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- ItemHigh-order harmonic generation by polyatomic molecules(Bristol : IOP Publ., 2017) Odžak, S.; Hasović, E.; Milošević, D.B.We present a theory of high-order harmonic generation by arbitrary polyatomic molecules based on the molecular strong-field approximation (MSFA) in the framework of the S-matrix theory. A polyatomic molecule is modeled by an (N + 1)-particle system, which consists of N heavy atomic (ionic) centers and an electron. We derived various versions (with or without the dressing of the initial and/or final molecular state) of the MSFA. The general expression for the T-matrix element takes a simple form for neutral polyatomic molecules. We show the existence of the interference minima in the harmonic spectrum and explain these minima as a multiple-slit type of interference. This is illustrated by numerical examples for the nitrous oxide (N2O) molecule exposed to strong linearly polarized laser field.
- ItemFull-dimensional treatment of short-time vibronic dynamics in a molecular high-order-harmonic-generation process in methane(College Park, Md : APS, 2017) Patchkovskii, Serguei; Schuurman, Michael S.We present derivation and implementation of the multiconfigurational strong-field approximation with Gaussian nuclear wave packets (MC-SFA-GWP) - a version of the molecular strong-field approximation which treats all electronic and nuclear degrees of freedom, including their correlations, quantum mechanically. The technique allows realistic simulation of high-order-harmonic emission in polyatomic molecules without invoking reduced-dimensionality models for the nuclear motion or the electronic structure. We use MC-SFA-GWP to model isotope effects in high-order-harmonic-generation (HHG) spectroscopy of methane. The HHG emission in this molecule transiently involves the strongly vibronically coupled F22 electronic state of the CH4+ cation. We show that the isotopic HHG ratio in methane contains signatures of (a) field-free vibronic dynamics at the conical intersection (CI); (b) resonant features in the recombination cross sections; (c) laser-driven bound-state dynamics; as well as (d) the well-known short-time Gaussian decay of the emission. We assign the intrinsic vibronic feature (a) to a relatively long-lived (≥4 fs) vibronic wave packet of the singly excited ν4 (t2) and ν2 (e) vibrational modes, strongly coupled to the components of the F22 electronic state. We demonstrate that these physical effects differ in their dependence on the wavelength, intensity, and duration of the driving pulse, allowing them to be disentangled. We thus show that HHG spectroscopy provides a versatile tool for exploring both conical intersections and resonant features in photorecombination matrix elements in the regime not easily accessible with other techniques.
- ItemAttosecond control of electron-ion recollision in high harmonic generation(Bristol : IOP, 2011) Gademann, G.; Kelkensberg, F.; Siu, W.K.; Johnsson, P.; Gaarde, M.B.; Schafer, K.J.; Vrakking, M.J.J.We show that high harmonic generation driven by an intense nearinfrared (IR) laser can be temporally controlled when an attosecond pulse train (APT) is used to ionize the generation medium, thereby replacing tunnel ionization as the first step in the well-known three-step model. New harmonics are formed when the ionization occurs at a well-defined time within the optical cycle of the IR field. The use of APT-created electron wave packets affords new avenues for the study and application of harmonic generation. In the present experiment, this makes it possible to study harmonic generation at IR intensities where tunnel ionization does not give a measurable signal.
- ItemUsing the third state of matter: High harmonic generation from liquid targets(Bristol : IOP, 2014) Heissler, P.; Lugovoy, E.; Hörlein, R.; Waldecker, L.; Wenz, J.; Heigoldt, M.; Khrennikov, K.; Karsch, S.; Krausz, F.; Abel, B.; Tsakiris, G.D.High harmonic generation on solid and gaseous targets has been proven to be a powerful platform for the generation of attosecond pulses. Here we demonstrate a novel technique for the XUV generation on a smooth liquid surface target in vacuum, which circumvents the problem of low repetition rate and limited shot numbers associated with solid targets, while it maintains some of its merits. We employed atomically smooth, continuous liquid jets of water, aqueous salt solutions and ethanol that allow uninterrupted high harmonic generation due to the coherent wake emission mechanism for over 8 h. It has been found that the mechanism of plasma generation is very similar to that for smooth solid target surfaces. The vapor pressure around the liquid target in our setup has been found to be very low such that the presence of the gas phase around the liquid jet could be neglected.
- ItemChirp-control of resonant high-order harmonic generation in indium ablation plumes driven by intense few-cycle laser pulses(Washington, DC : Optical Society of America, OSA, 2018) Abdelrahman, Z.; Khokhlova, M.A.; Walke, D.J.; Witting, T.; Zair, A.; Strelkov, V.V.; Marangos, J.P.; Tisch, J.W.G.We have studied high-order harmonic generation (HHG) in an indium ablation plume driven by intense few-cycle laser pulses centered at 775 nm as a function of the frequency chirp of the laser pulse. We found experimentally that resonant emission lines between 19.7 eV and 22.3 eV (close to the 13th and 15th harmonic of the laser) exhibit a strong, asymmetric chirp dependence, with pronounced intensity modulations. The chirp dependence is reproduced by our numerical time-dependent Schrödinger equation simulations of a resonant HHG by the model indium ion. As demonstrated with our separate simulations of HHG within the strong field approximation, the resonance can be understood in terms of the chirp-dependent HHG photon energy coinciding with the energy of an autoionizing state to ground state transition with high oscillator strength. This supports the validity of the general theory of resonant four-step HHG in the few-cycle limit.
- ItemExtended high-harmonic spectra through a cascade resonance in confined quantum systems(College Park, MD : APS, 2022) Zhang, Xiao; Zhu, Tao; Du, Hongchuan; Luo, Hong-Gang; van den Brink, Jeroen; Ray, RajyavardhanThe study of high-harmonic generation in confined quantum systems is vital to establishing a complete physical picture of harmonic generation from atoms and molecules to bulk solids. Based on a multilevel approach, we demonstrate how intraband resonances significantly influence the harmonic spectra via charge pumping to the higher subbands and thus redefine the cutoff laws. As a proof of principle, we consider the interaction of graphene nanoribbons, with zigzag as well as armchair terminations, and resonant fields polarized along the cross-ribbon direction. Here, this effect is particularly prominent due to many nearly equiseparated energy levels. In such a scenario, a cascade resonance effect can take place in high-harmonic generation when the field strength is above a critical threshold, which is completely different from the harmonic generation mechanism of atoms, molecules, and bulk solids. We further discuss the implications not only for other systems in a nanoribbon geometry, but also systems where only a few subbands (energy levels) meet this frequency-matching condition by considering a generalized multilevel Hamiltonian. Our study highlights that cascade resonance has a fundamentally distinct influence on the laws of harmonic generation, specifically the cutoff laws based on laser duration, field strength, and wavelength, thus unraveling additional insights in solid-state high-harmonic generation.
- ItemHighly efficient soft x-ray spectrometer for transient absorption spectroscopy with broadband table-top high harmonic sources(Melville, NY : AIP Publishing LLC, 2021) Kleine, Carlo; Ekimova, Maria; Winghart, Marc-Oliver; Eckert, Sebastian; Reichel, Oliver; Löchel, Heike; Probst, Jürgen; Braig, Christoph; Seifert, Christian; Erko, Alexei; Sokolov, Andrey; Vrakking, Marc J. J.; Nibbering, Erik T. J.; Rouzée, ArnaudWe present a novel soft x-ray spectrometer for ultrafast absorption spectroscopy utilizing table-top femtosecond high-order harmonic sources. Where most commercially available spectrometers rely on spherical variable line space gratings with a typical efficiency on the order of 3% in the first diffractive order, this spectrometer, based on a Hettrick-Underwood design, includes a reflective zone plate as a dispersive element. An improved efficiency of 12% at the N K-edge is achieved, accompanied by a resolving power of 890. The high performance of the soft x-ray spectrometer is further demonstrated by comparing nitrogen K-edge absorption spectra from calcium nitrate in aqueous solution obtained with our high-order harmonic source to previous measurements performed at the electron storage ring facility BESSY II.