XUV Pulses Research Articles

Production of intense isolated attosecond pulses with circular polarization by using counter-propagating relativistic lasers

We demonstrate theoretically and numerically that intense isolated circularly polarized (CP) attosecond pulses can be generated from ultrathin foil targets irradiated by two relativistic lasers from opposite sides, where their polarizations are orthogonal to each other. With a proper matching condition, the compressed oscillating plasma mirrors on both sides of the foil are pushed inside by laser radiation pressures, eventually merging together to form a dense electron nanobunch under the effect of orthogonal laser fields. This nanobunch reaches both high density and high energy in only half a laser cycle and smears out in others, resulting in coherent synchrotron emission of a single attosecond pulse with circular polarization. Two-dimensional particle-in-cell simulations show that an intense isolated CP attosecond XUV pulse with an intensity of 1.2 × 1019 W cm−2 and a duration of ∼75 as can be obtained by two lasers with the same intensity of 2.1 × 1020 W cm−2.

Response of free-standing graphene monolayer exposed to ultrashort intense XUV pulse from free-electron laser.

The response of a free-standing graphene monolayer exposed to a few tens of femtoseconds long extreme ultraviolet (XUV) pulse was studied theoretically in order to analyze and compare contributions of various mechanisms to the graphene damage, understood here as a global atomic disintegration. Our simulation results indicate that nonthermal disintegration of the atomic structure is the predominant damage mechanism for a free-standing graphene layer. Only at high absorbed doses, charge-induced disintegration of the graphene structure prevails. We also demonstrate that the progressing damage can be probed by femtosecond optical pulses in the soft UV regime (4eV photon energy). The achieved quantitative understanding of the damage mechanisms may enable a better control of graphene-based devices when they are exposed to x-ray radiation, as well as an efficient processing of graphene layers with ultrashort intense XUV pulses.

Coherent Control of High Harmonic Generation Driven by Metal Nanotip PhotoemissionSupported by the National Key Research and Development Program of China (Grant Nos. 2019YFA0307700 and 2016YFA0401100), the National Natural Science Foundation of China (Grant Nos. 11774215, 11674209, 91950101, 11947243, 11334009, 11425414, and 11947080), Sino-German Mobility Programme (Grant No. M-0031), Department of Education of Guangdong Province (Grant No. 2018KCXTD011), High Level

Steering ultrafast electron dynamics with well-controlled laser fields is very important for generation of intense supercontinuum radiation. It can be achieved through coherent control of the symmetry of the interaction between strong-field laser fields and a metal nanotip. We employ a scheme of two-color laser pulses combined with a weak static field to realize the control of a single quantum path to generate high harmonic generation from a single solid-state nanoemitter. Moreover, a smooth and ultrabroad supercontinuum in the extreme ultraviolet region is obtained, which can produce a single attosecond pulse. Our findings are beneficial for efficient generation of isolated sub-100 as XUV pulses from solid-state sources.

Probing ultrafast coherent dynamics in core-excited xenon by using attosecond XUV-NIR transient absorption spectroscopy

We investigate the capability of attosecond transient absorption spectroscopy to characterize the dynamics of inner-shell-excited systems. In the transient absorption spectroscopy setup considered, wave packets are prepared by an attosecond XUV pulse and probed by a femtosecond NIR pulse. By using this, we study coherent electron dynamics in core-excited xenon atoms. In particular, we clarify which aspects of the dynamics can be revealed when the wave packets are probed using an NIR pulse and analyze why the inner-shell hole dynamics is more difficult to probe than the dynamics of the excited electron. We perform a theoretical analysis of the transient absorption signal as a function of the time delay between the XUV pump and NIR probe pulses, treating the excitation pulse perturbatively and the probe pulse nonperturbatively. We also demonstrate that an additional NIR dressing field can dramatically influence the transient absorption spectrum. Our theoretical predictions are compared with experimental results, suggesting that a precise characterization of the NIR pulse is necessary for a qualitative and quantitative comparison.

Extreme ultraviolet photon effect on ionization and recombination of high-order harmonic generation

The extreme ultraviolet (XUV) pulse effect on the ionization and recombination of the high-order harmonic generation has been theoretically studied. It is shown that (i) with the introduction of a shorter duration XUV pulse to a fundamental infrared (IR) pulse, the XUV photon can only be absorbed during the electron ionization process. Thus, the harmonic signal can be enhanced due to the XUV resonance transition and ionization. (ii) With the introduction of a longer-duration XUV pulse to a fundamental IR pulse, the XUV photon can be absorbed not only in the electron ionization process, but also in the electron recombination process. As a result, not only the harmonic signal can be improved, but also the harmonic cutoff can be extended with an additional XUV photon energy region (. Moreover, as the XUV intensity increases, much more XUV photons can be absorbed in the electron recombination process, thus leading to the harmonic cutoff extension with the extra photon energy region of .

Study of temporal, spectral, arrival time and energy fluctuations of SASE FEL pulses.

Self-amplified spontaneous emission (SASE) pulses delivered by free electron lasers (FELs) are inherently fluctuating sources; each pulse varies in energy, duration, arrival time and spectral shape. Therefore, there is strong demand for a full characterization of the properties of SASE radiation, which will facilitate more precise interpretation of the experimental data taken at SASE FELs. In this paper, we present an investigation into the fluctuations of pulse duration, spectral distribution, arrival time and pulse energy of SASE XUV pulses at FLASH, both on a shot-to-shot basis and on average over many pulses. With the aid of simulations, we derived scaling laws for these parameters and disentangled the statistical SASE fluctuations from accelerator-based fluctuations and measurement uncertainties.

Comparative study of photoionization of atomic hydrogen by solving the one- and three-dimensional time-dependent Schrödinger equations* *Project supported by the National Natural Science Foundation of China (Gant Nos. 12074265, 11804233, and 11575118), the National Key Research and Development Project of China (Grant No. 2017YFF0106500), the Natural Science Foundation of Guangdong, China (Grant Nos. 2018A0303130311 and 2021A1515010082), and the Shenzhen Fundamental

We develop a numerical scheme for solving the one-dimensional (1D) time-dependent Schrödinger equation (TDSE), and use it to study the strong-field photoionization of the atomic hydrogen. The photoelectron energy spectra obtained for pulses ranging from XUV to near infrared are compared in detail to the spectra calculated with our well-developed code for accurately solving the three-dimensional (3D) TDSE. For XUV pulses, our discussions cover intensities at which the ionization is in the perturbative and nonperturbative regimes. For pulses of 400 nm or longer wavelengths, we distinguish the multiphoton and tunneling regimes. Similarities and discrepancies between the 1D and 3D calculations in each regime are discussed. The observed discrepancies mainly originate from the differences in the transition matrix elements and the energy level structures created in the 1D and 3D calculations.

Extreme-ultraviolet spectral compression by four-wave mixing

Extreme-ultraviolet (XUV) sources including high-harmonic generation (HHG), free-electron lasers (FELs), soft-X-ray lasers and laser-driven plasmas are widely used for applications ranging from femtochemistry and attosecond science to coherent diffractive imaging and EUV (or XUV) lithography. The bandwidth of the XUV light emitted by these sources reflects the XUV generation process used. Whereas light from soft-X-ray lasers1 and seeded XUV FELs2 typically has a relatively narrow bandwidth, plasma sources and HHG sources often emit broadband XUV pulses3. Since these characteristic properties of a given source impose limitations on applications, techniques enabling modification of the bandwidth are highly desirable. Here we introduce a concept for efficient spectral compression by four-wave mixing (FWM), exploiting a phase-matching scheme based on closely-spaced resonances. We demonstrate the compression of broadband radiation in the 145–130 nm wavelength range into a narrow-bandwidth XUV pulse at 100.3 nm wavelength in the presence of a broadband near-infrared (NIR) pulse in a krypton gas jet. Our concept provides new possibilities for tailoring the spectral bandwidth of XUV beams.

Time-frequency analysis of high harmonic generation using a probe XUV pulse.

Interpretation of strong-field phenomena is mostly based on the analysis of classical electron trajectories in an intense laser field, whose specific properties determine general features of nonlinear laser-matter interaction. Currently, the visualization of closed electron trajectories contributing to high harmonic generation (HHG) of the laser field is the prerogative of a theoretical analysis based on the time-frequency spectrogram of the induced dipole acceleration. Here, we propose a method for direct reconstruction of the HHG time-frequency spectrogram using a time-delayed probe XUV pulse. Our analytical theory and ab initio numerical simulations demonstrate that the XUV-assisted HHG yield as a function of time delay and harmonic energy mimics the short-time Fourier transform of the dipole acceleration induced by the laser field, thereby providing possible in-situ experimental access for tracing electron dynamics in strong-field phenomena.

Time-energy analysis of the photoionization process in a double-XUV pulse combined with a few-cycle IR field

We calculate the time-energy distribution (TED) and ionization time distribution (ITD) of photoelectrons emitted by a double-extreme-ultraviolet (XUV) pulse and a two-color XUV-IR pulse using the Wigner distribution-like function based on the strong field approximation. For a double-XUV pulse, besides two identical broad distributions generated by two XUV pulses, many interference fringes resulting from the interference between electrons generated, respectively, by two pulses appear in the TED. After adding an IR field, the TED intuitively exhibits the effect of the IR field on the electron dynamics. The ITDs during two XUV pulses are no longer the same and show the different changes for the different two-color fields, the origin of which is attributed to the change of the electric field induced by the IR field. Our analysis shows that the emission time of electrons ionized during two XUV pulses mainly depends on the electric field of the combined XUV pulse and IR pulse.

Molecular fragmentation as a way to reveal early electron dynamics induced by attosecond pulses.

We present a theoretical study of the electron and nuclear dynamics that would arise in an attosecond two-color XUV-pump/XUV-probe experiment in glycine. In this scheme, the broadband pump pulse suddenly ionizes the molecule and creates an electronic wave packet that subsequently evolves under the influence of the nuclear motion until it is finally probed by the second XUV pulse. To describe the different steps of such an experiment, we have combined a multi-reference static-exchange scattering method with a trajectory surface hopping approach. We show that by changing the central frequency of the pump pulse, i.e., by engineering the initial electronic wave packet with the pump pulse, one can drive the cation dynamics into a specific fragmentation pathway. Reminiscence of this early electron dynamics can be observed in specific fragmentation channels (not all of them) as a function of the pump-probe delay and in time-resolved photoelectron spectra at specific photoelectron energies. The optimum conditions to visualize the initial electronic coherence in photoelectron and photo-ion spectra depend very much on the characteristics of the pump pulse as well as on the electronic structure of the molecule under study.

Pump-Probe Delay Controlled by Laser-dressed Ionization with Isolated Attosecond Pulses

In a recent work [1], we demonstrated how laser-dressed ionization can be harnessed to control with attosecond accuracy the time delay between an extreme-ultraviolet (XUV) attosecond pulse train and an infrared (IR) femtosecond pulse. In this case, the comb-like photoelectron spectrum obtained by ionizing a gas target with the two superimposed beams exhibits peaks oscillating with the delay. Two of them can be found to oscillate in phase quadrature, allowing an optimal measurement and stabilization of the delay over a large range. Here we expand this technique to isolated attosecond pulses, by taking advantage of the delay-modulation of attosecond streaking traces. Although the photoelectron spectrum contains no peaks in that case, it is possible to reconstruct the pump-probe delay by simply monitoring the mean energy of the spectrum and the amplitude at this energy. In general, we find that active delay stabilization based on laser-dressed ionization is possible as long as the XUV pulses are chirped.

Multi-channel photodissociation and XUV-induced charge transfer dynamics in strong-field-ionized methyl iodide studied with time-resolved recoil-frame covariance imaging.

The photodissociation dynamics of strong-field ionized methyl iodide (CH3I) were probed using intense extreme ultraviolet (XUV) radiation produced by the SPring-8 Angstrom Compact free electron LAser (SACLA). Strong-field ionization and subsequent fragmentation of CH3I was initiated by an intense femtosecond infrared (IR) pulse. The ensuing fragmentation and charge transfer processes following multiple ionization by the XUV pulse at a range of pump-probe delays were followed in a multi-mass ion velocity-map imaging (VMI) experiment. Simultaneous imaging of a wide range of resultant ions allowed for additional insight into the complex dynamics by elucidating correlations between the momenta of different fragment ions using time-resolved recoil-frame covariance imaging analysis. The comprehensive picture of the photodynamics that can be extracted provides promising evidence that the techniques described here could be applied to study ultrafast photochemistry in a range of molecular systems at high count rates using state-of-the-art advanced light sources.

Coupled nuclear-electronic decay dynamics of O2 inner valence excited states revealed by attosecond XUV wave-mixing spectroscopy.

Multiple Rydberg series converging to the O2+c4Σ-u state, accessed by 20-25 eV extreme ultraviolet (XUV) light, serve as important model systems for the competition between nuclear dissociation and electronic autoionization. The dynamics of the lowest member of these series, the 3sσg state around 21 eV, has been challenging to study owing to its ultra-short lifetime (<10 fs). Here, we apply transient wave-mixing spectroscopy with an attosecond XUV pulse to investigate the decay dynamics of this electronic state. Lifetimes of 5.8 ± 0.5 fs and 4.5 ± 0.7 fs at 95% confidence intervals are obtained for v = 0 and v = 1 vibrational levels of the 3s Rydberg state, respectively. A theoretical treatment of predissociation and electronic autoionization finds that these lifetimes are dominated by electronic autoionization. The strong dependence of the electronic autoionization rate on the internuclear distance because of two ionic decay channels that cross the 3s Rydberg state results in the different lifetimes of the two vibrational levels. The calculated lifetimes are highly sensitive to the location of the 3s potential with respect to the decay channels; by slight adjustment of the location, values of 6.2 and 5.0 fs are obtained computationally for the v = 0 and v = 1 levels, respectively, in good agreement with experiment. Overall, an intriguing picture of the coupled nuclear-electronic dynamics is revealed by attosecond XUV wave-mixing spectroscopy, indicating that the decay dynamics are not a simple competition between isolated autoionization and predissociation processes.

Reconstruction of few-fs XUV pulses with a perturbative approach

A precise temporal characterization of the pulses involved in pump-probe experiments is crucial for a proper investigation of the ultrafast dynamics in several physical systems. Indeed, it is required for the assessment of the dynamical properties under examination with sufficient temporal resolution. In the fewfs/attosecond domain, typical reconstruction procedures require time-consuming interative methods, which are also sensitive to the experimental noise and to the distortion of the measurement. We developed an approach, called Simplified Trace Reconstruction In the Perturbative regimE (STRIPE), which allows us for a precise characterization of the infrared (IR) and extreme ultraviolet (XUV) pulses, used in a pump-probe experiment. Our method is not based on a phase retrival algorithm, and for this it is typically much faster than the other ones currently known. Moreover, it allows for easily including in the reconstruction the experimental non-idealities that may affect the measurement, like possible distortion due to the measurement procedure itself.

Imaging multiphoton ionization dynamics of CH3I at a high repetition rate XUV free-electron laser

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core–hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (∼75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.

Ultrafast dynamics of correlation bands following XUV molecular photoionization

Modern ultrashort X-ray/XUV (extreme ultraviolet) sources provide unique opportunities to investigate the primary reactions of matter upon energetic excitation. Understanding these processes in molecules on ultrafast timescales is required to improve bespoke high-energy radiation detectors, nanomedicine schemes or to study the molecular composition of interstellar media. However, current experiments struggle to provide a general framework because of the uniqueness and complexity of each system. Here we show the universal role of correlation bands—features created by electron correlation. This is done by studying ultrafast energy relaxation of size-scalable two-dimensional molecules following ionization by an ultrashort XUV pulse. We observed long lifetimes that nonlinearly increase with the number of valence electrons. A general law based on solid-like electron–phonon scattering is proposed, which explains both our results and previously reported measurements. This offers new opportunities in attosecond science and high-energy photophysics. The size-dependent lifetimes observed in the ultrafast molecular relaxation dynamics of an entire class of polycyclic aromatic hydrocarbons can be explained by correlation bands and electron–phonon scattering, reminiscent of solid-state systems.

Multiple Sequential Ionization of Valence n = 4 Shell of Krypton by Intense Femtosecond XUV Pulses

Sequential photoionization of krypton by intense extreme ultraviolet femtosecond pulses is studied theoretically for the photon energies below the 3d excitation threshold. This regime with energetically forbidden Auger decay is characterized by special features, such as time scaling of the level population. The model is based on the solution of rate equations with photoionization cross sections of krypton in different charge and multiplet states determined using R-matrix calculations. Predictions of the ion yields and photoelectron spectra for various photon fluence are presented and discussed.

Pulse length effects on autoionizing states under the influence of intense SASE XUV fields

The Fano absorption line shape of an autoionizing state encodes information on its internal atomic structure and dynamics. When driven near-resonantly with intense extreme ultraviolet (XUV) electric fields, the absorption profile can be deliberately modified, including observable changes of both the line-shape asymmetry and strength of the resonance, revealing information on the underlying dynamics of the system in response to such external driving. We report on the influence of the XUV pulse parameters at high intensity that can be achieved with a free-electron laser (FEL) with statistically broadened spectra based on self-amplified spontaneous emission (SASE). More specifically, the impact of the FEL pulse duration is studied for the example of the doubly excited 2s2p resonance in helium, where line-shape modifications have been measured with XUV transient absorption spectroscopy in Fraunhofer-type transmission geometry. A computational few-level-model provides insight into the impact of different average pulse durations of the stochastic FEL pulses. These findings are supported by measurements performed at the Free-Electron Laser in Hamburg (FLASH) and provide further insight into XUV strong-coupling dynamics of resonant transitions driven by intense high-frequency FEL sources.

Thin-disk laser-pumped OPCPA system delivering 4.4 TW few-cycle pulses.

We present an optical parametric chirped pulse amplification (OPCPA) system delivering 4.4 TW pulses centered at 810 nm with a sub-9 fs duration and a carrier-envelope phase stability of 350 mrad. The OPCPA setup pumped by sub-10 ps pulses from two Yb:YAG thin-disk lasers at 100 Hz repetition rate is optimized for a high conversion-efficiency. The terawatt pulses of the OPCPA are utilized for generating intense extreme ultraviolet (XUV) pulses by high-order harmonic generation, achieving XUV pulse energies approaching the microjoule level.