Attosecond light pulses have revolutionized the study of electron dynamics in materials by enabling the observation of ultrafast processes with unprecedented attosecond temporal resolution.They are primarily generated...Attosecond light pulses have revolutionized the study of electron dynamics in materials by enabling the observation of ultrafast processes with unprecedented attosecond temporal resolution.They are primarily generated through the process of high-order harmonic generation.This paper presents a comprehensive setup for attosecond pulse generation and measurement.Using a 900 nm,7 mJ,and 7 fs femtosecond laser with stabilized carrier-envelope phase,we employ polarization gating to generate a near single-cycle,linearly polarized pulse that interacts with neon gas to produce a broadband extreme-ultraviolet continuum with a cutoff photon energy of∼120 eV.The temporal and spectral characteristics of the generated single attosecond pulses are measured using an attosecond streak camera,and the pulse duration is determined to be 59 as through the frequency-resolved optical gating for complete reconstruction of attosecond bursts retrieval algorithm.As part of the Synergetic Extreme Condition User Facility,this setup will facilitate ultrafast research in transient absorption and photoelectron spectroscopy,providing global users with a powerful tool for studying electron dynamics in various materials.展开更多
This review comprehensively explores the theory and applications of attosecond transient absorption spectroscopy(ATAS)in studying ultrafast electronic dynamics across various systems,from atoms to solids.Driven by sig...This review comprehensively explores the theory and applications of attosecond transient absorption spectroscopy(ATAS)in studying ultrafast electronic dynamics across various systems,from atoms to solids.Driven by significant advancements in ultrafast laser technology,such as generating isolated attosecond pulses,ATAS enables detailed investigations of ultrafast electronic processes with unprecedented time resolution.The article introduces the fundamental principles and historical development of ATAS.Applications of ATAS are discussed in three main domains:in atoms,where it has been used to study build-up dynamics of Autler–Townes splitting,Fano resonance,light-induced states,etc.;in molecules,where it has revealed coherent molecular wavepacket dynamics and non-adiabatic dynamics near conical intersections;and in solids,where it has been extended to investigate ultrafast charge carrier dynamics in metals,semiconductors,and insulators.The review highlights the potential of ATAS in developing ultrafast optical switches and petahertz electronics.The ability of ATAS to probe and manipulate electronic dynamics at the attosecond timescale provides a powerful tool for exploring the fundamental limits of electronic and optical processes in materials.展开更多
A mid-infrared femtosecond pulse laser with a single cycle and high intensity is an ideal driving light source for generating isolated attosecond pulses. Due to current experimental limitations, it is difficult to dir...A mid-infrared femtosecond pulse laser with a single cycle and high intensity is an ideal driving light source for generating isolated attosecond pulses. Due to current experimental limitations, it is difficult to directly achieve this type of laser light source in the laboratory. In this paper, we obtain such an ideal light source by adding a Ti sapphire pulse to the combined pulse laser consisting of two mid-infrared pulses. Specifically, by combining the synthesized pulse consisting of 8 fs/1200 nm/1.62 × 10^(14)W cm^(-2)and 12 fs/1800 nm/2.71 × 10^(14)W cm^(-2)with an additional 8 fs/800 nm/1.26 × 10^(14)W cm^(-2)Ti sapphire pulse, the resulting electric field waveform is very close to that of a 1170 nm femtosecond pulse with an intensity of 1.4 × 10^(15)W cm^(-2), a single-cycle pulse width, and a carrier-envelope phase of 0.25π. Numerical simulations show that both cases produce high-order harmonic emission spectra with broadband supercontinuum spectra, however, the bandwidth of the supercontinuum spectra and the harmonic intensities in the synthesized pulses are significantly better than those in the single1170 nm pulse. After inverse Fourier transform, we obtain 66 as a high-intensity isolated attosecond pulse, whose intensity is five orders of magnitude higher than that of a monochromatic field. Here, the phase differences between three combined pulse lasers have little effect on the numerical simulation results when they vary in the range of 0.3π.展开更多
The attosecond extreme ultraviolet(XUV) pulse pump and femtosecond infrared(IR) pulse probe scheme is commonly used to study the dynamics and attosecond transient absorption(ATA) spectra of microscopic systems. In a r...The attosecond extreme ultraviolet(XUV) pulse pump and femtosecond infrared(IR) pulse probe scheme is commonly used to study the dynamics and attosecond transient absorption(ATA) spectra of microscopic systems. In a recent report [Proc. Natl. Acad. Sci. USA 121 e2307836121(2024)], we showed that shaped XUV pulses with spectral minima can significantly alter the absorption line shape of helium's 2s2p doubly excited state within a few tens of attoseconds.However, it remains unclear if similar effects could be observed in a singly excited state. In this study, we use shaped XUV pulses to excite helium's 2p singly excited state and couple the 2p and 3d states with a delayed IR pulse. Comparing these results with those from Gaussian XUV pulses, we find that the ATA spectra for the shaped XUV pulses exhibit more pronounced changes with delay, while the changes for the Gaussian pulses are gradual. We also explain these differences through population changes and analytical models. Our findings show that shaped XUV pulses can regulate the dynamics and absorption spectra of a singly excited state.展开更多
We introduce a time-dependent generalized Floquet(TDGF)approach to calculate attosecond transient absorption spectra of helium atoms subjected to the combination of an attosecond extreme ultraviolet(XUV)pulse and a de...We introduce a time-dependent generalized Floquet(TDGF)approach to calculate attosecond transient absorption spectra of helium atoms subjected to the combination of an attosecond extreme ultraviolet(XUV)pulse and a delayed few-cycle infrared(IR)laser pulse.This TDGF approach provides a Floquet understanding of the laser-induced change of resonant absorption lineshape.It is analytically demonstrated that the phase shift of the time-dependent dipole moment that results in the lineshape changes consists of two components,the adiabatic laser-induced phase(LIP)due to the IR-induced Stark shifts of adiabatic Floquet states and the non-adiabatic phase correction due to the non-adiabatic IR-induced coupling between adiabatic Floquet states.Comparisons of the spectral lineshape calculated based on the TDGF approach with the results obtained with the LIP model[Phys.Rev.A 88033409(2013)]and the rotating-wave approximation(RWA)are presented for several typical cases,demonstrating that TDGF universally and accurately captures IR-induced lineshape changes.It is suggested that the LIP model works as long as the generalized adiabatic theorem[PRX Quantum 2030302(2021)]holds,and the RWA works when the higher-order IR-coupling effect in the formation of adiabatic Floquet states is neglectable.展开更多
Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast ele...Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.展开更多
We theoretically investigate the high-order harmonic generation from stretched molecules in a linearly polarized intense field. By adopting an infrared pulse combined with an ultraviolet （UV） attosecond pulse, the i...We theoretically investigate the high-order harmonic generation from stretched molecules in a linearly polarized intense field. By adopting an infrared pulse combined with an ultraviolet （UV） attosecond pulse, the ionization process can be controlled effectively. In this excitation scheme, the harmonic spectrum beyond Ip ＋ 3.17Up is significantly enhanced by two orders, where Ip and Up = e^2E0^2/（4mew^2） are the ionization and ponderomotive potential, then smooth broadband supercontinuum with the bandwidth of about 120 eV is obtained, which leads to an isolated sub-60- as attosecond pulse with a high signal-noise ratio. Moreover, the bandwidth of the supercontinuum is weakly dependent on the location and pulse duration of the UV pulse.展开更多
We utilized a set of fused silica thin plates to broaden the spectrum of 1kHz,30 fs Ti:sapphire amplified laser pulses to an octave.Following the compression by chirped mirror pairs,the generated few-cycle pulses were...We utilized a set of fused silica thin plates to broaden the spectrum of 1kHz,30 fs Ti:sapphire amplified laser pulses to an octave.Following the compression by chirped mirror pairs,the generated few-cycle pulses were focused onto an argon filled gas cell.We detected high order harmonics corresponding to a train of 209 as pulses,characterized by the reconstruction of attosecond beating by interference of two-photon transition(RABITT)technique.Compared with the conventional attosecond pulse trains,the broad harmonics in such pulse trains cover more energy range,so it is more efficient in studying some typical cases,such as resonances,with frequency resolved RABITT.As the solid thin plates can support high power supercontinuum generation,it is feasible to tailor the spectrum to have different central wavelength and spectral width,which will make the RABITT source work in different applications.展开更多
We theoretically investigate high-order harmonic generation in a two-color multi-cycle inhomogeneous field combined with a 27th harmonic pulse. By considering a bowtie-shaped gold nanostructure, the spatiotemporal pro...We theoretically investigate high-order harmonic generation in a two-color multi-cycle inhomogeneous field combined with a 27th harmonic pulse. By considering a bowtie-shaped gold nanostructure, the spatiotemporal profiles of enhanced plasmonic fields are obtained by solving the Maxwell equation using finite-domain time-difference method. Based on quantum-mechanical and classical models, the effect of 27th harmonic pulse, temporal profile of enhanced plasmonic field and inhomogeneity on supercontinuum generation are analyzed and discussed. As a result, broadband supercontinuum can be generated from our approach with optimized gap size of nanostructure. Moreover, these results are not sensitively dependent on the relative phase in the two-color field.展开更多
The attosecond laser station （ALS） at the Synergetic Extreme Condition User Facility （SECUF） is a sophisticated and user-friendly platform for the investigation of the electron dynamics in atoms, molecules, and co...The attosecond laser station （ALS） at the Synergetic Extreme Condition User Facility （SECUF） is a sophisticated and user-friendly platform for the investigation of the electron dynamics in atoms, molecules, and condensed matter on timescales ranging from tens of femtoseconds to tens of attoseconds. Short and tunable coherent extreme-ultraviolet （XUV） light sources based on high-order harmonic generation in atomic gases are being developed to drive a variety of endstations for inspecting and controlling ultrafast electron dynamics in real time. The combination of such light sources and end-stations offers a route to investigate fundamental physical processes in atoms, molecules, and condensed matter. The ALS consists of four beamlines, each containing a light source designed specifically for application experiments that will be performed in its own end-station. The first beamline will produce broadband XUV light for attosecond photoelectron spectroscopy and attosecond transient absorption spectroscopy. It is also capable of performing attosecond streaking to characterize isolated attosecond pulses and will allow studies on the electron dynamics in atoms, moleculars, and condensed matter. The second XUV beamline will produce narrowband femtoseeond XUV pulses for time-resolved and angle-resolved photoelectron spectroscopy, to study the electronic dynamics on the timescale of fundamental correlations and interactions in solids, especially in superconductors and topological insulators. The third beamline will produce broadband XUV pulses for attosecond coincidence spectroscopy in a cold-target recoil-ion momentum spectrometer, to study the ultrafast dynamics and reactions in atomic and molecular systems. The last beamline produces broadband attosecond XUV pulses designed for time-resolved photoemission electron microscopy, to study the ultrafast dynamics of plasmons in nanostructures and the surfaces of solid materials with high temporal and spatial resolutions simultaneously. The main object of the ALS is to provide domestic and international scientists with unique tools to study fundamental processes in physics, chemistry, biology, and material sciences with ultrafast temporal resolutions on the atomic scale.展开更多
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 o...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.展开更多
We investigate the ionization dynamics of atoms by chirped attosecond pulses using the strong field approximation method. The pulse parameters are carefully chosen in the regime where the strong field approximation me...We investigate the ionization dynamics of atoms by chirped attosecond pulses using the strong field approximation method. The pulse parameters are carefully chosen in the regime where the strong field approximation method is valid. We analyse the effects of the chirp of attosecond pulses on the energy distributions and the corresponding left-right asymmetry of the ionized electrons. For a single chirped attosecond pulse, the ionized electrons can be redistributed and the left-right asymmetry shows oscillations because of the introduction of the chirp. For time-delayed double attosecond pulses at different intensities with the weaker one chirped, exchanging the order of the two pulses shows a relative shift of the energy spectra, which can be explained by the different effective time delays of different frequency components because of the chirp.展开更多
We present photoelectron angular distribution of the aligned molecular ion H2^＋ by intense ultrashort attosecond extreme ultraviolet laser pulses from numerical solutions of timedependent Schrodinger equations. Photo...We present photoelectron angular distribution of the aligned molecular ion H2^＋ by intense ultrashort attosecond extreme ultraviolet laser pulses from numerical solutions of timedependent Schrodinger equations. Photoionization from a superposition state of the ground 1sσg and the excited 2pσu states with pulses at photon energies above the ionization potential, hω〉Ip, and intensity 10^14 W/cm^2, yields pulse duration dependent asymmetry of photoelectron angular distributions. We attribute the asymmetry to the periodical oscillation of the coherent electron wave packets, resulting from the interference of the two electronic states. For the processes with long pulse durations, such duration dependence is absent and symmetric angular distributions are obtained.展开更多
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...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）.展开更多
We theoretically investigate high-order harmonic generation（HHG） from a helium ion model in a two-color laser field,which is synthesized by a fundamental pulse and its second harmonic pulse.It is shown that a superc...We theoretically investigate high-order harmonic generation（HHG） from a helium ion model in a two-color laser field,which is synthesized by a fundamental pulse and its second harmonic pulse.It is shown that a supercontinuum spectrum can be generated in the two-color field.However,the spectral intensity is very low,limiting the application of the generated attosecond（as） pulse.By adding a static electric field to the synthesized two-color field,not only is the ionization yield of electrons contributing to the harmonic emission remarkably increased,but also the quantum paths of the HHG can be significantly modulated.As a result,the extension and enhancement of the supercontinuum spectrum are achieved,producing an intense isolated 26-as pulse with a bandwidth of about 170.5 eV.In particular,we also analyse the influence of the laser parameters on the ultrabroad supercontinuum spectrum and isolated sub-30-as pulse generation.展开更多
We theoretically investigate the high-order harmonic generation(HHG) of helium atom driven by bichromatic counterrotating circularly polarized laser fields. By changing the intensity ratio of the two driving laser fie...We theoretically investigate the high-order harmonic generation(HHG) of helium atom driven by bichromatic counterrotating circularly polarized laser fields. By changing the intensity ratio of the two driving laser fields, the spectral chirality of the HHG can be controlled. As the intensity ratio increases, the spectral chirality will change from positive-to negativevalue around a large intensity ratio of the two driving fields when the total laser intensity keeps unchanged. However, the sign of the spectral chirality can be changed from positive to negative around a small intensity ratio of the two driving fields when the total laser intensity changes. At this time, we can effectively control the helicity of the harmonic spectrum and the polarization of the resulting attosecond pulses by adjusting the intensity ratio of the two driving laser fields. As the intensity ratio and the total intensity of the driving laser fields increase, the relative intensity of either the left-circularly or right-circularly polarized harmonic can be enhanced. The attosecond pulses can evolve from being elliptical to near linear correspondingly.展开更多
We present a theoretical investigation of high-order harmonic generation in a chirped two-color laser field, which is synthesized by a 10-fs/800-nm fundamental chirped pulse and a 10-fs/1760-nm subharmonic pulse. It i...We present a theoretical investigation of high-order harmonic generation in a chirped two-color laser field, which is synthesized by a 10-fs/800-nm fundamental chirped pulse and a 10-fs/1760-nm subharmonic pulse. It is shown that a supercontinuum can be produced using the multicycle two-color chirped field. However, the supercontinuum reveals a strong modulation structure, which is not good for the generation of an isolated attosecond pulse. By adding a static electric field to the multicycle two-color chirped field, not only the harmonic cutoff is extended remarkably, but also the quantum paths of the high-order harmonic generation （HHG） are modified significantly. As a result, both the extension of the supercontinuum and the selection of a single quantum path are achieved, producing an isolated 23-as pulse with a bandwidth of about 170.6 eV. Furthermore, the influences of the laser intensities on the supercontinuum and isolated attosecond pulse generation are investigated.展开更多
As a crucial parameter for a few-cycle laser pulse, the carrier envelope phase(CEP) substantially determines the laser waveform. We propose a method to directly describe the CEP of an isolated attosecond pulse(IAP) by...As a crucial parameter for a few-cycle laser pulse, the carrier envelope phase(CEP) substantially determines the laser waveform. We propose a method to directly describe the CEP of an isolated attosecond pulse(IAP) by the vortex-shaped momentum pattern, which is generated from the tunneling ionization of a hydrogen atom by a pair of time-delayed, oppositely and circularly polarized IAP-IR pulses. Superior to the angular streaking method that characterizes the CEP in terms of only one streak, our method describes the CEP of an IAP by the features of multiple streaks in the vortex pattern. The proposed method may open the possibility of capturing sub-cycle extreme ultraviolet dynamics.展开更多
In this paper, we theoretically investigate the high-order harmonic generation and attosecond pulse generation when a two-electron He atom is exposed to the intense laser pulse. It shows that due to the two-electron d...In this paper, we theoretically investigate the high-order harmonic generation and attosecond pulse generation when a two-electron He atom is exposed to the intense laser pulse. It shows that due to the two-electron double recombination mechanism, an extended plateau beyond the classical single-electron harmonic has been obtained on the two-electron harmonic spectrum. Further by using this two-electron harmonic extension scheme combined with the two-color field, two supercontinuum bandwidths with 200 e V have been obtained. As a result, a series of sub-60 as extreme ultraviolet（XUV）pulses have been directly generated.展开更多
In this paper, we theoretically investigate the effect of noise on the photoionization, the generation of the high-order harmonic and the attosecond pulse irradiated from a model He＋ ion. It shows that by properly ad...In this paper, we theoretically investigate the effect of noise on the photoionization, the generation of the high-order harmonic and the attosecond pulse irradiated from a model He＋ ion. It shows that by properly adding noise fields, such as Gaussian white noise, random light or colored noise, both the ionization probabilities （IPs） and the harmonic yields can be enhanced by several orders of magnitude. Further, by tuning the noise intensity, a stochastic resonance-like curve is observed, showing the existence of an optimal noise in the ionization enhancement process. Finally, by superposing a properly selected harmonic, an intense attosecond pulse with a duration of 67 as is directly generated.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.12174435,12034020,and 92250303)the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-091)the National Key R&D Program of China(Grant No.2022YFA1604200).
文摘Attosecond light pulses have revolutionized the study of electron dynamics in materials by enabling the observation of ultrafast processes with unprecedented attosecond temporal resolution.They are primarily generated through the process of high-order harmonic generation.This paper presents a comprehensive setup for attosecond pulse generation and measurement.Using a 900 nm,7 mJ,and 7 fs femtosecond laser with stabilized carrier-envelope phase,we employ polarization gating to generate a near single-cycle,linearly polarized pulse that interacts with neon gas to produce a broadband extreme-ultraviolet continuum with a cutoff photon energy of∼120 eV.The temporal and spectral characteristics of the generated single attosecond pulses are measured using an attosecond streak camera,and the pulse duration is determined to be 59 as through the frequency-resolved optical gating for complete reconstruction of attosecond bursts retrieval algorithm.As part of the Synergetic Extreme Condition User Facility,this setup will facilitate ultrafast research in transient absorption and photoelectron spectroscopy,providing global users with a powerful tool for studying electron dynamics in various materials.
基金Project supported by the National Natural Science Foundation of China(Grant No.12174034)。
文摘This review comprehensively explores the theory and applications of attosecond transient absorption spectroscopy(ATAS)in studying ultrafast electronic dynamics across various systems,from atoms to solids.Driven by significant advancements in ultrafast laser technology,such as generating isolated attosecond pulses,ATAS enables detailed investigations of ultrafast electronic processes with unprecedented time resolution.The article introduces the fundamental principles and historical development of ATAS.Applications of ATAS are discussed in three main domains:in atoms,where it has been used to study build-up dynamics of Autler–Townes splitting,Fano resonance,light-induced states,etc.;in molecules,where it has revealed coherent molecular wavepacket dynamics and non-adiabatic dynamics near conical intersections;and in solids,where it has been extended to investigate ultrafast charge carrier dynamics in metals,semiconductors,and insulators.The review highlights the potential of ATAS in developing ultrafast optical switches and petahertz electronics.The ability of ATAS to probe and manipulate electronic dynamics at the attosecond timescale provides a powerful tool for exploring the fundamental limits of electronic and optical processes in materials.
基金supported by the Natural Science Foundation of Jilin Province under Grant No. 20220101028JC。
文摘A mid-infrared femtosecond pulse laser with a single cycle and high intensity is an ideal driving light source for generating isolated attosecond pulses. Due to current experimental limitations, it is difficult to directly achieve this type of laser light source in the laboratory. In this paper, we obtain such an ideal light source by adding a Ti sapphire pulse to the combined pulse laser consisting of two mid-infrared pulses. Specifically, by combining the synthesized pulse consisting of 8 fs/1200 nm/1.62 × 10^(14)W cm^(-2)and 12 fs/1800 nm/2.71 × 10^(14)W cm^(-2)with an additional 8 fs/800 nm/1.26 × 10^(14)W cm^(-2)Ti sapphire pulse, the resulting electric field waveform is very close to that of a 1170 nm femtosecond pulse with an intensity of 1.4 × 10^(15)W cm^(-2), a single-cycle pulse width, and a carrier-envelope phase of 0.25π. Numerical simulations show that both cases produce high-order harmonic emission spectra with broadband supercontinuum spectra, however, the bandwidth of the supercontinuum spectra and the harmonic intensities in the synthesized pulses are significantly better than those in the single1170 nm pulse. After inverse Fourier transform, we obtain 66 as a high-intensity isolated attosecond pulse, whose intensity is five orders of magnitude higher than that of a monochromatic field. Here, the phase differences between three combined pulse lasers have little effect on the numerical simulation results when they vary in the range of 0.3π.
基金Project supported by the National Natural Science Foundation of China (Grant No. 12274230)the Funding of Nanjing University of Science and Technology (Grant No. TSXK2022D005)。
文摘The attosecond extreme ultraviolet(XUV) pulse pump and femtosecond infrared(IR) pulse probe scheme is commonly used to study the dynamics and attosecond transient absorption(ATA) spectra of microscopic systems. In a recent report [Proc. Natl. Acad. Sci. USA 121 e2307836121(2024)], we showed that shaped XUV pulses with spectral minima can significantly alter the absorption line shape of helium's 2s2p doubly excited state within a few tens of attoseconds.However, it remains unclear if similar effects could be observed in a singly excited state. In this study, we use shaped XUV pulses to excite helium's 2p singly excited state and couple the 2p and 3d states with a delayed IR pulse. Comparing these results with those from Gaussian XUV pulses, we find that the ATA spectra for the shaped XUV pulses exhibit more pronounced changes with delay, while the changes for the Gaussian pulses are gradual. We also explain these differences through population changes and analytical models. Our findings show that shaped XUV pulses can regulate the dynamics and absorption spectra of a singly excited state.
基金supported by the National Natural Science Foundation of China(Grant Nos.W2411002 and 12375018).
文摘We introduce a time-dependent generalized Floquet(TDGF)approach to calculate attosecond transient absorption spectra of helium atoms subjected to the combination of an attosecond extreme ultraviolet(XUV)pulse and a delayed few-cycle infrared(IR)laser pulse.This TDGF approach provides a Floquet understanding of the laser-induced change of resonant absorption lineshape.It is analytically demonstrated that the phase shift of the time-dependent dipole moment that results in the lineshape changes consists of two components,the adiabatic laser-induced phase(LIP)due to the IR-induced Stark shifts of adiabatic Floquet states and the non-adiabatic phase correction due to the non-adiabatic IR-induced coupling between adiabatic Floquet states.Comparisons of the spectral lineshape calculated based on the TDGF approach with the results obtained with the LIP model[Phys.Rev.A 88033409(2013)]and the rotating-wave approximation(RWA)are presented for several typical cases,demonstrating that TDGF universally and accurately captures IR-induced lineshape changes.It is suggested that the LIP model works as long as the generalized adiabatic theorem[PRX Quantum 2030302(2021)]holds,and the RWA works when the higher-order IR-coupling effect in the formation of adiabatic Floquet states is neglectable.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.92150105,11834004,12227807,and 12241407)the Science and Technology Commission of Shanghai Municipality (Grant No.21ZR1420100)。
文摘Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.
基金Project supported by the National Natural Science Foundation of China(Grant No.10774054)the National Key Basic Research Special Foundation of China(NKBRSFC)(Grant No.2006CB806006)
文摘We theoretically investigate the high-order harmonic generation from stretched molecules in a linearly polarized intense field. By adopting an infrared pulse combined with an ultraviolet （UV） attosecond pulse, the ionization process can be controlled effectively. In this excitation scheme, the harmonic spectrum beyond Ip ＋ 3.17Up is significantly enhanced by two orders, where Ip and Up = e^2E0^2/（4mew^2） are the ionization and ponderomotive potential, then smooth broadband supercontinuum with the bandwidth of about 120 eV is obtained, which leads to an isolated sub-60- as attosecond pulse with a high signal-noise ratio. Moreover, the bandwidth of the supercontinuum is weakly dependent on the location and pulse duration of the UV pulse.
基金Project supported by the National Key R&D Program of China(Grant No.2017YFB0405202)the Major Program of the National Natural Science Foundation of China(Grant No.61690221)+1 种基金the Key Program of the National Natural Science Foundation of China(Grant No.11434016)the National Natural Science Foundation of China(Grant Nos.11574384,11674386,and 11774277)
文摘We utilized a set of fused silica thin plates to broaden the spectrum of 1kHz,30 fs Ti:sapphire amplified laser pulses to an octave.Following the compression by chirped mirror pairs,the generated few-cycle pulses were focused onto an argon filled gas cell.We detected high order harmonics corresponding to a train of 209 as pulses,characterized by the reconstruction of attosecond beating by interference of two-photon transition(RABITT)technique.Compared with the conventional attosecond pulse trains,the broad harmonics in such pulse trains cover more energy range,so it is more efficient in studying some typical cases,such as resonances,with frequency resolved RABITT.As the solid thin plates can support high power supercontinuum generation,it is feasible to tailor the spectrum to have different central wavelength and spectral width,which will make the RABITT source work in different applications.
基金supported by the National Natural Science Foundation of China(Grants Nos.11404153,11175076,11135002,and 11405077)the Fundamental Research Funds for the Central Universities of China(Grant Nos.lzujbky-2014-10,lzujbky-2014-13,and lzujbky-2014-14)
文摘We theoretically investigate high-order harmonic generation in a two-color multi-cycle inhomogeneous field combined with a 27th harmonic pulse. By considering a bowtie-shaped gold nanostructure, the spatiotemporal profiles of enhanced plasmonic fields are obtained by solving the Maxwell equation using finite-domain time-difference method. Based on quantum-mechanical and classical models, the effect of 27th harmonic pulse, temporal profile of enhanced plasmonic field and inhomogeneity on supercontinuum generation are analyzed and discussed. As a result, broadband supercontinuum can be generated from our approach with optimized gap size of nanostructure. Moreover, these results are not sensitively dependent on the relative phase in the two-color field.
基金Project supported by the National Key R&D Program of China(Grant Nos.2018YFB1107200,2017YFC0110301,and 2017YFB0405202)Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0703030)the National Natural Science Foundation of China(Grant Nos.11474002,11674386,61575219,and 61690221)
文摘The attosecond laser station （ALS） at the Synergetic Extreme Condition User Facility （SECUF） is a sophisticated and user-friendly platform for the investigation of the electron dynamics in atoms, molecules, and condensed matter on timescales ranging from tens of femtoseconds to tens of attoseconds. Short and tunable coherent extreme-ultraviolet （XUV） light sources based on high-order harmonic generation in atomic gases are being developed to drive a variety of endstations for inspecting and controlling ultrafast electron dynamics in real time. The combination of such light sources and end-stations offers a route to investigate fundamental physical processes in atoms, molecules, and condensed matter. The ALS consists of four beamlines, each containing a light source designed specifically for application experiments that will be performed in its own end-station. The first beamline will produce broadband XUV light for attosecond photoelectron spectroscopy and attosecond transient absorption spectroscopy. It is also capable of performing attosecond streaking to characterize isolated attosecond pulses and will allow studies on the electron dynamics in atoms, moleculars, and condensed matter. The second XUV beamline will produce narrowband femtoseeond XUV pulses for time-resolved and angle-resolved photoelectron spectroscopy, to study the electronic dynamics on the timescale of fundamental correlations and interactions in solids, especially in superconductors and topological insulators. The third beamline will produce broadband XUV pulses for attosecond coincidence spectroscopy in a cold-target recoil-ion momentum spectrometer, to study the ultrafast dynamics and reactions in atomic and molecular systems. The last beamline produces broadband attosecond XUV pulses designed for time-resolved photoemission electron microscopy, to study the ultrafast dynamics of plasmons in nanostructures and the surfaces of solid materials with high temporal and spatial resolutions simultaneously. The main object of the ALS is to provide domestic and international scientists with unique tools to study fundamental processes in physics, chemistry, biology, and material sciences with ultrafast temporal resolutions on the atomic scale.
基金supported by the National Natural Science Foundation of China (Grant No.10974068)
文摘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.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 10704003 and 10821062)the National Basic Research Program of China (Grant No 2006CB806007)
文摘We investigate the ionization dynamics of atoms by chirped attosecond pulses using the strong field approximation method. The pulse parameters are carefully chosen in the regime where the strong field approximation method is valid. We analyse the effects of the chirp of attosecond pulses on the energy distributions and the corresponding left-right asymmetry of the ionized electrons. For a single chirped attosecond pulse, the ionized electrons can be redistributed and the left-right asymmetry shows oscillations because of the introduction of the chirp. For time-delayed double attosecond pulses at different intensities with the weaker one chirped, exchanging the order of the two pulses shows a relative shift of the energy spectra, which can be explained by the different effective time delays of different frequency components because of the chirp.
基金This work was supported by the National Natural Science Foundation of China （No.21222308, No.21103187, and No.21133006）, the Chinese Academy of Sciences, and the National Basic Research Program of China （No. 2013CB922200）.
文摘We present photoelectron angular distribution of the aligned molecular ion H2^＋ by intense ultrashort attosecond extreme ultraviolet laser pulses from numerical solutions of timedependent Schrodinger equations. Photoionization from a superposition state of the ground 1sσg and the excited 2pσu states with pulses at photon energies above the ionization potential, hω〉Ip, and intensity 10^14 W/cm^2, yields pulse duration dependent asymmetry of photoelectron angular distributions. We attribute the asymmetry to the periodical oscillation of the coherent electron wave packets, resulting from the interference of the two electronic states. For the processes with long pulse durations, such duration dependence is absent and symmetric angular distributions are obtained.
基金supported by the National Natural Science Foundation of China(Grant Nos.11174108,11104108,and 11271158)
文摘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）.
基金Project supported by the Science Foundation of Baoji University of Arts and Sciences,China (Grant Nos. ZK10122,ZK11061,ZK11135,ZK11060,and ZK1032)the Education Committee Natural Science Foundation of Shaanxi Province,China (GrantNo. 2010JK405)
文摘We theoretically investigate high-order harmonic generation（HHG） from a helium ion model in a two-color laser field,which is synthesized by a fundamental pulse and its second harmonic pulse.It is shown that a supercontinuum spectrum can be generated in the two-color field.However,the spectral intensity is very low,limiting the application of the generated attosecond（as） pulse.By adding a static electric field to the synthesized two-color field,not only is the ionization yield of electrons contributing to the harmonic emission remarkably increased,but also the quantum paths of the HHG can be significantly modulated.As a result,the extension and enhancement of the supercontinuum spectrum are achieved,producing an intense isolated 26-as pulse with a bandwidth of about 170.5 eV.In particular,we also analyse the influence of the laser parameters on the ultrabroad supercontinuum spectrum and isolated sub-30-as pulse generation.
基金Project supported by the National Natural Science Foundation of China(Grant No.61575077)the Natural Science Foundation of Jilin Province of China(Grant No.20180101225JC)+1 种基金the China Postdoctoral Science Foundation(Grants Nos.2018M641766 and 2019T120232)the Graduate Innovation Fund of Jilin University,China(Grant No.101832018C105)
文摘We theoretically investigate the high-order harmonic generation(HHG) of helium atom driven by bichromatic counterrotating circularly polarized laser fields. By changing the intensity ratio of the two driving laser fields, the spectral chirality of the HHG can be controlled. As the intensity ratio increases, the spectral chirality will change from positive-to negativevalue around a large intensity ratio of the two driving fields when the total laser intensity keeps unchanged. However, the sign of the spectral chirality can be changed from positive to negative around a small intensity ratio of the two driving fields when the total laser intensity changes. At this time, we can effectively control the helicity of the harmonic spectrum and the polarization of the resulting attosecond pulses by adjusting the intensity ratio of the two driving laser fields. As the intensity ratio and the total intensity of the driving laser fields increase, the relative intensity of either the left-circularly or right-circularly polarized harmonic can be enhanced. The attosecond pulses can evolve from being elliptical to near linear correspondingly.
基金Project supported by the Science Foundation of Baoji University of Arts and Sciences,China(Grant No.ZK11061)the Natural Science Foundation of Education Committee of Shaanxi Province,China(Grant No.2013JK0637)
文摘We present a theoretical investigation of high-order harmonic generation in a chirped two-color laser field, which is synthesized by a 10-fs/800-nm fundamental chirped pulse and a 10-fs/1760-nm subharmonic pulse. It is shown that a supercontinuum can be produced using the multicycle two-color chirped field. However, the supercontinuum reveals a strong modulation structure, which is not good for the generation of an isolated attosecond pulse. By adding a static electric field to the multicycle two-color chirped field, not only the harmonic cutoff is extended remarkably, but also the quantum paths of the high-order harmonic generation （HHG） are modified significantly. As a result, both the extension of the supercontinuum and the selection of a single quantum path are achieved, producing an isolated 23-as pulse with a bandwidth of about 170.6 eV. Furthermore, the influences of the laser intensities on the supercontinuum and isolated attosecond pulse generation are investigated.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11674243 and 11674242
文摘As a crucial parameter for a few-cycle laser pulse, the carrier envelope phase(CEP) substantially determines the laser waveform. We propose a method to directly describe the CEP of an isolated attosecond pulse(IAP) by the vortex-shaped momentum pattern, which is generated from the tunneling ionization of a hydrogen atom by a pair of time-delayed, oppositely and circularly polarized IAP-IR pulses. Superior to the angular streaking method that characterizes the CEP in terms of only one streak, our method describes the CEP of an IAP by the features of multiple streaks in the vortex pattern. The proposed method may open the possibility of capturing sub-cycle extreme ultraviolet dynamics.
基金supported by the Scientific Research Fund of Liaoning Provincial Education Department,China(No.L2014242)the Scientific Research Fund of Liaoning University of Technology,China(Grant Nos.X201319 and X201312)
文摘In this paper, we theoretically investigate the high-order harmonic generation and attosecond pulse generation when a two-electron He atom is exposed to the intense laser pulse. It shows that due to the two-electron double recombination mechanism, an extended plateau beyond the classical single-electron harmonic has been obtained on the two-electron harmonic spectrum. Further by using this two-electron harmonic extension scheme combined with the two-color field, two supercontinuum bandwidths with 200 e V have been obtained. As a result, a series of sub-60 as extreme ultraviolet（XUV）pulses have been directly generated.
基金Project supported by the National Natural Science Foundations of China(Grant Nos.10874096 and 20633070)
文摘In this paper, we theoretically investigate the effect of noise on the photoionization, the generation of the high-order harmonic and the attosecond pulse irradiated from a model He＋ ion. It shows that by properly adding noise fields, such as Gaussian white noise, random light or colored noise, both the ionization probabilities （IPs） and the harmonic yields can be enhanced by several orders of magnitude. Further, by tuning the noise intensity, a stochastic resonance-like curve is observed, showing the existence of an optimal noise in the ionization enhancement process. Finally, by superposing a properly selected harmonic, an intense attosecond pulse with a duration of 67 as is directly generated.
