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- 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.
- ItemMapping the Dissociative Ionization Dynamics of Molecular Nitrogen with Attosecond Time Resolution(College Park, Md. : APS, 2015) Trabattoni, A.; Klinker, M.; González-Vázquez, J.; Liu, C.; Sansone, G.; Linguerri, R.; Hochlaf, M.; Klei, J.; Vrakking, M. J. J.; Martín, F.; Nisoli, M.; Calegari, F.Studying the interaction of molecular nitrogen with extreme ultraviolet (XUV) radiation is of prime importance to understand radiation-induced processes occurring in Earth’s upper atmosphere. In particular, photoinduced dissociation dynamics involving excited states of N2+ leads to N and N+ atomic species that are relevant in atmospheric photochemical processes. However, tracking the relaxation dynamics of highly excited states of N2+ is difficult to achieve, and its theoretical modeling is notoriously complex. Here, we report on an experimental and theoretical investigation of the dissociation dynamics of N2+ induced by isolated attosecond XUV pulses in combination with few-optical-cycle near-infrared/visible (NIR/VIS) pulses. The momentum distribution of the produced N+ fragments is measured as a function of pump-probe delay with subfemtosecond resolution using a velocity map imaging spectrometer. The time-dependent measurements reveal the presence of NIR/VIS-induced transitions between N2+ states together with an interference pattern that carries the signature of the potential energy curves activated by the XUV pulse. We show that the subfemtosecond characterization of the interference pattern is essential for a semiquantitative determination of the repulsive part of these curves.
- ItemDetailed characterization of electron sources yielding first demonstration of European x-ray free-electron laser beam quality(College Park, Md. : APS, 2010) Stephan, F.; Boulware, C.H.; Krasilnikov, M.; Bähr, J.; Asova, G.; Donat, A.; Gensch, U.; Grabosch, H.J.; Hänel, M.; Hakobyan, L.; Henschel, H.; Ivanisenko, Y.; Jachmann, L.; Khodyachykh, S.; Khojoyan, M.; Kohler, W.; Korepanov, S.; Koss, G.; Kretzschmann, A.; Leich, H.; Ludecke, H.; Meissner, A.; Oppelt, A.; Petrosyan, B.; Pohl, M.; Riemann, S.; Rimjaem, S.; Sachwitz, M.; Schoneich, B.; Scholz, T.; Schulze, H.; Schultze, J.; Schwendicke, U.; Shapovalov, A.; Spesyvtsev, R.; Staykov, L.; Tonisch, F.; Walter, T.; Weisse, S.; Wenndorff, R.; Winde, M.; Vu, L.V.; Durr, H.; Kamps, T.; Richter, D.; Sperling, M.; Ovsyannikov, R.; Vollmer, A.; Knobloch, J.; Jaeschke, E.; Boster, J.; Brinkmann, R.; Choroba, S.; Flechsenhar, K.; Flottmann, K.; Gerdau, W.; Katalev, V.; Koprek, W.; Lederer, S.; Martens, C.; Pucyk, P.; Schreiber, S.; Simrock, S.; Vogel, E.; Vogel, V.; Rosbach, K.; Bonev, I.; Tsakov, I.; Michelato, P.; Monaco, L.; Pagani, C.; Sertore, D.; Garvey, T.; Will, I.; Templin, I.; Sandner, W.; Ackermann, W.; Arévalo, E.; Gjonaj, E.; Muller, W.F.O.; Schnepp, S.; Weiland, T.; Wolfheimer, F.; Ronsch, J.; Rossbach, J.The photoinjector test facility at DESY, Zeuthen site (PITZ), was built to develop and optimize photoelectron sources for superconducting linacs for high-brilliance, short-wavelength free-electron laser (FEL) applications like the free-electron laser in Hamburg (FLASH) and the European x-ray free-electron laser (XFEL). In this paper, the detailed characterization of two laser-driven rf guns with different operating conditions is described. One experimental optimization of the beam parameters was performed at an accelerating gradient of about 43 MV/m at the photocathode and the other at about 60 MV/m. In both cases, electron beams with very high phase-space density have been demonstrated at a bunch charge of 1 nC and are compared with corresponding simulations. The rf gun optimized for the lower gradient has surpassed all the FLASH requirements on beam quality and rf parameters (gradient, rf pulse length, repetition rate) and serves as a spare gun for this facility. The rf gun studied with increased accelerating gradient at the cathode produced beams with even higher brightness, yielding the first demonstration of the beam quality required for driving the European XFEL: The geometric mean of the normalized projected rms emittance in the two transverse directions was measured to be 1.260±13 mmmrad for a 1-nC electron bunch. When a 10% charge cut is applied excluding electrons from those phase-space regions where the measured phase-space density is below a certain level and which are not expected to contribute to the lasing process, the normalized projected rms emittance is about 0.9 mmmrad. © 2010 The American Physical Society.
- ItemEvolution of a molecular shape resonance along a stretching chemical bond(College Park, Md. : APS, 2020) Brausse, Felix; Bach, Florian; Krečinić, Faruk; Vrakking, Marc J.J.; Rouzée, ArnaudWe report experiments on laser-assisted electron recollisions that result from strong-field ionization of photoexcited I2 molecules in the regime of low-energy electron scattering (<25 eV impact energy). By comparing differential scattering cross sections extracted from the angle-resolved photoelectron spectra to differential scattering cross sections from quantum-scattering calculations, we demonstrate that the electron-scattering dynamics is dominated by a shape resonance. When the molecular bond stretches during the evolution of a vibrational wave packet this shape resonance shifts to lower energies, both in experiment and theory. We explain this behavior by the nature of the resonance wave function, which closely resembles an antibonding molecular orbital of I2.
- ItemUltrafast Optically Induced Ferromagnetic State in an Elemental Antiferromagnet(College Park, Md. : APS, 2021) Golias, E.; Kumberg, I.; Gelen, I.; Thakur, S.; Gördes, J.; Hosseinifar, R.; Guillet, Q.; Dewhurst, J.K.; Sharma, S.; Schüßler-Langeheine, C.; Pontius, N.; Kuch, W.We present evidence for an ultrafast optically induced ferromagnetic alignment of antiferromagnetic Mn in Co/Mn multilayers. We observe the transient ferromagnetic signal at the arrival of the pump pulse at the Mn L3 resonance using x-ray magnetic circular dichroism in reflectivity. The timescale of the effect is comparable to the duration of the excitation and occurs before the magnetization in Co is quenched. Theoretical calculations point to the imbalanced population of Mn unoccupied states caused by the Co interface for the emergence of this transient ferromagnetic state.
- ItemTwo-Dimensional Partial-Covariance Mass Spectrometry of Large Molecules Based on Fragment Correlations(College Park, Md. : APS, 2020) Driver, Taran; Cooper, Bridgette; Ayers, Ruth; Pipkorn, Rüdiger; Patchkovskii, Serguei; Averbukh, Vitali; Klug, David R.; Marangos, Jon P.; Frasinski, Leszek J.; Edelson-Averbukh, MarinaCovariance mapping [L. J. Frasinski, K. Codling, and P. A. Hatherly, Science 246, 1029 (1989)] is a well-established technique used for the study of mechanisms of laser-induced molecular ionization and decomposition. It measures statistical correlations between fluctuating signals of pairs of detected species (ions, fragments, electrons). A positive correlation identifies pairs of products originating from the same dissociation or ionization event. A major challenge for covariance-mapping spectroscopy is accessing decompositions of large polyatomic molecules, where true physical correlations are overwhelmed by spurious signals of no physical significance induced by fluctuations in experimental parameters. As a result, successful applications of covariance mapping have so far been restricted to low-mass systems, e.g., organic molecules of around 50 daltons (Da). Partial-covariance mapping was suggested to tackle the problem of spurious correlations by taking into account the independently measured fluctuations in the experimental conditions. However, its potential has never been realized for the decomposition of large molecules, because in these complex situations, determining and continuously monitoring multiple experimental parameters affecting all the measured signals simultaneously becomes unfeasible. We introduce, through deriving theoretically and confirming experimentally, a conceptually new type of partial-covariance mapping—self-correcting partial-covariance spectroscopy—based on a parameter extracted from the measured spectrum itself. We use the readily available total ion count as the self-correcting partial-covariance parameter, thus eliminating the challenge of determining experimental parameter fluctuations in covariance measurements of large complex systems. The introduced self-correcting partial covariance enables us to successfully resolve correlations of molecules as large as 103–104 Da, 2 orders of magnitude above the state of the art. This opens new opportunities for mechanistic studies of large molecule decompositions through revealing their fragment-fragment correlations. Moreover, we demonstrate that self-correcting partial covariance is applicable to solving the inverse problem: reconstruction of a molecular structure from its fragment spectrum, within two-dimensional partial-covariance mass spectrometry.
- ItemThree-Dimensional Shapes of Spinning Helium Nanodroplets(College Park, Md. : APS, 2018) Langbehn, Bruno; Sander, Katharina; Ovcharenko, Yevheniy; Peltz, Christian; Clark, Andrew; Coreno, Marcello; Cucini, Riccardo; Drabbels, Marcel; Finetti, Paola; Di Fraia, Michele; Giannessi, Luca; Grazioli, Cesare; Iablonskyi, Denys; LaForge, Aaron C.; Nishiyama, Toshiyuki; Oliver Álvarez de Lara, Verónica; Piseri, Paolo; Plekan, Oksana; Ueda, Kiyoshi; Zimmermann, Julian; Prince, Kevin C.; Stienkemeier, Frank; Callegari, Carlo; Fennel, Thomas; Rupp, Daniela; Möller, ThomasA significant fraction of superfluid helium nanodroplets produced in a free-jet expansion has been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large data set allows us to follow the evolution from axisymmetric oblate to triaxial prolate and two-lobed droplets. We find that the shapes of spinning superfluid helium droplets exhibit the same stages as classical rotating droplets while the previously reported metastable, oblate shapes of quantum droplets are not observed. Our three-dimensional analysis represents a valuable landmark for clarifying the interrelation between morphology and superfluidity on the nanometer scale.
- ItemAttosecond electron spectroscopy using a novel interferometric pump-probe technique(College Park, Md. : APS, 2010) Mauritsson, J.; Remetter, T.; Swoboda, M.; Klünder, K.; L'Huillier, A.; Schafer, K.J.; Ghafur, O.; Kelkensberg, F.; Siu, W.; Johnsson, P.; Vrakking, M.J.J.; Znakovskaya, I.; Uphues, T.; Zherebtsov, S.; Kling, M.F.; Lépine, F.; Benedetti, E.; Ferrari, F.; Sansone, G.; Nisoli, M.We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse (AP) with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original AP. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multipath interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the AP duration. © 2010 The American Physical Society.
- ItemUltrafast Demagnetization Dominates Fluence Dependence of Magnetic Scattering at Co M Edges(College Park, Md. : APS, 2020) Schneider, Michael; Pfau, Bastian; Günther, Christian M.; von Korff Schmising, Clemens; Weder, David; Geilhufe, Jan; Perron, Jonathan; Capotondi, Flavio; Pedersoli, Emanuele; Manfredda, Michele; Hennecke, Martin; Vodungbo, Boris; Lüning, Jan; Eisebitt, StefanWe systematically study the fluence dependence of the resonant scattering cross-section from magnetic domains in Co/Pd-based multilayers. Samples are probed with single extreme ultraviolet (XUV) pulses of femtosecond duration tuned to the Co M3,2 absorption resonances using the FERMI@Elettra free-electron laser. We report quantitative data over 3 orders of magnitude in fluence, covering 16 mJ/cm2/pulse to 10 000 mJ/cm2/pulse with pulse lengths of 70 fs and 120 fs. A progressive quenching of the diffraction cross-section with fluence is observed. Compression of the same pulse energy into a shorter pulse—implying an increased XUV peak electric field—results in a reduced quenching of the resonant diffraction at the Co M3,2 edge. We conclude that the quenching effect observed for resonant scattering involving the short-lived Co 3p core vacancies is noncoherent in nature. This finding is in contrast to previous reports investigating resonant scattering involving the longer-lived Co 2p states, where stimulated emission has been found to be important. A phenomenological model based on XUV-induced ultrafast demagnetization is able to reproduce our entire set of experimental data and is found to be consistent with independent magneto-optical measurements of the demagnetization dynamics on the same samples.