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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.
- ItemThin-disk laser-pumped OPCPA system delivering 4.4 TW few-cycle pulses(Washington, DC : Soc., 2020) Kretschmar, Martin; Tuemmler, Johannes; Schütte, Bernd; Hoffmann, Andreas; Senfftleben, Björn; Mero, Mark; Sauppe, Mario; Rupp, Daniela; Vrakking, Marc J.J.; Will, Ingo; Nagy, TamasWe present an optical parametric chirped pulse amplification (OPCPA) system delivering 4.4 TW pulses centered at 810 nm with a sub-9 fs duration and a carrier-envelope phase stability of 350 mrad. The OPCPA setup pumped by sub-10 ps pulses from two Yb:YAG thin-disk lasers at 100 Hz repetition rate is optimized for a high conversion-efficiency. The terawatt pulses of the OPCPA are utilized for generating intense extreme ultraviolet (XUV) pulses by high-order harmonic generation, achieving XUV pulse energies approaching the microjoule level. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
- ItemSESAM mode-locked Tm:Y2O3 ceramic laser(Washington, DC : Soc., 2022) Zhang, Ning; Liu, Shande; Wang, Zhanxin; Liu, Jian; Xu, Xiaodong; Xu, Jun; Wang, Jun; Liu, Peng; Ma, Jie; Shen, Deyuan; Tang, Dingyuan; Lin, Hui; Zhang, Jian; Chen, Weidong; Zhao, Yongguang; Griebner, Uwe; Petrov, ValentinWe demonstrate a widely tunable and passively mode-locked Tm:Y2O3 ceramic laser in-band pumped by a 1627-nm Raman fiber laser. A tuning range of 318 nm, from 1833 to 2151 nm, is obtained in the continuous-wave regime. The SESAM mode-locked laser produces Fourier-transform-limited pulses as short as 75 fs at ∼ 2.06 µm with an average output power of 0.26 W at 86.3 MHz. For longer pulse durations of 178 fs, an average power of 0.59 W is achieved with a laser efficiency of 29%. This is, to the best of our knowledge, the first mode-locked Tm:Y2O3 laser in the femtosecond regime. The spectroscopic properties and laser performance confirm that Tm:Y2O3 transparent ceramics are a promising gain material for ultrafast lasers at 2 µm.
- ItemReference shape effects on Fourier transform holography(Washington, DC : Soc., 2022) Malm, Erik; Pfau, Bastian; Schneider, Michael; Günther, Christian M.; Hessing, Piet; Büttner, Felix; Mikkelsen, Anders; Eisebitt, StefanSoft-x-ray holography which utilizes an optics mask fabricated in direct contact with the sample, is a widely applied x-ray microscopy method, in particular, for investigating magnetic samples. The optics mask splits the x-ray beam into a reference wave and a wave to illuminate the sample. The reconstruction quality in such a Fourier-transform holography experiment depends primarily on the characteristics of the reference wave, typically emerging from a small, high-aspect-ratio pinhole in the mask. In this paper, we study two commonly used reference geometries and investigate how their 3D structure affects the reconstruction within an x-ray Fourier holography experiment. Insight into these effects is obtained by imaging the exit waves from reference pinholes via high-resolution coherent diffraction imaging combined with three-dimensional multislice simulations of the x-ray propagation through the reference pinhole. The results were used to simulate Fourier-transform holography experiments to determine the spatial resolution and precise location of the reconstruction plane for different reference geometries. Based on our findings, we discuss the properties of the reference pinholes with view on application in soft-x-ray holography experiments.
- 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.
- 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.
- ItemPropagator operator for pulse propagation in resonant media(Washington, DC : Soc., 2021) Morales, Felipe; Richter, Maria; Olvo, Vlad; Husakou, AntonWe show that, for the case of resonant media, the available models for unidirectional propagation of short pulses can face serious challenges with respect to numerical efficiency, accuracy, or numerical artifacts. We propose an alternative approach based on a propagator operator defined in the time domain. This approach enables precise simulations using short time windows even for resonant media and facilitates coupling of the propagation equation with first-principle methods such as the time-dependent Schödinger equation. Additionally, we develop a numerically efficient recipe to construct and apply such a propagator operator.
- ItemCross-polarized common-path temporal interferometry for high-sensitivity strong-field ionization measurements(Washington, DC : Soc., 2022) Nie, Zan; Nambu, Noa; Marsh, Kenneth A.; Welch, Eric; Matteo, Daniel; Zhang, Chaojie; Wu, Yipeng; Patchkovskii, Serguei; Morales, Felipe; Smirnova, Olga; Joshi, ChanAbsolute density measurements of low-ionization-degree or low-density plasmas ionized by lasers are very important for understanding strong-field physics, atmospheric propagation of intense laser pulses, Lidar etc. A cross-polarized common-path temporal interferometer using balanced detection was developed for measuring plasma density with a sensitivity of ∼0.6 mrad, equivalent to a plasma density-length product of ∼2.6 × 1013 cm-2 if using an 800 nm probe laser. By using this interferometer, we have investigated strong-field ionization yield versus intensity for various noble gases (Ar, Kr, and Xe) using 800 nm, 55 fs laser pulses with both linear (LP) and circular (CP) polarization. The experimental results were compared to the theoretical models of Ammosov-Delone-Krainov (ADK) and Perelomov-Popov-Terent'ev (PPT). We find that the measured phase change induced by plasma formation can be explained by the ADK theory in the adiabatic tunneling ionization regime, while PPT model can be applied to all different regimes. We have also measured the photoionization and fractional photodissociation of molecular (MO) hydrogen. By comparing our experimental results with PPT and MO-PPT models, we have determined the likely ionization pathways when using three different pump laser wavelengths of 800 nm, 400 nm, and 267 nm.
- Item43 W, 1.55 μm and 12.5 W, 3.1 μm dual-beam, sub-10 cycle, 100 kHz optical parametric chirped pulse amplifier(Washington, DC : Soc., 2018) Mero, Mark; Heiner, Zsuzsanna; Petrov, Valentin; Rottke, Horst; Branchi, Federico; Thomas, Gabrielle M.; Vrakking, Marc J. J.We present a 100 kHz optical parametric chirped pulse amplifier (OPCPA) developed for strong-field attosecond physics and soft-x-ray transient absorption experiments. The system relies on noncollinear potassium titanyl arsenate booster OPCPAs and is pumped by a 244 W, 1.1 ps Yb:YAG Innoslab chirped pulse laser amplifier. Two optically synchronized infrared output beams are simultaneously available: a 430 μJ, 51 fs, carrier-envelope phase stable beam at 1.55 μm and an angular-dispersion-compensated, 125 μJ, 73 fs beam at 3.1 μm.