XUV yield optimization of two-color high-order harmonic generation in gases
Ann-Kathrin Raab, Melvin Redon, Sylvianne Roscam Abbing, Yuman Fang, Chen Guo, Peter Smorenburg, Johan Mauritsson, Anne-Lise Viotti, Anne L'Huillier, Cord L. Arnold
We perform an experimental two-color high-order harmonic generation study in argon with the fundamental of an ytterbium ultrashort pulse laser and its second harmonic. The intensity of the second harmonic and its phase relative to the fundamental are varied, in a large range compared to earlier works, while keeping the total intensity constant. We extract the optimum values for the relative phase and ratio of the two colors which lead to a maximum yield enhancement for each harmonic order in the extreme ultraviolet spectrum. Within the semi-classical three-step model, the yield maximum can be associated with a flat electron return time vs. return energy distribution. An analysis of different distributions allows to predict the required relative two-color phase and ratio for a given harmonic order, total laser intensity, fundamental wavelength, and ionization potential.
Based on the frequency-domain theory, we investigate the above-threshold ionization (ATI) process of an atom in a two-color laser field with infrared (IR) and extreme ultraviolet (XUV) frequencies, where the photon energy of the XUV laser is close to or larger than the atomic ionization threshold. By using the channel analysis, we find that the two laser fields play different roles in an ionization process, where the XUV laser determines the ionization probability by the photon number that the atom absorbs from it, while the IR laser accelerates the ionized electron and hence widens the electr…
High-order above-threshold ionization (HATI) spectrum in IR+XUV two-color laser fields has been investigated. We found that the quantum features corresponding to the absorption of the XUV photon is well illustrated by a peculiar dip structure in the second plateau of the HATI spectrum. By the channel analysis, we show that the angular distribution of the spectrum is attributed to the coherent summation over contributions of different channels, and the dip structure in the spectrum is directly related to the absorption of one XUV photon of the ionized electron during the laser-assisted collisio…
The collision-ionization mechanism of nonsequential double ionization (NSDI) process in IR+XUV two-color laser fields [\PRA \textbf{93}, 043417 (2016)] has been investigated by us recently. Here we extend this work to study the collision-excitation-ionization (CEI) mechanism of NSDI processes in the two-color laser fields with different laser conditions. It is found that the CEI mechanism makes a dominant contribution to the NSDI as the XUV photon energy is smaller than the ionization threshold of the He$^+$ ion, and the momentum spectrum shows complex interference patterns and symmetrical str…
We observe a new regime of coherent XUV radiation generation in noble gases induced by femtosecond pulses at very high intensities. This XUV emission has both a reduced divergence and spectral width as compared to high-order harmonic generation (HHG). It is not emitted at a moderate intensity of the driving pulses where only high-order harmonics are generated. At high driving intensities, the additional XUV comb appears near all harmonic orders and even exceeds the HHG signal on the axis. The peaks are observed in several gases and their frequencies do not depend on the driving intensity or ga…
The two-color above-threshold ionization (ATI) of atoms and ions is investigated for a vortex Bessel beam in the presence of a strong near-infrared (NIR) light field. While the photoionization is caused by the photons from the weak but extreme ultra-violet (XUV) vortex Bessel beam, the energy and angular distribution of the photoelectrons and their sideband structure are affected by the plane-wave NIR field. We here explore the energy spectra and angular emission of the photoelectrons in such two-color fields as a function of the size and location of the target (atoms) with regard to the beam …
The development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics ($\approx14\,$eV) in argon and krypton. Our technique simultaneously provides high phase st…
We present an {\it ab initio} and non-perturbative time-dependent approach to the problem of double ionization of a general atom driven by intense XUV laser pulses. After using a highly flexible $B$-Spline $R$-matrix method to generate field-free Hamiltonian and electric dipole matrices, the initial state is propagated in time using an efficient Arnoldi-Lanczos scheme. Test calculations for double ionization of He by a single laser pulse yield good agreement with benchmark results obtained with other methods. The method is then applied to two-color pump-probe processes, for which momentum and …
High-order harmonic generation (HHG) in gases leads to short-pulse extreme ultraviolet (XUV) radiation useful in a number of applications, for example, attosecond science and nanoscale imaging. However, this process depends on many parameters and there is still no consensus on how to choose the target geometry to optimize the source efficiency. Here, we review the physics of HHG with emphasis on the macroscopic aspects of the nonlinear interaction. We analyze the influence of medium length, pressure, position of the medium and intensity of the driving laser on the HHG conversion efficiency (CE…
We investigate the evolution of extreme ultraviolet (XUV) spectral lineshapes in an optically-thick helium gas under near-infrared (IR) perturbation. In our experimental and theoretical work, we systematically vary the IR intensity, time-delay, gas density and IR polarization parameters to study lineshape modifications induced by collective interactions, in a regime beyond the single atom response of a thin, dilute gas. In both experiment and theory, we find that specific features in the frequency-domain absorption profile, and their evolution with propagation distance, can be attributed to th…
Density-gradient effect in high-harmonic generation in gases
ELI ALPS, The Extreme Light Infrastructure ERIC（ELI ALPS，极轻基础设施 ERIC）；Institute of Physics, University of Szeged（塞格德大学物理研究所）；Department of Optics and Quantum Electronics, University of Szeged（塞格德大学光学与量子电子学系）
In this study the generation of energetic coherent extreme ultraviolet (XUV) radiation with controlled polarization, is reported. The XUV radiation results from the process of high harmonic generation (HHG), in a gas phase atomic medium, driven by an intense two-color circularly polarized counter-rotating laser field, under loose focusing geometry conditions. The energy of the XUV radiation emitted per laser pulse is found to be of the order of ~100 nJ with the spectrum spanning from 17 to 26 eV. The demonstrated energy values along with tight focusing geometries is sufficient to induce nonlin…
We analytically describe the strong-field light-electron interaction using a quantized coherent laser state with arbitrary photon number. We obtain a light-electron wave function which is a closed-form solution of the time-dependent Schrodinger equation (TDSE). This wave function provides information about the quantum optical features of the interaction not accessible by semi-classical theories. With this approach we can reveal the quantum optical properties of high harmonic generation (HHG) process in gases by measuring the photon statistics of the transmitted infrared (IR) laser radiation. T…
Measurements of the phase of two-photon matrix elements are presented for resonant and antiresonant two-color ionization of helium. A tunable, narrow-bandwidth, near-infrared (NIR) laser source is used for extreme ultra-violet (XUV) high-harmonic generation (HHG). The 15th harmonic of the laser is used within (1+1') XUV+NIR two-photon ionization, and tuned in and out of resonance with members of the 1s$n$p $^1$P$_1$ ($n=3,4,5$) Rydberg series, covering a broad spectral range with high spectral resolution. The technique allows to observe characteristic rapid changes in the phase of the two-phot…
The high-order harmonic spectrum generated in two-color intense laser field under certain conditions has a pronounced maximum caused by the so called spectral caustic. Using a numerical solution of the 3D time-dependent Schrödinger equation we study the width of the maximum and the degree of the generation enhancement due to the caustic as a function of the fundamental intensity, wavelength, and atomic ionization potential. It is shown that the degree of this enhancement can be well quantitatively characterized by a single parameter: the ratio of the radius of the free electronic oscillation i…
Photoelectron energy spectra resulting by the interaction of hydrogen with two short pulses having carrier frequencies, respectively, in the range of the infrared and XUV regions have been calculated. The effects of the pulse duration and timing of the X-ray pulse on the photoelectron energy spectra are discussed. Analysis of the spectra obtained for very long pulses show that certain features may be explained in terms of quantum interferences in the time domain. It is found that, depending on the duration of the X-ray pulse, ripples in the energy spectra separated by the infrared photon energ…
D$_2$ molecules, excited by linearly cross-polarized femtosecond extreme ultraviolet (XUV) and near-infrared (NIR) light pulses, reveal highly structured D$^+$ ion fragment momenta and angular distributions that originate from two different 4-step dissociative ionization pathways after four photon absorption (1 XUV + 3 NIR). We show that, even for very low dissociation kinetic energy release $\le$~240~meV, specific electronic excitation pathways can be identified and isolated in the final ion momentum distributions. With the aid of {\it ab initio} electronic structure and time-dependent Schröd…
We report a novel quasi-phase matching technique for high-order harmonic generation in low-density gases. Numerical simulations show that in few-optical cycle pulsed Bessel beams it is possible to control the pulse envelope and phase velocities which in turn allows to control the carrier-envelope phase during propagation. The resulting oscillations in the peak intensity allow to phase-match the high-order harmonic generation process with a nearly two decade enhancement in the XUV power spectrum.
Transversely loaded bidimensional-magneto-optical-traps (2D-MOT) have been recently developed as high flux sources for cold strontium atoms to realize a new generation of compact experimental setups. Here, we discuss on the implementation of a cross-polarized bi-color slower for a strontium atomic beam improving the 2D-MOT loading, and increasing the number of atoms in a final MOT by eleven times. Our slowing scheme addresses simultaneously two excited Zeeman substates of the 88Sr 1S0->1P1 transition at 461 nm. We also realized a 3-axis active feedback control of the magnetic field down to the…
We present theoretical investigations of high-order harmonic generation (HHG) resulting from the interaction of noble gases with localized surface plasmons. These plasmonic fields are produced when a metal nanoparticle is subject to a few-cycle laser pulse. The enhanced field, which largely depends on the geometrical shape of the metallic structure, has a strong spatial dependency. We demonstrate that the strong non-homogeneity of this laser field plays an important role in the HHG process and leads to a significant increase of the harmonic cut-off energy. In order to understand and characteri…
We study theoretically the effect of the giant resonance in Xe on the phase difference between the consecutive high order resonantly-enhanced harmonics and calculate the duration of the attosecond pulses produced by these harmonics. For certain conditions resonantly-induced dephasing compensates the phase difference which is intrinsic for the off-resonance harmonics. We find these conditions analytically and compare them with the numerical results. This harmonic synchronization allows attosecond pulse shortening in conjunction with the resonance-induced intensity increase by more than an order…
A way to considerably enhance terahertz radiation, emitted in the interaction of intense mid-infrared laser pulses with atomic gases, in both the total energy and the electric-field amplitude is suggested. The scheme is based on the application of a two-color field consisting of a strong circularly polarized mid-infrared pulse with wavelengths of $1.6÷4\,μ{\rm m}$ and its linearly or circularly polarized second harmonic of lower intensity. By combining the strong-field approximation for the ionization of a single atom with particle-in-cell simulations of the collective dynamics of the generate…
High-harmonic generation (HHG) normally requires a careful adjustment of the driving laser intensity (typically $10^{14} - 10^{15}$ W/cm$^2$) and gas medium parameters to enable good phase matching conditions. In contrast with conventional wisdom, we present experimental results indicating phase-matched HHG in all rare gases, using a high-density medium and a driver laser intensity of around $10^{16}$ W/cm$^2$. The experimental results are corroborated by theoretical simulations, which indicate that ionization-induced self-phase modulation and plasma defocusing self-regulate the driver laser i…
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…
Subcycle phase matching effects in short attosecond pulse trains
Universidad de Salamanca（萨拉曼卡大学）；Lund University（隆德大学）；Politecnico di Milano（米兰理工大学）；Institute for Photonics and Nanotechnologies, IFN-CNR（光子与纳米技术研究所，意大利国家研究委员会）
Isolated attosecond pulses (IAPs) produced through laser-driven high-harmonic generation (HHG) hold promise for unprecedented insight into biological processes via attosecond x-ray diffraction with tabletop sources. However, efficient scaling of HHG towards x-ray energies has been hampered by ionization-induced plasma generation impeding the coherent buildup of high-harmonic radiation. Recently, it has been shown that these limitations can be overcome in the so-called 'overdriven regime' where ionization loss and plasma dispersion strongly modify the driving laser pulse over small distances, a…
