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- ItemGraphene Q-switched Yb:KYW planar waveguide laser(New York, NY : American Inst. of Physics, 2015) Kim, Jun Wan; Young Choi, Sun; Aravazhi, Shanmugam; Pollnau, Markus; Griebner, Uwe; Petrov, Valentin; Bae, Sukang; Jun Ahn, Kwang; Yeom, Dong-Il; Rotermund, FabianA diode-pumped Yb:KYW planar waveguide laser, single-mode Q-switched by evanescent-field interaction with graphene, is demonstrated for the first time. Few-layer graphene grown by chemical vapor deposition is transferred onto the top of a guiding layer, which initiates stable Q-switched operation in a 2.4-cm-long waveguide laser operating near 1027 nm. Average output powers up to 34 mW and pulse durations as short as 349 ns are achieved. The measured output beam profile, clearly exhibiting a single mode, agrees well with the theoretically calculated mode intensity distribution inside the waveguide. As the pump power is increased, the repetition rate and pulse energy increase from 191 to 607 kHz and from 7.4 to 58.6 nJ, respectively, whereas the pulse duration decreases from 2.09 μs to 349 ns.
- ItemProperties of LiGa0.5In0.5Se2: A Quaternary Chalcogenide Crystal for Nonlinear Optical Applications in the Mid-IR(Basel : MDPI, 2016) Isaenko, Ludmila; Yelisseyev, Alexander; Lobanov, Sergei; Vedenyapin, Vitaliy; Krinitsyn, Pavel; Petrov, ValentinLiGaSe2 (LGSe) and LiInSe2 (LISe) are wide band-gap nonlinear crystals transparent in the mid-IR spectral range. LiGa0.5In0.5Se2 (LGISe) is a new mixed crystal, a solid solution in the system LGSe–LISe, which exhibits the same orthorhombic structure (mm2) as the parent compounds in the same time being more technological with regard to the growth process. In comparison with LGSe and LISe its homogeneity range is broader in the phase diagram. About 10% of the Li ions in LGISe occupy octahedral positions (octapores) with coordination number of 3. The band-gap of LGISe is estimated to be 2.94 eV at room temperature and 3.04 eV at 80 K. The transparency at the 0-level extends from 0.47 to 13 µm. LGISe crystals exhibit luminescence in broad bands centered near 1.7 and 1.25 eV which is excited most effectively by band-to-band transition. From the measured principal refractive indices and the fitted Sellmeier equations second-harmonic generation from 1.75 to 11.8 μm (fundamental wavelength) is predicted. The nonlinear coefficients of LGISe have values between those of LGSe and LISe. 6LGISe crystals are considered promising also for detection of thermal neutrons.
- ItemExcited-state relaxation of hydrated thymine and thymidine measured by liquid-jet photoelectron spectroscopy: experiment and simulation(Washington, DC : ACS Publications, 2015) Buchner, Franziska; Nakayama, Akira; Yamazaki, Shohei; Ritze, Hans-Hermann; Lübcke, AndreaTime-resolved photoelectron spectroscopy is performed on thymine and thymidine in aqueous solution to study the excited-state relaxation dynamics of these molecules. We find two contributions with sub-ps lifetimes in line with recent excited-state QM/MM molecular dynamics simulations (J. Chem. Phys.2013, 139, 214304). The temporal evolution of ionization energies for the excited ππ* state along the QM/MM molecular dynamics trajectories were calculated and are compatible with experimental results, where the two contributions correspond to the relaxation paths in the ππ* state involving different conical intersections with the ground state. Theoretical calculations also show that ionization from the nπ* state is possible at the given photon energies, but we have not found any experimental indication for signal from the nπ* state. In contrast to currently accepted relaxation mechanisms, we suggest that the nπ* state is not involved in the relaxation process of thymine in aqueous solution.
- ItemPlasma rotation with circularly polarized laser pulse(London : Hindawi, 2015) Lécz, Z.; Andreev, A.; Seryi, A.The efficient transfer of angular orbital momentum from circularly polarized laser pulses into ions of solid density targets is investigated with different geometries using particle-in-cell simulations. The detailed electron and ion dynamics presented focus upon the energy and momentum conversion efficiency. It is found that the momentum transfer is more efficient for spiral targets and the maximum value is obtained when the spiral step is equal to twice the laser wavelength. This study reveals that the angular momentum distribution of ions strongly depends up on the initial target shape and density.
- ItemMultidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields(Cambridge [u.a.] : Soc., 2016) Bruner, Barry D.; Mašín, Zdeněk; Negro, Matteo; Morales, Felipe; Brambila, Danilo; Devetta, Michele; Faccialà, Davide; Harvey, Alex G.; Ivanov, Misha; Mairesse, Yann; Patchkovskii, Serguei; Serbinenko, Valeria; Soifer, Hadas; Stagira, Salvatore; Vozzi, Caterina; Dudovich, Nirit; Smirnova, OlgaHigh harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
- 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.
- ItemGraphene mode-locked Tm,Ho-codoped crystalline garnet laser producing 70-fs pulses near 21 µm(Washington, DC : OSA, 2019) Zhao, Yongguang; Chen, Weidong; Wang, Li; Wang, Yicheng; Pan, Zhongben; Dai, Xiaojun; Yuan, Hualei; Cai, Huaqiang; Zhang, Yan; Bae, Ji Eun; Park, Tae Gwan; Rotermund, Fabian; Loiko, Pavel; Serres, Josep Maria; Mateos, Xavier; Shen, Deyuan; Griebner, Uwe; Petrov, ValentinBilayer graphene synthesized by chemical vapor deposition is successfully applied as a saturable absorber (SA) for the passive mode-locking of a Tm,Ho:CLNGG laser at 2093nm. Near transform-limited pulses as short as 70 fs, i.e., 10 optical cycles, are produced at a 89 MHz repetition rate with 69 mW average output power. To the best of our knowledge, these are the shortest pulses ever reported from graphene-SA mode-locked Tm, or Ho-lasers in the 2 µm spectral region, including bulk and fiber lasers.
- ItemEvolution of planar defects during homoepitaxial growth of β-Ga2O3 layers on (100) substrates—A quantitative model(Melville, NY : American Inst. of Physics, 2016) Schewski, R.; Baldini, M.; Irmscher, K.; Fiedler, A.; Markurt, T.; Neuschulz, B.; Remmele, T.; Schulz, T.; Wagner, G.; Galazka, Z.; Albrecht, M.We study the homoepitaxial growth of β-Ga2O3 (100) grown by metal-organic vapour phase as dependent on miscut-angle vs. the c direction. Atomic force microscopy of layers grown on substrates with miscut-angles smaller than 2° reveals the growth proceeding through nucleation and growth of two-dimensional islands. With increasing miscut-angle, step meandering and finally step flow growth take place. While step-flow growth results in layers with high crystalline perfection, independent nucleation of two-dimensional islands causes double positioning on the (100) plane, resulting in twin lamellae and stacking mismatch boundaries. Applying nucleation theory in the mean field approach for vicinal surfaces, we can fit experimentally found values for the density of twin lamellae in epitaxial layers as dependent on the miscut-angle. The model yields a diffusion coefficient for Ga adatoms of D = 7 × 10−9 cm2 s−1 at a growth temperature of 850 °C, two orders of magnitude lower than the values published for GaAs.
- ItemIntracluster Coulombic decay following intense NIR ionization of clusters(Bristol : IOP Publ., 2015) Schütte, Bernd; Arbeiter, Mathias; Fennel, Thomas; Jabbari, Ghazal; Gokhberg, Kirill; Kuleff, Alexander I.; Vrakking, Marc J. J.; Rouzée, ArnaudWe report on the observation of a novel intracluster Coulombic decay process following Rydberg atom formation in clusters ionized by intense near-infrared fields. A new decay channel emerges, in which a Rydberg atom relaxes to the ground state by transferring its excess energy to a weakly bound electron in the environment that is emitted from the cluster. We find evidence for this process in the electron spectra, where a peak close to the corresponding atomic ionization potential is observed. For Ar clusters, a decay time of 87 ps is measured, which is significantly longer than in previous time-resolved studies of interatomic Coulombic decay.
- ItemXUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment([London] : Nature Publishing Group UK, 2015) Marciniak, A.; Despré, V.; Barillot, T.; Rouzée, A.; Galbraith, M.C.E.; Klei, J.; Yang, C.-H.; Smeenk, C.T.L.; Loriot, V.; Nagaprasad Reddy, S.; Tielens, A.G.G.M.; Mahapatra, S.; Kuleff, A.I.; Vrakking, M.J.J.; Lépine, F.Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.