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- ItemHigh-energy few-cycle pulses: post-compression techniques(Abingdon : Taylor & Francis Group, 2021) Nagy, Tamas; Simon, Peter; Veisz, LaszloContemporary ultrafast science requires reliable sources of high-energy few-cycle light pulses. Currently two methods are capable of generating such pulses: post compression of short laser pulses and optical parametric chirped-pulse amplification (OPCPA). Here we give a comprehensive overview on the post-compression technology based on optical Kerr-effect or ionization, with particular emphasis on energy and power scaling. Relevant types of post compression techniques are discussed including free propagation in bulk materials, multiple-plate continuum generation, multi-pass cells, filaments, photonic-crystal fibers, hollow-core fibers and self-compression techniques. We provide a short theoretical overview of the physics as well as an in-depth description of existing experimental realizations of post compression, especially those that can provide few-cycle pulse duration with mJ-scale pulse energy. The achieved experimental performances of these methods are compared in terms of important figures of merit such as pulse energy, pulse duration, peak power and average power. We give some perspectives at the end to emphasize the expected future trends of this technology. © 2020 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
- ItemX-ray spectroscopy of super-intense laser-produced plasmas for the study of nonlinear processes. Comparison with PIC simulations(Bristol : IOP Publ., 2017) Dalimier, E.; Ya Faenov, A.; Oks, E.; Angelo, P.; Pikuz, T.A.; Fukuda, Y.; Andreev, A.; Koga, J.; Sakaki, H.; Kotaki, H.; Pirozhkov, A.; Hayashi, Y.; Skobelev, I.Yu.; Pikuz, S.A.; Kawachi, T.; Kando, M.; Kondo, K.; Zhidkov, A.; Tubman, E.; Butler, N.M.H.; Dance, R.J.; Alkhimova, M.A.; Booth, N.; Green, J.; Gregory, C.; McKenna, P.; Woolsey, N.; Kodama, R.We present X-ray spectroscopic diagnostics in femto-second laser-driven experiments revealing nonlinear phenomena caused by the strong coupling of the laser radiation with the created plasma. Among those nonlinear phenomena, we found the signatures of the Two Plasmon Decay (TPD) instability in a laser-driven CO2 cluster-based plasma by analyzing the Langmuir dips in the profile of the O VIII Lyϵ line, caused by the Langmuir waves created at the high laser intensity 3 1018Wcm-2. With similar laser intensities, we reveal also the nonlinear phenomenon of the Second Harmonic Generation (SHG) of the laser frequency by analyzing the nonlinear phenomenon of satellites of Lyman δ and ϵ lines of Ar XVII. In the case of relativistic laser-plasma interaction we discovered the Parametric Decay Instability (PDI)-induced ion acoustic turbulence produced simultaneously with Langmuir waves via irradiation of thin Si foils by laser intensities of 1021Wcm-2.
- ItemOrigin of Terahertz Soft-Mode Nonlinearities in Ferroelectric Perovskites(College Park, Md. : APS, 2021) Pal, Shovon; Strkalj, Nives; Yang, Chia-Jung; Weber, Mads C.; Trassin, Morgan; Woerner, Michael; Fiebig, ManfredSoft modes are intimately linked to structural instabilities and are key for the understanding of phase transitions. The soft modes in ferroelectrics, for example, map directly the polar order parameter of a crystal lattice. Driving these modes into the nonlinear, frequency-changing regime with intense terahertz (THz) light fields is an efficient way to alter the lattice and, with it, the physical properties. However, recent studies show that the THz electric-field amplitudes triggering a nonlinear soft-mode response are surprisingly low, which raises the question on the microscopic picture behind the origin of this nonlinear response. Here, we use linear and two-dimensional terahertz (2D THz) spectroscopy to unravel the origin of the soft-mode nonlinearities in a strain-engineered epitaxial ferroelectric SrTiO3 thin film. We find that the linear dielectric function of this mode is quantitatively incompatible with pure ionic or pure electronic motions. Instead, 2D THz spectroscopy reveals a pronounced coupling of electronic and ionic-displacement dipoles. Hence, the soft mode is a hybrid mode of lattice (ionic) motions and electronic interband transitions. We confirm this conclusion with model calculations based on a simplified pseudopotential concept of the electronic band structure. It reveals that the entire THz nonlinearity is caused by the off-resonant nonlinear response of the electronic interband transitions of the lattice-electronic hybrid mode. With this work, we provide fundamental insights into the microscopic processes that govern the softness that any material assumes near a ferroic phase transition. This knowledge will allow us to gain an efficient all-optical control over the associated large nonlinear effects.
- ItemUltrasensitive Chiral Spectroscopy by Dynamical Symmetry Breaking in High Harmonic Generation(College Park, Md. : APS, 2019) Neufeld, Ofer; Ayuso, David; Decleva, Piero; Ivanov, Misha Y.; Cohen, OrenWe propose and numerically demonstrate a new chiral spectroscopy method that is based on a universal system-independent mechanism of dynamical symmetry breaking in high harmonic generation (HHG). The proposed technique relies only on intense electric-dipole transitions and not on their interplay with magnetic dipole transitions. The symmetry breaking results in the emission of otherwise “forbidden” harmonics from chiral media (i.e., that are not emitted from achiral or racemic media), yielding a huge, nearly background-free, chiral-achiral signal that is correlated to the magnitude of the medium’s enantiomeric excess. The handedness of the medium can be directly detected by measuring the polarization helicity of the emitted harmonics. Moreover, the strength of the “allowed” harmonics (that are not related to symmetry breaking) is chirality independent; hence, they can be used as a reference to probe chiral degrees of freedom within a single measurement. We numerically demonstrate up to 99% chiral-achiral signal level (normalized difference between the chiral and achiral HHG spectra) from microscopic gas-phase emission using state-of-the-art models for HHG in bromochlorofluoromethane and propylene oxide. We expect the new method to give rise to precise tabletop characterization of chiral media in the gas phase and for highly sensitive time-resolved probing of dynamical chiral processes with femtosecond-to-attosecond temporal resolution.
- ItemOnset of Bloch oscillations in the almost-strong-field regime([London] : Nature Publishing Group UK, 2022-12-13) Reislöhner, Jan; Kim, Doyeong; Babushkin, Ihar; Pfeiffer, Adrian N.In the field of high-order harmonic generation from solids, the electron motion typically exceeds the edge of the first Brillouin zone. In conventional nonlinear optics, on the other hand, the excursion of band electrons is negligible. Here, we investigate the transition from conventional nonlinear optics to the regime where the crystal electrons begin to explore the first Brillouin zone. It is found that the nonlinear optical response changes abruptly already before intraband currents due to ionization become dominant. This is observed by an interference structure in the third-order harmonic generation of few-cycle pulses in a non-collinear geometry. Although approaching Keldysh parameter γ = 1, this is not a strong-field effect in the original sense, because the iterative series still converges and reproduces the interference structure. The change of the nonlinear interband response is attributed to Bloch motion of the reversible (or transient or virtual) population, similar to the Bloch motion of the irreversible (or real) population which affects the intraband currents that have been observed in high-order harmonic generation.
- ItemFocus on nonlinear terahertz studies(Bristol : IOP, 2014) Leitenstorfer, A.; Nelson, K.A.; Reimann, K.; Tanaka, K.Resulting from the availability of improved sources, research in the terahertz (THz) spectral range has increased dramatically over the last decade, leading essentially to the disappearance of the so-called 'THz gap'. While most work to date has been carried out with THz radiation of low field amplitude, a growing number of experiments are using THz radiation with large electric and magnetic fields that induce nonlinearities in the system under study. This 'focus on' collection contains a number of articles, both experimental and theoretical, in the new subfield of THz nonlinear optics and spectroscopy on various systems, among them molecular gases, superconductors, semiconductors, antiferromagnets and graphene.
- ItemCompact intense extreme-ultraviolet source(Washington, DC : OSA, 2021) Major, Balázs; Ghafur, Omair; Kovács, Katalin; Varjú, Katalin; Tosa, Valer; Vrakking, Marc J. J.; Schütte, B.High-intensity laser pulses covering the ultraviolet to terahertz spectral regions are nowadays routinely generated in a large number of laboratories. In contrast, intense extreme-ultraviolet (XUV) pulses have only been demonstrated using a small number of sources including free-electron laser facilities [1-3] and long high-harmonic generation (HHG) beamlines [4-9]. Here we demonstrate a concept for a compact intense XUV source based on HHG that is focused to an intensity of $2 \times 10^{14}$ W/cm$^2$, with a potential increase up to $10^{17}$ W/cm$^2$ in the future. Our approach uses tight focusing of the near-infrared (NIR) driving laser and minimizes the XUV virtual source size by generating harmonics several Rayleigh lengths away from the NIR focus. Accordingly, the XUV pulses can be refocused to a small beam waist radius of 600 nm, enabling the absorption of up to four XUV photons by a single Ar atom in a setup that fits on a modest (2 m) laser table. Our concept represents a straightforward approach for the generation of intense XUV pulses in many laboratories, providing novel opportunities for XUV strong-field and nonlinear optics experiments, for XUV-pump XUV-probe spectroscopy and for the coherent diffractive imaging of nanoscale structures.
- ItemNon-instantaneous third-order optical response of gases in low-frequency fields(Washington, DC : Soc., 2022) Morales, Felipe; Richter, Maria; Ivanov, Misha; Husakou, AntonIt is commonly assumed that for low-intensity short optical pulses far from resonance, the third-order optical nonlinear response is instantaneous. We solve the three-dimensional time-dependent Schrödinger equation for the hydrogen atom and show that this is not the case: the polarization is not simply proportional to the cube of the electric field even at low intensities. We analyze the fundamental-frequency and third-harmonic nonlinear susceptibilities of hydrogen, investigate their dependence on intensity, and find that the delays in the Kerr response rapidly approach the femtosecond time-scale at higher intensities, while the delays in the third harmonic generation remain much lower. We also propose an experimental scheme to detect and characterize the above effects.
- ItemNon-instantaneous polarization dynamics in dielectric media(Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2014) Hofmann, Michael; Hyyti, Janne; Birkholz, Simon; Bock, Martin; Das, Susanta K.; Grunwald, Rüdiger; Hoffmann, Mathias; Nagy, Tamas; Demircan, Ayhan; Jupé, Marco; Ristau, Detlev; Morgner, Uwe; Brée, Carsten; Woerner, Michael; Elsaesser, Thomas; Steinmeyer, GünterThird-order optical nonlinearities play a vital role for generation1,2 and characterization 3-5 of some of the shortest optical pulses to date, for optical switching applications6,7, and for spectroscopy8,9. In many cases, nonlinear optical effects are used far off resonance, and then an instantaneous temporal response is expected. Here, we show for the first time resonant frequency-resolved optical gating measurements1012 that indicate substantial nonlinear polarization relaxation times up to 6.5 fs in dielectric media, i.e., significantly beyond the shortest pulses directly available from commercial lasers. These effects are among the fastest effects observed in ultrafast spectroscopy. Numerical solutions of the time-dependent Schrödinger equation13,14 are in excellent agreement with experimental observations. The simulations indicate that pulse generation and characterization in the ultraviolet may be severely affected by this previously unreported effect. Moreover, our approach opens an avenue for application of frequency-resolved optical gating as a highly selective spectroscopic probe in high-field physics.
- ItemUnusual terahertz waveforms from a resonant medium controlled by diffractive optical elements([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Pakhomov, A.V.; Arkhipov, R.M.; Arkhipov, M.V.; Demircan, A.; Morgner, U.; Rosanov, N.N.; Babushkin, I.Up to now, full tunability of waveforms was possible only in electronics, up to radio-frequencies. Here we propose a new concept of producing few-cycle terahertz (THz) pulses with widely tunable waveforms. It is based on control of the phase delay between different parts of the THz wavefront using linear diffractive optical elements. Suitable subcycle THz wavefronts can be generated via coherent excitation of nonlinear low-frequency oscillators by few-cycle optical pulses. Using this approach it is possible to shape the electric field rather than the slow pulse envelope, obtaining, for instance, rectangular or triangular waveforms in the THz range. The method is upscalable to the optical range if the attosecond pump pulses are used.