10 results
Search Results
Now showing 1 - 10 of 10
- 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.
- ItemSpatial distribution of electric-field enhancement across the gap of terahertz bow-tie antennas(Washington, DC : Soc., 2020) Runge, Matthias; Engel, Dieter; Schneider, Michael; Reimann, Klaus; Woerner, Michael; Elsaesser, ThomasThe electric-field enhancement in terahertz (THz) antennas designed for nonlinear THz spectroscopy of soft matter is characterized by spatially resolved electrooptic sampling. To mimic the relevant interaction geometry, metallic, resonant bow-tie antennas are deposited on a thin zinc telluride crystal of 10 µm thickness. The THz electric field transmitted through the antenna gap is recorded by electrooptic sampling. By focusing the 800 nm, sub-20 fs sampling pulses, we achieve a spatial resolution of some 3 µm, which is 1/3 to 1/8 of the antenna-gap width. The THz field in the gap displays an enhancement by a factor of up to 4.5 with a pronounced spectral variation, depending sensitively on the antenna-arm length and the gap width. By scanning the 800 nm probe spot laterally through the antenna gap, the spatial variation of the enhancement is determined, reaching the highest values at the edges of the gap. The results are in agreement with simulations of the electric-field distributions by finite-element calculations. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
- ItemTowards shot-noise limited diffraction experiments with table-top femtosecond hard x-ray sources(Melville, NY : AIP Publishing LLC, 2017) Holtz, Marcel; Hauf, Christoph; Weisshaupt, Jannick; Salvador, Antonio-Andres Hernandez; Woerner, Michael; Elsaesser, ThomasTable-top laser-driven hard x-ray sources with kilohertz repetition rates are an attractive alternative to large-scale accelerator-based systems and have found widespread applications in x-ray studies of ultrafast structural dynamics. Hard x-ray pulses of 100 fs duration have been generated at the Cu Kα wavelength with a photon flux of up to 109 photons per pulse into the full solid angle, perfectly synchronized to the sub- 100-fs optical pulses from the driving laser system. Based on spontaneous x-ray emission, such sources display a particular noise behavior which impacts the sensitivity of x-ray diffraction experiments. We present a detailed analysis of the photon statistics and temporal fluctuations of the x-ray flux, together with experimental strategies to optimize the sensitivity of optical pump/x-ray probe experiments. We demonstrate measurements close to the shot-noise limit of the x-ray source.
- ItemUltrafast spatio-temporal dynamics of terahertz generation by ionizing two-color femtosecond pulses in gases(Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2010) Babushkin, Ihar; Kuehn, Wihelm; Köhler, Christian; Skupin, Stefan; Bergé, Luc; Reimann, Klaus; Woerner, Michael; Herrmann, Joachim; Elsaesser, ThomasWe present a combined theoretical and experimental study of spatio-temporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatio-temporal reshaping and of a plasma-induced blue-shift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.
- 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.
- ItemTheoretical analysis of hard x-ray generation by nonperturbative interaction of ultrashort light pulses with a metal(Melville, NY : AIP Publishing LLC, 2015) Weisshaupt, Jannick; Juvé, Vincent; Holtz, Marcel; Woerner, Michael; Elsaesser, ThomasThe interaction of intense femtosecond pulses with metals allows for generating ultrashort hard x-rays. In contrast to plasma theories, tunneling from the target into vacuum is introduced as electron generation step, followed by vacuum acceleration in the laser field and re-entrance into the target to generate characteristic x-rays and Bremsstrahlung. For negligible space charge in vacuum, the Kα flux is proportional to the incident intensity and the wavelength squared, suggesting a strong enhancement of the x-ray flux by mid-infrared driving pulses. This prediction is in quantitative agreement with experiments on femtosecond Cu Kα generation.
- ItemSoft-mode driven polarity reversal in ferroelectrics mapped by ultrafast x-ray diffraction(Melville, NY : AIP Publishing LLC, 2018) Hauf, Christoph; Hernandez Salvador, Antonio-Andres; Holtz, Marcel; Woerner, Michael; Elsaesser, ThomasQuantum theory has linked microscopic currents and macroscopic polarizations of ferroelectrics, but the interplay of lattice excitations and charge dynamics on atomic length and time scales is an open problem. Upon phonon excitation in the prototypical ferroelectric ammonium sulfate [(NH4)2SO4], we determine transient charge density maps by femtosecond x-ray diffraction. A newly discovered low frequency-mode with a 3 ps period and sub-picometer amplitudes induces periodic charge relocations over some 100 pm, a hallmark of soft-mode behavior. The transient charge density allows for deriving the macroscopic polarization, showing a periodic reversal of polarity.
- ItemPhonon driven charge dynamics in polycrystalline acetylsalicylic acid mapped by ultrafast x-ray diffraction(Melville, NY : AIP Publishing LLC, 2019) Hauf, Christoph; Hernandez Salvador, Antonio-Andres; Holtz, Marcel; Woerner, Michael; Elsaesser, ThomasThe coupled lattice and charge dynamics induced by phonon excitation in polycrystalline acetylsalicylic acid (aspirin) are mapped by femtosecond x-ray powder diffraction. The hybrid-mode character of the 0.9 ± 0.1 THz methyl rotation in the aspirin molecules is evident from collective charge relocations over distances of some 100 pm, much larger than the sub-picometer nuclear displacements. Oscillatory charge relocations around the methyl group generate a torque on the latter, thus coupling electronic and nuclear motions.
- ItemField-Induced Tunneling Ionization and Terahertz-Driven Electron Dynamics in Liquid Water(Washington, DC : ACS, 2020) Ghalgaoui, Ahmed; Koll, Lisa-Marie; Schütte, Bernd; Fingerhut, Benjamin P.; Reimann, Klaus; Woerner, Michael; Elsaesser, ThomasLiquid water at ambient temperature displays ultrafast molecular motions and concomitant fluctuations of very strong electric fields originating from the dipolar H2O molecules. We show that such random intermolecular fields induce the tunnel ionization of water molecules, which becomes irreversible if an external terahertz (THz) pulse imposes an additional directed electric field on the liquid. Time-resolved nonlinear THz spectroscopy maps charge separation, transport, and localization of the released electrons on a few-picosecond time scale. The highly polarizable localized electrons modify the THz absorption spectrum and refractive index of water, a manifestation of a highly nonlinear response. Our results demonstrate how the interplay of local electric field fluctuations and external electric fields allows for steering charge dynamics and dielectric properties in aqueous systems. Copyright © 2020 American Chemical Society.
- ItemTwo-color two-dimensional terahertz spectroscopy: A new approach for exploring even-order nonlinearities in the nonperturbative regime(Melville, NY : American Institute of Physics, 2021) Woerner, Michael; Ghalgaoui, Ahmed; Reimann, Klaus; Elsaesser, ThomasNonlinear two-dimensional terahertz (2D-THz) spectroscopy at frequencies of the emitted THz signal different from the driving frequencies allows for exploring the regime of (off-)resonant even-order nonlinearities in condensed matter. To demonstrate the potential of this method, we study two phenomena in the nonlinear THz response of bulk GaAs: (i) The nonlinear THz response to a pair of femtosecond near-infrared pulses unravels novel fourth- and sixth-order contributions involving interband shift currents, Raman-like excitations of transverse-optical phonon and intervalence-band coherences. (ii) Transient interband tunneling of electrons driven by ultrashort mid-infrared pulses can be effectively controlled by a low-frequency THz field with amplitudes below 50 kV/cm. The THz field controls the electron–hole separation modifying decoherence and the irreversibility of carrier generation.