-ⅡWeyl cones also show different selective responses under the circularly polarized light.Finally,using a more realistic model containing two pairs of Weyl points,we demonstrate that paired Weyl points with opposite chirality can suppress the overall even-order generations.
基金Project supported by the National Natural Science Foundation of China （Grant No 10474138） and the National High-Tech Inertial Confinement Fusion Committee in China.
文摘Response of the wave packet of a one-dimensional Coulomb atom to an intense laser field is calculated using the symmetrized split operator fast Fourier method. The high-order harmonic generation （HHG） of the initial state separately being the ground and excited states is presented. When the hardness parameter a in the soft Coulomb potential V（x） =-1√x^2＋α is chosen to be small enough, the so-called hard Coulomb potential V（x）=1/｜x｜ can be obtained. It is well known that the hard one-dimensional Coulomb atom has an unstable ground state with an energy eigenvalue of - 0.5 and it has no states corresponding to physical states in the true atoms, and has the first and second excited states being degenerate. The parity effects on the HHG can be seen from the first and second excited states of the hard one-dimensional Coulomb atom. The HHG spectra of the excited states from both the soft and hard Coulomb atom models are shown to have more complex structures and to be much stronger than the corresponding HHG spectrum of the ground state of the soft Coulomb model with a = 2 in the same laser field. Laser-induced non-resonant one-photon emission is also observed.
文摘Applying Fourier transform technique to deduction of background and noise on dE/dt-t curve, a new electrochemical method, high order harmonic oscillographic chronopotentiometry is proposed in this paper.
基金Zhangjiang LaboratoryNational Natural Science Foundation of China(91950203,11874374)。
文摘The high-order harmonic generation(HHG)in solids permits the exploration of the ultrafast electron dynamics in strong-field light–matter interaction.In particular,the laser ellipticity dependence of HHG provides insight into the energy band structure and the electron dynamics.Here,we report the harmonics up to the 10th order generated from monolayer MoS2in experiment.The perpendicular components of even harmonics display unreported enhanced yield at a finite ellipticity,which is sensitive to the crystal orientations.The abnormal ellipticity dependence indicates a novel mechanism that the Berry curvature distributed in a two-dimensional structure manipulates the subcycle electron dynamics during harmonics generation.So far,the research of the BC is limited to the theoretical configuration or one-dimensional experimental measurement,lacking a comprehensive characterization of the BC in the whole Brillouin zone.Our experiment provides a potential experimental scheme to characterize the complex BC structure in two-or three-dimensional materials and a new way to control the subcycle electron dynamics based on the Berry curvature field.
基金supported by National Natural Science Foundation of China(Grants Nos.12450402,12134005,92250306,11627807,and 12274230)the National Basic Research Program of China(No.2019YFA0307700)+1 种基金Funding of Nanjing University of Science and Technology(NJUST)(No.TSXK2022D005)the Fundamental Research Funds for the Central Universities.
文摘Generating Bessel-Gauss beams in the extreme ultraviolet(EUV)with attosecond pulse durations poses a significant challenge due to the limitations of conventional transmission optical components.Here,we propose a novel approach to produce such beams by inducing an annular EUV source through high-order harmonic generation(HHG)under nonadiabatic phase-matching conditions.The resulting light pulse maintains temporal coherence and manifests attosecond pulse trains as confirmed by the reconstruction of attosecond beating by interference of two-photon transitions(RABBIT)measurements.Macroscopic HHG calculations reproduce the measured spatiotemporal structures,demonstrating the plasma-induced spatial modulation on the formation of an annular source.Propagation simulations further confirm the feasibility of this approach for generating attosecond Bessel-Gauss beams,presenting exciting prospects for various applications in EUV photonics and attosecond science.
