Extreme-ultraviolet (XUV) sources including high-harmonic generation, free-electron lasers, 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 lithography. The bandwidth of the XUV light emitted by these sources reflects the XUV generation process used. While light from soft-x-ray lasers and XUV FELs typically has a relatively narrow bandwidth, plasma sources and HHG sources driven by few-cycle laser pulses emit broadband XUV pulses. Since these characteristic properties of a given XUV source impose limitations to applications, techniques enabling modification of the XUV bandwidth are highly desirable. Here we demonstrate a concept for efficient spectral compression of a broadband XUV pulse via four-wave mixing (FWM) in the presence of a broadband near-infrared (NIR) pulse in a krypton gas jet, exploiting a phase-matching scheme based on closely-spaced resonances. Our concept provides new possibilities for tailoring the spectral bandwidth of XUV beams.
Noncollinear wave-mixing spectroscopies with attosecond extreme ultraviolet (XUV) pulses provide unprecedented insight into electronic dynamics. In infrared and visible regimes, heterodyne detection techniques utilize a reference field to amplify wave-mixing signals while simultaneously allowing for phase-sensitive measurements. Here, we implement a self-heterodyned detection scheme in noncollinear wave-mixing measurements with a short attosecond XUV pulse train and two few-cycle near infrared (NIR) pulses. The initial spatiotemporally overlapped XUV and NIR pulses generate a coherence of both…
We report here experimental results of perturbative nonlinear optical wave-mixing processes in the extreme ultraviolet region by using two-color and three-color laser fields. Besides the usual odd-harmonic spectrum of high harmonic generation, new spectral components are observed when multiple incommensurate lasers (one driving plus one or two control field) interact with neutral krypton gas. To demonstrate the wave-mixing process underlying such an observation, we firstly couple the driving field with either the signal or the idler field of an optical parametric amplifier in the gaseous ensem…
We perform a post-compression of high energy pulses by using optical-field ionization of low pressure helium gas in a guided geometry. We apply this approach to a TW chirped-pulse-amplification based Ti:Sapphire laser chain and show that spectral broadening can be controlled both with the input pulse energy and gas pressure. Under optimized conditions, we generate 10 fs pulses at TW level directly under vacuum and demonstrate a high stability of the post compressed pulse duration. These high energy post-compressed pulses are thereafter used to perform high harmonic generation in a loose focusi…
The emission of high-order harmonics from solids \cite{ghimire11a,schubert14a,luu15a,golde08a} under intense laser-pulse irradiation is revolutionizing our understanding of strong-field solid-light interactions \cite{ghimire11a,schubert14a,luu15a,vampa15b,yoshikawa17a,hafez18a,jurgens20a}, while simultaneously opening avenues towards novel, all-solid, coherent, short-wavelength table-top sources with tailored emission profiles and nanoscale light-field control\cite{franz19a,roscamCLEO21}. To date, broadband spectra have been generated well into the extreme-ultraviolet (XUV) \cite{luu15a,luu18b…
The ongoing development of intense high-harmonic generation (HHG) sources has recently enabled highly nonlinear ionization of atoms by the absorption of at least 10 extreme-ultraviolet (XUV) photons within a single atom [Senfftleben \textit{et al.}, arXiv1911.01375]. Here we investigate the role that reshaping of the fundamental, few-cycle, near-infrared (NIR) driving laser within the 30-cm-long HHG Xe medium plays in the generation of the intense HHG pulses. Using an incident NIR intensity that is higher than what is required for phase-matched HHG, signatures of reshaping are found by measuri…
We report here a detailed study of the four-wave mixing process in the extreme ultraviolet (XUV) region around 30 nm by using two collinear incommensurate frequency laser pulses. The experimental results reveal evidence of the coherent accumulation of the wave-mixing fields and low-order (third-order and fifth-order) nonlinear response of an argon medium. The dependence of the intensities of the mixing fields on the intensity of a weak control field, on the argon pressure and on the interaction length is analyzed to show that the four-wave mixing fields in this spectral range are generated und…
Advancing table-top attosecond sources in brightness and pulse duration is of immense interest and importance for an expanding sphere of applications. Recent theoretical studies [New J. Phys., 22 093030 (2020)] have found that high-order frequency mixing (HFM) in a two-color laser field can be much more efficient than high-order harmonic generation (HHG). Here we study the attosecond properties of the coherent XUV generated via HFM analytically and numerically, focusing on the practically important case when one of the fields has much lower frequency and much lower intensity than the other one…
We present a theoretical model and respective numerical simulation of cascaded four-wave mixing of femtosecond pulses in bulk chi(3) media, evidencing the importance of two-dimensional interaction geometries in the efficient generation of frequency-converted beams, and in agreement with the experimental results in terms spectral and spatial distribution and efficiency, demonstrating compression without the need of complex amplitude or phase control.
Probing of Core Excitons in Solid NaF with Polarization-Selective Attosecond Time-Resolved Four-Wave Mixing Spectroscopy
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；University of Regensburg（雷根斯堡大学）；Lund University（隆德大学）
We report on the generation of a train of ~ 2 ps, 10 um laser pulses via multiple four-wave mixing and compression of an infrared laser beat-wave propagating in the negative group velocity dispersion region of bulk GaAs and a combination of GaAs and NaCl. The use of a 200 ps, 106 GHz beat-wave, produced by combining laser pulses amplified on the 10P(20) and 10P(16) transition of a CO2 laser, provides a novel method for generating high-power, picosecond, mid-IR laser pulses at a high repetition rate. By using 165 and 882 GHz beat-waves we show that cascaded phase-mismatched difference frequency…
We numerically investigate the use of strong THz radiation in assisting single attosecond pulse generation by few-cycle, 800 nm laser pulses. We optimize focusing conditions to generate short and powerful single attosecond pulses of high-energy photons by keeping the parameters of the THz field within the limits achieved experimentally. We show that using optimal focusing geometry isolated attosecond pulses shorter than 100 as can be obtained even in the absence of further gating or XUV compression techniques, using an 8 fs generating pulse. Furthermore, quantum path control of short- and long…
The Free-Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high-flux, high-repetition rate XUV and soft X-ray pulses. The vast majority of experiments at FLASH are of pump-probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott-type multi-pass cell and subsequent pulse compression to sub-100 fs durations. Compared to other facility lasers employing optical parametric amplification, the new …
We study high-order harmonic generation (HHG) driven by seeded plasmonic-enhanced fields. On one hand, plasmonic-enhanced fields have shown a great potential to extend the HHG cutoff, an instrumental pre-requisite for the generation of attosecond pulses. On another hand, the use of XUV seeds appears to have a considerable potential to improve the HHG conversion efficiency, which is typically modest when a unique fundamental laser pulse is employed. By mixing these two sources, we show it is possible to, simultaneously, boost the HHG cutoff and to increase the harmonic photon flux. The combinat…
We report on the generation of four spatially multiplexed picosecond 40-GHz pulse trains in a km-long 6-LP multimode optical fiber. The principle of operation is based on the parallel nonlinear compression of initial beat-signals into well separated pulse trains owing to intra-modal multiple four-wave mixings. A series of four 40-GHz dual-frequency beatings at different wavelengths are simultaneously injected into the LP01, LP11, LP02 and LP12 modes of a 1.8-km long graded-index few-mode fiber. The combined effects of Kerr nonlinearity and anomalous chromatic dispersion lead to the simultaneou…
We experimentally demonstrate a spectral compression scheme for heralded single photons with narrow spectral bandwidth around 795 nm, generated through four-wave mixing in a cloud of cold Rb-87 atoms. The scheme is based on an asymmetric cavity as a dispersion medium and a simple binary phase modulator, and can be, in principle, without any optical losses. We observe a compression from 20.6 MHz to less than 8 MHz, almost matching the corresponding atomic transition.
Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG) process in a free-electron laser (FEL) is a promising approach to facilitate various coherent nonlinear spectroscopy schemes in the extreme ultraviolet (XUV) spectral range. However, in collinear arrangements using a single nonlinear medium, temporally overlapping seed pulses may introduce nonlinear mixing signals that compromise the experiment at short time delays. Here, we investigate these effects in detail by extending the analysis described in a recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). Hi…
The cascaded biphoton state generated from a cold atomic ensemble presents one of the strongly correlated resources that can preserve and relay quantum information. Under the four-wave mixing condition, the emitted signal and idler photons from the upper and lower excited states become highly correlated in their traveling directions and entangled in continuous frequency spaces. In this system, we theoretically study the spectral compression of the biphoton source using an external cavity and show the reduction in its frequency entanglement entropy. This indicates, respectively, an improved lig…
We investigate the generation of optical frequency combs through a cascade of four-wave mixing processes in nonlinear fibres with optimised parameters. The initial optical field consists of two continuous-wave lasers with frequency separation larger than 40 GHz (312.7 pm at 1531 nm). It propagates through three nonlinear fibres. The first fibre serves to pulse shape the initial sinusoidal-square pulse, while a strong pulse compression down to sub-100 fs takes place in the second fibre which is an amplifying erbium-doped fibre. The last stage is a low-dispersion highly nonlinear fibre where the…
XUV and X-ray Free Electron Lasers (FELs) produce short wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilised for many experiments previously possible at long wavelengths only: multiphoton ionization, pumping an atomic laser, and four-wave mixing spectroscopy. However one important optical technique, coherent control, has not yet been demonstrated, because Self- Amplified Spontaneous Emission FELs have limited longitudinal coherence. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent, and t…
The emission of dispersive waves (DWs) by temporal solitons can be described as a cascaded four-wave mixing process triggered by a pair of monochromatic continuous waves (CWs). We report experimental and numerical results demonstrating that the efficiency of this process is strongly and non-trivially affected by the frequency detuning of the CW pump lasers. We explain our results by showing that individual cycles of the input dual-frequency beat signal can evolve as higher-order solitons whose temporal compression and soliton fission govern the DW efficiency. Analytical predictions based on th…
We present a design for a high-energy single stage mid-IR difference frequency generation adapted to a two-color Ti:sapphire amplifier system. The optimized mixing process is based on chirped pulse difference frequency generation (CP-DFG), allowing for a higher conversion efficiency, larger bandwidth and reduced two photon absorption losses. The numerical start-to-end simulations include stretching, chirped pulse difference frequency generation and pulse compression. Realistic design parameters for commercially available non linear crystals (GaSe, AgGaS2, LiInSe2, LiGaSe2) are considered. Comp…
Bright and broadband coherent mid-IR radiation is important for exciting and probing molecular vibrations. Using cascaded nonlinearities in conventional quadratic nonlinear crystal like lithium niobate, self-defocusing near-IR solitons have been demonstrated that led to very broadband supercontinuum generation in the visible, near-IR and short-wavelength mid-IR. Here we conduct an experiment where a mid-IR crystal pumped in the mid-IR gives multiple-octave spanning supercontinua. The crystal is cut for noncritical interaction, so the three-wave mixing of a single mid-IR femtosecond pump source…
We experimentally demonstrate spectral broadening and shaping of exponentially-decaying nanosecond pulses via nonlinear mixing with a phase-modulated pump in a periodically-poled lithium niobate (PPLN) waveguide. A strong, 1550~nm pulse is imprinted with a temporal phase and used to upconvert a weak 980 nm pulse to 600 nm while simultaneously broadening the spectrum to that of a Lorentzian pulse up to 10 times shorter. While the current experimental demonstration is for spectral shaping, we also provide a numerical study showing the feasibility of subsequent spectral phase correction to achiev…
