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- ItemDifferential Cross Sections for the H + D2 → HD(v′ = 3, j′ = 4-10) + D Reaction above the Conical Intersection(Washington, DC : Soc., 2015) Gao, Hong; Sneha, Mahima; Bouakline, Foudhil; Althorpe, Stuart C.; Zare, Richard N.We report rovibrationally selected differential cross sections (DCSs) of the benchmark reaction H + D2 → HD(v′ = 3, j′ = 4–10) + D at a collision energy of 3.26 eV, which exceeds the conical intersection of the H3 potential energy surface at 2.74 eV. We use the PHOTOLOC technique in which a fluorine excimer laser at 157.64 nm photodissociates hydrogen bromide (HBr) molecules to generate fast H atoms and the HD product is detected in a state-specific manner by resonance-enhanced multiphoton ionization. Fully converged quantum wave packet calculations were performed for this reaction at this high collision energy without inclusion of the geometric phase (GP) effect, which takes into account coupling to the first excited state of the H3 potential energy surface. Multimodal structures can be observed in most of the DCSs up to j′ = 10, which is predicted by theory and also well-reproduced by experiment. The theoretically calculated DCSs are in good overall agreement with the experimental measurements, which indicates that the GP effect is not large enough that its existence can be verified experimentally at this collision energy.
- ItemSemiconductor saturable absorber mirror mode-locked Yb:YAP laser(Washington, DC : Soc., 2022) Lin, Zhang-Lang; Xue, Wen-Ze; Zeng, Huang-Jun; Zhang, Ge; Zhao, Yongguang; Xu, Xiaodong; Xu, Jun; Loiko, Pavel; Mateos, Xavier; Lin, Haifeng; Petrov, Valentin; Wang, Li; Chen, WeidongWe report on sub-30 fs pulse generation from a semiconductor saturable absorber mirror mode-locked Yb:YAP laser. Pumping by a spatially single-mode Yb fiber laser at 979 nm, soliton pulses as short as 29 fs were generated at 1091 nm with an average output power of 156 mW and a pulse repetition rate of 85.1 MHz. The maximum output power of the mode-locked Yb:YAP laser amounted to 320 mW for slightly longer pulses (32 fs) at an incident pump power of 1.52 W, corresponding to a peak power of 103 kW and an optical efficiency of 20.5%. To the best of our knowledge, this result represents the shortest pulses ever achieved from any solid-state Yb laser mode-locked by a slow, i.e., physical saturable absorber.
- ItemMagnesium Contact Ions Stabilize the Tertiary Structure of Transfer RNA: Electrostatics Mapped by Two-Dimensional Infrared Spectra and Theoretical Simulations(Washington, DC : Soc., 2021) Schauss, Jakob; Kundu, Achintya; Fingerhut, Benjamin P.; Elsaesser, ThomasIons interacting with hydrated RNA play a central role in defining its secondary and tertiary structure. While spatial arrangements of ions, water molecules, and phosphate groups have been inferred from X-ray studies, the role of electrostatic and other noncovalent interactions in stabilizing compact folded RNA structures is not fully understood at the molecular level. Here, we demonstrate that contact ion pairs of magnesium (Mg2+) and phosphate groups embedded in local water shells stabilize the tertiary equilibrium structure of transfer RNA (tRNA). Employing dialyzed tRNAPhe from yeast and tRNA from Escherichia coli, we follow the population of Mg2+ sites close to phosphate groups of the ribose-phosphodiester backbone step by step, combining linear and nonlinear infrared spectroscopy of phosphate vibrations with molecular dynamics simulations and ab initio vibrational frequency calculations. The formation of up to six Mg2+/phosphate contact pairs per tRNA and local field-induced reorientations of water molecules balance the phosphate-phosphate repulsion in nonhelical parts of tRNA, thus stabilizing the folded structure electrostatically. Such geometries display limited sub-picosecond fluctuations in the arrangement of water molecules and ion residence times longer than 1 µs. At higher Mg2+ excess, the number of contact ion pairs per tRNA saturates around 6 and weakly interacting ions prevail. Our results suggest a predominance of contact ion pairs over long-range coupling of the ion atmosphere and the biomolecule in defining and stabilizing the tertiary structure of tRNA. © 2020 American Chemical Society.
- Item8 fs laser pulses from a compact gas-filled multi-pass cell(Washington, DC : Soc., 2021) Rueda, P.; Videla, F.; Witting, T.; Torchia, G.A.; Furch, F.J.Compression of 42 fs, 0.29 mJ pulses from a Ti:Sapphire amplifier down to 8 fs (approximately 3 optical cycles) is demonstrated by means of spectral broadening in a compact multi-pass cell filled with argon. The efficiency of the nonlinear pulse compression is limited to 45 % mostly by losses in the mirrors of the cell. The experimental results are supported by 3-dimensional numerical simulations of the nonlinear pulse propagation in the cell that allow us to study spatio-spectral properties of the pulses after spectral broadening.
- ItemTowards Poisson noise limited optical pump soft X-ray probe NEXAFS spectroscopy using a laser-produced plasma source: erratum(Washington, DC : Soc., 2021) Jonas, Adrian; Stiel, Holger; Glöggler, Lisa; Dahm, Diana; Dammer, Katharina; Kanngießer, Birgit; Mantouvalou, IoannaWe provide corrections for our previous publication [Opt. Express27, 36524 (2019)10.1364/OE.27.036524].
- ItemSub-7 fs radially-polarized pulses by post-compression in thin fused silica plates(Washington, DC : Soc., 2021) Cao, Huabao; Nagymihaly, Roland S.; Khodakovskiy, Nikita; Pajer, Viktor; Bohus, Janos; Lopez-Martens, Rodrigo; Borzsonyi, Adam; Kalashnikov, MikhailWe experimentally demonstrate the post-compression of radially polarized 25 fs pulses at 800 nm central wavelength in a multiple thin plate arrangement for the first time, to the best of our knowledge. Sub-7 fs pulses with 90 µJ energy were obtained after dispersion compensation, corresponding to a compression factor of more than 3.5. Preservation of radial polarization state was confirmed by polarized intensity distribution measurements. Linear projections of the radially polarized pulses were also fully characterized in the temporal domain.
- ItemPhosphate Vibrations Probe Electric Fields in Hydrated Biomolecules: Spectroscopy, Dynamics, and Interactions(Washington, DC : Soc., 2021) Elsaesser, Thomas; Schauss, Jakob; Kundu, Achintya; Fingerhut, Benjamin P.Electric interactions have a strong impact on the structure and dynamics of biomolecules in their native water environment. Given the variety of water arrangements in hydration shells and the femto- to subnanosecond time range of structural fluctuations, there is a strong quest for sensitive noninvasive probes of local electric fields. The stretching vibrations of phosphate groups, in particular the asymmetric (PO2)− stretching vibration νAS(PO2)−, allow for a quantitative mapping of dynamic electric fields in aqueous environments via a field-induced redshift of their transition frequencies and concomitant changes of vibrational line shapes. We present a systematic study of νAS(PO2)− excitations in molecular systems of increasing complexity, including dimethyl phosphate (DMP), short DNA and RNA duplex structures, and transfer RNA (tRNA) in water. A combination of linear infrared absorption, two-dimensional infrared (2D-IR) spectroscopy, and molecular dynamics (MD) simulations gives quantitative insight in electric-field tuning rates of vibrational frequencies, electric field and fluctuation amplitudes, and molecular interaction geometries. Beyond neat water environments, the formation of contact ion pairs of phosphate groups with Mg2+ ions is demonstrated via frequency upshifts of the νAS(PO2)− vibration, resulting in a distinct vibrational band. The frequency positions of contact geometries are determined by an interplay of attractive electric and repulsive exchange interactions.
- ItemSingleshot polychromatic coherent diffractive imaging with a high-order harmonic source(Washington, DC : Soc., 2020) Malm, Erik; Wikmark, Hampus; Pfau, Bastian; Villanueva-Perez, Pablo; Rudawski, Piotr; Peschel, Jasper; Maclot, Sylvain; Schneider, Michael; Eisebitt, Stefan; Mikkelsen, Anders; L’Huillier, Anne; Johnsson, PerSingleshot polychromatic coherent diffractive imaging is performed with a high-intensity high-order harmonic generation source. The coherence properties are analyzed and several reconstructions show the shot-to-shot fluctuations of the incident beam wavefront. The method is based on a multi-step approach. First, the spectrum is extracted from double-slit diffraction data. The spectrum is used as input to extract the monochromatic sample diffraction pattern, then phase retrieval is performed on the quasi-monochromatic data to obtain the sample’s exit surface wave. Reconstructions based on guided error reduction (ER) and alternating direction method of multipliers (ADMM) are compared. ADMM allows additional penalty terms to be included in the cost functional to promote sparsity within the reconstruction. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.
- ItemSub-15-fs X-ray pump and X-ray probe experiment for the study of ultrafast magnetization dynamics in ferromagnetic alloys(Washington, DC : Soc., 2021) Liu, Xuan; Merhe, Alaaeldine; Jal, Emmanuelle; Delaunay, Renaud; Jarrier, Romain; Chardonnet, Valentin; Hennes, Marcel; Chiuzbaian, Sorin G.; Légaré, Katherine; Hennecke, Martin; Radu, Ilie; Von Korff Schmising, Clemens; Grunewald, Særen; Kuhlmann, Marion; Lüning, Jan; Vodungbo, BorisIn this paper, we present a new setup for the measurement of element-specific ultrafast magnetization dynamics in ferromagnetic thin films with a sub-15-fs time resolution. Our experiment relies on a split and delay approach which allows us to fully exploit the shortest X-rays pulses delivered by X-ray Free Electrons Lasers (close to the attosecond range), in an X-ray pump – X-ray probe geometry. The setup performance is demonstrated by measuring the ultrafast elemental response of Ni and Fe during demagnetization of ferromagnetic Ni and Ni80Fe20 (Permalloy) samples upon resonant excitation at the corresponding absorption edges. The transient demagnetization process is measured in both reflection and transmission geometry using, respectively, the transverse magneto-optical Kerr effect (T-MOKE) and the Faraday effect as probing mechanisms.
- ItemTerahertz absorption-saturation and emission from electron-doped germanium quantum wells(Washington, DC : Soc., 2020) Ciano, Chiara; Virgilio, Michele; Bagolini, Luigi; Baldassarre, Leonetta; Pashkin, Alexej; Helm, Manfred; Montanari, Michele; Persichetti, Luca; Di Gaspare, Luciana; Capellini, Giovanni; Paul, Douglas J.; Scalari, Giacomo; Faist, Jèrome; De Seta, Monica; Ortolani, MicheleWe study radiative relaxation at terahertz frequencies in n-type Ge/SiGe quantum wells, optically pumped with a terahertz free electron laser. Two wells coupled through a tunneling barrier are designed to operate as a three-level laser system with non-equilibrium population generated by optical pumping around the 1→3 intersubband transition at 10 THz. The non-equilibrium subband population dynamics are studied by absorption-saturation measurements and compared to a numerical model. In the emission spectroscopy experiment, we observed a photoluminescence peak at 4 THz, which can be attributed to the 3→2 intersubband transition with possible contribution from the 2→1 intersubband transition. These results represent a step towards silicon-based integrated terahertz emitters.