Attosecond Pulses Research Articles

Generation and applications of high-order harmonics and attosecond pulses in solids

Generation and applications of high-order harmonics and attosecond pulses in solids

“Beam à la carte”: Laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser

Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here, we demonstrate the use of a laser heater to shape electron bunches and enable the generation of attosecond x-ray pulses. We demonstrate that this method can be applied in a selective way, shaping a targeted subset of bunches while leaving the remaining bunches unchanged. This experiment enables the delivery of shaped x-ray pulses to multiple undulator beamlines, with pulse properties tailored to specialized scientific applications.

Attosecond transient interferometry

AbstractAttosecond transient absorption resolves the instantaneous response of a quantum system as it interacts with a laser field, by mapping its sub-cycle dynamics onto the absorption spectrum of attosecond pulses. However, the quantum dynamics are imprinted in the amplitude, phase and polarization state of the attosecond pulses. Here we introduce attosecond transient interferometry and measure the transient phase, as we follow its evolution within the optical cycle. We demonstrate how such phase information enables us to decouple the multiple quantum paths induced in a light-driven system, isolating their coherent contribution and retrieving their temporal evolution. Applying attosecond transient interferometry reveals the Stark shift dynamics in helium and retrieves long-term electronic coherences in neon. Finally, we present a vectorial generalization of our scheme, theoretically demonstrating the ability to isolate the underlying anomalous current in light-driven topological materials. Our scheme provides a direct insight into the interplay of light-induced dynamics and topology. Attosecond transient interferometry holds the potential to considerably extend the scope of attosecond metrology, revealing the underlying coherences in light-driven complex systems.

Topological phase transitions via attosecond x-ray absorption spectroscopy

We present a numerical experiment that demonstrates the possibility to capture topological phase transitions via an x-ray absorption spectroscopy scheme. We consider a Chern insulator whose topological phase is tuned via a second-order hopping. We perform time-dynamics simulations of the out-of-equilibrium laser-driven electron motion that enables us to model a realistic attosecond spectroscopy scheme. In particular, we use an ultrafast scheme with a circularly polarized IR pump pulse and an attosecond x-ray probe pulse. A laser-induced dichroism-type spectrum shows a clear signature of the topological phase transition. We are able to connect these signatures with the Berry structure of the system. This work extend the applications of attosecond absorption spectroscopy to systems presenting a non-trivial topological phase.

Relativistic treatment of hole alignment in noble gas atoms

The development in attosecond physics allows for unprecedented control of atoms and molecules in the time domain. Here, ultrashort pulses are used to prepare atomic ions in specific magnetic states, which may be important for controlling charge migration in molecules. Our work fills the knowledge gap of relativistic hole alignment prepared by femtosecond and attosecond pulses. The research focuses on optimizing the central frequency and duration of pulses to exploit specific spectral features, such as Fano profiles, Cooper minima, and giant resonances. Simulations are performed using the Relativistic Time-Dependent Configuration-Interaction Singles method. Ultrafast hole alignment with large ratios (on the order of one hundred) is observed in the outer-shell hole of argon. An even larger alignment (on the order of one thousand) is observed in the inner-shell hole of xenon.

Near-circularly polarized isolated attosecond pulse generation from a current-carrying state of Ar atom by two-color cross-linearly-polarized laser fields

Abstract We theoretically propose an efficient method to generate near-circularly polarized isolated attosecond (as) pulses (NCP-IAPs) from a current-carrying state of Ar atom driven by two-color cross-linearly-polarized laser fields. We find that the ellipticity of high harmonics can be controlled by adjusting the crossing angle of two linearly polarized lasers and the near-circularly polarized supercontinuum harmonics are obtained when the crossing angle is around 140°. Furthermore, we can produce the NCP-IAPs with the ellipticity up to 0.94 and the shortest one achieves 196 as. This work demonstrates the possibility for generating the NCP-IAPs using a current-carrying state of atoms driven by two-color cross-linearly-polarized laser fields.

Carrier-envelope phase effects on the reflectance of diamond films irradiated by ultrashort single-cycle light pulses: A comparison study in attosecond and femtosecond regimes

Diamond films irradiated with few-cycle laser pulses are emerging as a all-optical information processing device with high-speed and low-power-consumption. The possibility to steer, control or switch such few-cycle laser pulses with diamond films is expected to pave the way towards ultrafast all-optical switching. Here, we show theoretically the effect of the carrier-envelope phase (CEP) of the ultrashort single-cycle light pulses on the reflectance of diamond films within the framework of multi-scale theory. We observe clear variations in the reflectance behavior of femtosecond pulses and attosecond pulses. Our most important finding is that the reflectivity difference of attosecond pulses with different waveforms and the same spectrum on diamond films exhibits a perfect quadratic relationship with the CEP. This observation suggests that the nonlinearity of attosecond pulses is different from that of femtosecond pulses. Analysis of these results allows us to gain new insights in the interaction between attosecond light pulses and matter. This opens fascinating avenues for all-optical information processing over ultrashort lengths and timescales.

Octave-spanning supercontinuum coherent soft x-ray for producing a single-cycle soft x-ray pulse.

This study demonstrates the potential to generate a soft x-ray single-cycle attosecond pulse using a single-cycle mid-infrared pulse from advanced dual-chirped optical parametric amplification (DC-OPA). A super continuum high harmonic (HH) spectrum was generated in argon (80-160 eV) and neon (150-270 eV). The experimental spectra reasonably agree with those calculated by the strong-field approximation model and Maxwell's equations. In addition, simulation results indicate that the dispersion of HHs in argon can be compensated using a 207-nm Zr filter to obtain 40 as (Fourier transform limited (FTL)) pulses (1.1 cycles at 118 eV). For neon, a 278-nm Sn filter can compensate for the dispersion of HH and create 23 as FTL pulses (1.1 cycles at 206 eV). This soft x-ray single-cycle attosecond pulse is expected to be highly valuable for ultrafast science and applications in quantum information science.

Scheme for generation of spatiotemporal optical vortex attosecond pulse trains

The realization of spatiotemporal vortex structure of various physical fields with transverse orbital angular momentum (OAM) has attracted much attention and is expected to expand the research scope and open new opportunities in their respective fields. Here we present theoretically the first, to the best of our knowledge, study on the generation of attosecond pulse trains featuring a spatiotemporal optical vortex (STOV) structure by a two-color femtosecond light field, with each color carrying transverse OAM. Through careful optimization of relative phase and intensity ratio, we validate the efficient upconversion of the infrared pulse into its tens of order harmonics, showing that each harmonic preserves a corresponding intact topological charge. This unique characteristic enables the synthesis of an extreme ultraviolet attosecond pulse train with transverse OAM. In addition, we reveal that ionization depletion plays an outsize role therein. Our studies pave the way for the generation and utilization of light fields with STOV in the attosecond regime.

Attosecond impulsive stimulated X-ray Raman scattering in liquid water.

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a nonlinear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity-dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarization response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density.

Direct generation of a narrowband EUV vortex with ring Pearcey-Gaussian-vortex-beam-driven harmonics.

The generation of tunable extreme-ultraviolet (EUV) vortex beams is highly sought after for optoelectronic applications in the EUV region. In this study, we investigate the generation of vortex high-order harmonics using a ring Pearcey-Gaussian vortex beam as the driving source. We analyze the beam's spatial structure through phase-matching conditions and simulate high-order harmonic generation by solving the Maxwell wave equations. The beam's self-focusing characteristics and low-diffraction properties after focusing significantly enhance harmonics near the 53rd order, indicating the generation of a narrowband EUV vortex. Our findings underscore the advantages of using a ring Pearcey-Gaussian vortex beam for narrowband EUV vortex generation, paving the way for creating tunable vortex high-order harmonics or attosecond pulses with innovative vortex beams.

Few-femtosecond soft X-ray transient absorption spectroscopy with tuneable DUV-Vis pump pulses

Achieving few-femtosecond resolution for a pump-probe experiment is crucial to measuring the fastest electron dynamics and for creating superpositions of valence states in quantum systems. However, traditional UV-Vis pump pulses cannot achieve few-fs durations and usually operate at fixed wavelengths. Here, we present, to our knowledge, an unprecedented temporal resolution and pump tuneability for UV-Vis-pumped soft X-ray transient absorption spectroscopy. We have combined few-fs deep-UV to visible tuneable pump pulses from resonant dispersive wave emission in hollow capillary fiber with attosecond soft X-ray probe pulses from high harmonic generation. We achieve sub-5-fs time resolution, sub-fs interferometric stability, and continuous tuneability of the pump pulses from 230 to 700 nm. We demonstrate that the pump can initiate an ultrafast photochemical reaction and that the dynamics at different atomic sites can be resolved simultaneously. These capabilities will allow studies of the fastest electronic dynamics in a large range of photochemical, photobiological and photovoltaic reactions.

Controlling the generation of elliptically polarized isolated attosecond pulses from mixed gases with a polarization-gating technique

Controlling the generation of elliptically polarized isolated attosecond pulses from mixed gases with a polarization-gating technique

Nobel Lecture: Genesis and applications of attosecond pulse trains

Nobel Lecture: Genesis and applications of attosecond pulse trains

Nobel Lecture: The route to attosecond pulses

Nobel Lecture: The route to attosecond pulses

Deciphering the role of three-color synthesized laser pulse parameters in N2 ionization and attosecond pulse shaping

Photoionization of atoms or molecules is a fundamental process in strong-field physics, essential for generating high-order harmonics and producing attosecond pulses. Here, we investigate how a three-color laser field, consisting of wavelengths at 800 nm and its second and third harmonics, photoionizes N2 molecules and evaluates its effect on the properties of attosecond pulses. It has been discovered that by altering the relative phase, these harmonics periodically influence molecular ionization, increasing the discreteness and strength of the attosecond pulse trains. Three-color field driving dramatically raises the pulse peak while decreasing the width of the strongest peak pulse, whereas two-color field driving just slightly enhances the pulse intensity and duration. Furthermore, the effectiveness of harmonic production is significantly increased by varying the laser intensity ratios. Even though the efficiency and pulse intensity of the three-color field are limited by conversion efficiency, attosecond pulses with higher intensities can be produced with proper parameter tuning at lower ionization rates. These findings offer a significant foundation for precisely controlling attosecond pulse generation. Ocis codes320.7110; 320.7120.

Isolated attosecond pulse generation in a semi-infinite gas cell driven by time-gated phase matching

Isolated attosecond pulse (IAP) generation usually involves the use of short-medium gas cells operated at high pressures. In contrast, long-medium schemes at low pressures are commonly perceived as inherently unsuitable for IAP generation due to the nonlinear phenomena that challenge favourable phase-matching conditions. Here we provide clear experimental evidence on the generation of isolated extreme-ultraviolet attosecond pulses in a semi-infinite gas cell, demonstrating the use of extended-medium geometries for effective production of IAPs. To gain a deeper understanding we develop a simulation method for high-order harmonic generation (HHG), which combines nonlinear propagation with macroscopic HHG solving the 3D time-dependent Schrödinger equation at the single-atom level. Our simulations reveal that the nonlinear spatio-temporal reshaping of the driving field, observed in the experiment as a bright plasma channel, acts as a self-regulating mechanism boosting the phase-matching conditions for the generation of IAPs.

Photoelectron momentum distributions of triatomic CO2 molecules by circularly polarized attosecond pulses

Abstract Molecular-frame photoelectron momentum distributions (MF-PMDs) have been studied for imaging molecular structures. We investigate the MF-PMDs of CO2 molecules exposed to circularly polarized (CP) attosecond laser pulses by solving the time-dependent Schrödinger equations based on the single-active-electron approximation frames. Results show that high-frequency photons lead to photoelectron diffraction patterns, indicating molecular orbitals, these diffraction patterns can be illustrated by the ultrafast photoionization models. However, for the driving pulses with 30 nm, a deviation between MF-PMDs and theoretically predicted results of the ultrafast photoionization models is produced because the Coulomb effect strongly influences the molecular photoionization. Meanwhile, the MF-PMDs rotates in the same direction as the helicity of driving laser pulses. Our results also demonstrate that the MF-PMDs in a CP laser pulse are the superposition of those in the parallel and perpendicular linearly polarized cases. The simulations efficiently visualize molecular orbital geometries and structures by ultrafast photoelectron imaging. Furthermore, we determine the contribution of HOMO and HOMO-1 orbitals to ionization by varying the relative phase and the ratio of these two orbitals.

Lightwave-controlled relativistic plasma mirrors.

We report on attosecond-scale control of high-harmonic and fast electron emission from plasma mirrors driven by relativistic-intensity near-single-cycle light waves at a kHz repetition rate. By controlling the waveform of the intense light transient, we reproducibly form a sub-cycle temporal intensity gate at the plasma mirror surface, leading to the observation of extreme ultraviolet spectral continua, characteristic of isolated attosecond pulse (IAP) generation. We also observe the correlated emission of a waveform-dependent relativistic electron beam, paving the way toward fully lightwave-controlled dynamics of relativistic plasma mirrors.

Attosecond vortex pulse trains

The landscape of ultrafast structured light pulses has significantly advanced thanks to the ability of high-order harmonic generation (HHG) to translate the spatial properties of infrared laser beams to the extreme-ultraviolet (EUV) spectral range. In particular, the up-conversion of orbital angular momentum (OAM) has enabled the generation of high-order harmonics whose OAM scales linearly with the harmonic order and the topological charge of the driving field. Having a well-defined OAM, each harmonic is emitted as an EUV femtosecond vortex pulse. However, the order-dependent OAM across the harmonic comb precludes the synthesis of attosecond vortex pulses. Here we demonstrate a method for generating attosecond vortex pulse trains, i.e., a succession of attosecond pulses with a helical wavefront, resulting from the coherent superposition of a comb of EUV high-order harmonics with the same OAM. By driving HHG with a polarization tilt-angle fork grating, two spatially separated circularly polarized high-order harmonic beams with order-independent OAM are created. Our work opens the route towards attosecond-resolved light-matter interactions with two extra degrees of freedom, spin and OAM, which are particularly interesting for probing chiral systems and magnetic materials.