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- ItemEffect of synthesis catalyst on structure of nitrogen-doped carbon nanotubes and electrical conductivity and electromagnetic interference shielding of their polymeric nanocomposites(New York, NY [u.a.] : Pergamon Press, 2016) Arjmand, Mohammad; Chizari, Kambiz; Krause, Beate; Pötschke, Petra; Sundararaj, UttandaramanDifferent catalysts including Co, Fe, and Ni were used to synthesize nitrogen-doped carbon nanotubes (N-CNTs) by chemical vapor deposition technique. Synthesized N-CNTs were melt mixed with a polyvinylidene fluoride (PVDF) matrix using a small scale mixer at different concentrations ranging from 0.3 to 3.5 wt%, and then compression molded. The characterization techniques revealed significant differences in the synthesis yield and the morphological and electrical properties of both N-CNTs and nanocomposites depending on the catalyst type. Whereas Co and Fe resulted in yields comparable to industrial multiwalled CNTs, Ni was much less effective. The N-CNT aspect ratio was the highest for Co catalyst, followed by Ni and Fe, whereas nitrogen content was the highest for Ni. Raman spectroscopy revealed lowest defect number and highest N-CNT crystallinity for Fe catalyst. Characterization of N-CNT/PVDF nanocomposites showed better dispersion for N-CNTs based on Co and Fe as compared to Ni, and the following order of electrical conductivity and electromagnetic interference shielding (from high to low): Co > Fe > Ni. The superior electrical properties of (N-CNT)Co nanocomposites were ascribed to a combination of high synthesis yield, high aspect ratio, low nitrogen content and high crystallinity of N-CNTs combined with a good state of N-CNT dispersion.
- ItemObservation of discrete, vortex light bullets(College Park : American Institute of Physics Inc., 2014) Eilenberger, F.; Prater, K.; Minardi, S.; Geiss, R.; Röpke, U.; Kobelke, J.; Schuster, K.; Bartelt, H.; Nolte, S.; Tünnermann, A.; Pertsch, T.We report the first experimental observation of vortex light bullets that are discrete, spatiotemporal, solitary waves with orbital angular momentum. We analyze conditions for their existence and investigate their rich properties and dynamics. Vortex light bullets are excited in fiber arrays with spatially shaped femtosecond pulses and analyzed with a spatiotemporal cross correlator. Most importantly, we find that they have entirely new stability properties, being robust against considerable degrees of perturbation in a limited range of energies. All experimental findings are backed up by rigorous simulations, giving further insight into the rich dynamics of vortex light bullets.
- ItemFew-cycle 65-µJ pulses at 11.4 µm for ultrafast nonlinear longwave-infrared spectroscopy(Washington, DC : Optical Society of America, OSA, 2022) Fuertjes, Pia; Bock, Martin; Grafenstein, Lorenz von; Ueberschaer, Dennis; Griebner, Uwe; Elsaesser, ThomasLow-energy excitations can provide insight into the basic ultrafast nonequilibrium dynamics of condensed matter. High-energy femtosecond pulses in the long-wavelength infrared are required to induce such processes, and can be generated in an optical parametric chirped pulse amplification (OPCPA) system comprising three GaSe stages. A femtosecond Cr:ZnS laser serves as the front-end, providing the seed for the 2.0-µm pump and the 2.4-µm signal pulses without nonlinear conversion processes. The OPCPA system is pumped at 2.05 µm by a picosecond Ho:YLF regenerative amplifier at a 1-kHz repetition rate. The recompressed idler pulses at 11.4 µm have a duration of 185 fs and an unprecedented energy of 65 µJ, corresponding to a pump-to-idler conversion efficiency of 1.2%. Nonlinear transmission experiments in the range of the L2 infrared band of liquid water demonstrate the potential of the pulses for nonlinear vibrational spectroscopy of liquids and solids.
- ItemTm3+-doped calcium lithium tantalum gallium garnet (Tm:CLTGG): novel laser crystal(Washington, DC : OSA, 2021) Alles, Adrian; Pan, Zhongben; Loiko, Pavel; Serres, Josep Maria; Slimi, Sami; Yingming, Shawuti; Tang, Kaiyang; Wang, Yicheng; Zhao, Yongguang; Dunina, Elena; Kornienko, Alexey; Camy, Patrice; Chen, Weidong; Wang, Li; Griebner, Uwe; Petrov, Valentin; Solé, Rosa Maria; Aguiló, Magdalena; Díaz, Francesc; Mateos, XavierWe report on the development of a novel laser crystal with broadband emission properties at ∼2 µm – a Tm3+,Li+-codoped calcium tantalum gallium garnet (Tm:CLTGG). The crystal is grown by the Czochralski method. Its structure (cubic, sp. gr. 𝐼𝑎3¯𝑑, a = 12.5158(0) Å) is refined by the Rietveld method. Tm:CLTGG exhibits a relatively high thermal conductivity of 4.33 Wm-1K-1. Raman spectroscopy confirms a weak concentration of vacancies due to the charge compensation provided by Li+ codoping. The transition probabilities of Tm3+ ions are determined using the modified Judd-Ofelt theory yielding the intensity parameters Ω2 = 5.185, Ω4 = 0.650, Ω6 = 1.068 [10−20 cm2] and α = 0.171 [10−4 cm]. The crystal-field splitting of the Tm3+ multiplets is revealed at 10 K. The first diode-pumped Tm:CLTGG laser generates 1.08 W at ∼2 µm with a slope efficiency of 23.8%. The Tm3+ ions in CLTGG exhibit significant inhomogeneous spectral broadening due to the structure disorder (a random distribution of Ta5+ and Ga3+ cations over octahedral and tetrahedral lattice sites) leading to smooth and broad gain profiles (bandwidth: 130 nm) extending well above 2 µm and rendering Tm:CLTGG suitable for femtosecond pulse generation.
- ItemDiode-pumped sub-50-fs Kerr-lens mode-locked Yb:GdYCOB laser(Washington, DC : Soc., 2021) Zeng, Huangjun; Lin, Haifeng; Lin, Zhanglang; Zhang, Lizhen; Lin, Zhoubin; Zhang, Ge; Petrov, Valentin; Loiko, Pavel; Mateos, Xavier; Wang, Li; Chen, WeidongWe present a sub-50-fs diode-pumped Kerr-lens mode-locked laser employing a novel “mixed” monoclinic Yb:Ca4(Gd,Y)O(BO3)3 (Yb:GdYCOB) crystal as a gain medium. Nearly Fourier-limited pulses as short as 43 fs at 1036.7 nm are generated with an average power of 84 mW corresponding to a pulse repetition rate of ∼70.8 MHz. A higher average power of 300 mW was achieved at the expense of the pulse duration (113 fs) corresponding to an optical-to-optical efficiency of 35.8% representing a record-high value for any Yb-doped borate crystal. Non-phase-matched self-frequency doubling is observed in the mode-locked regime with pronounced strong spectral fringes which originate from two delayed green replicas of the fundamental femtosecond pulses in the time domain.
- ItemUltrathin structures derived from interfacially modified polymeric nanocomposites to curb electromagnetic pollution(Cambridge : Royal Society of Chemistry, 2021) Sushmita, Kumari; Formanek, Petr; Fischer, Dieter; Pötschke, Petra; Madras, Giridhar; Bose, SuryasarathiThe use of electronic devices and wireless networks is increasing rapidly, and electromagnetic (EM) pollution remediation remains a challenge. We employed a unique approach to fabricate two ultrathin (approx. 53 μm) multilayered assemblies to address this. By sequentially stacking thin films of polyvinylidene difluoride (PVDF) and polycarbonate (PC) nanocomposites and interfacially locking them with a mutually miscible polymer (PMMA, polymethyl methacrylate), materials with enhanced structural properties and electromagnetic interference (EMI) shielding performance can be designed. Utilizing reduced graphene oxide (rGO) and molybdenum disulfide (MoS2) as a template, ferrite was grown on the surface to design two different nanohybrid structures (rGO–Fe3O4 and MoS2–Fe3O4). PVDF was composited with either rGO–Fe3O4 or MoS2–Fe3O4, and multiwall carbon nanotubes (CNTs) were dispersed in the PC component. As PC and PVDF are immiscible, their poor interface would result in inferior structural properties, which can be challenging in designing EMI shielding materials due to cyclic thermal fatigue. Hence, PMMA is sandwiched to interfacially stitch the components (PC and PVDF) and improve interfacial adhesion. This was confirmed using SEM/EDS and Raman mapping/imaging. The mechanical stability of the multilayered assemblies was characterized using a dynamic mechanical analyzer (DMA), and the storage modulus was found to be as high as 2767 MPa at 40 °C (@constant frequency and strain amplitude), for the multilayered film with rGO–Fe3O4 in PVDF, PMMA as a sandwich layer and CNTs in PC. A typical assembly of 9 multilayers (∼480 μm) with rGO–Fe3O4 in PVDF, and CNTs in PC, and interfacially stitched with PMMA gave rise to a high EMI shield effectiveness (SET) of −26.3 dB @ 26.5 GHz. This unique arrangement of a multilayered assembly suppressed EMI primarily by absorption.
- 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.
- ItemPhotodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization(Melville, NY : AIP Publishing LLC, 2018) Amini, Kasra; Savelyev, Evgeny; Brauße, Felix; Berrah, Nora; Bomme, Cédric; Brouard, Mark; Burt, Michael; Christensen, Lauge; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Kierspel, Thomas; Krecinic, Faruk; Lauer, Alexandra; Lee, Jason W. L.; Müller, Maria; Müller, Erland; Mullins, Terence; Redlin, Harald; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Vallance, Claire; Wiese, Joss; Johnsson, Per; Küpper, Jochen; Rudenko, Artem; Rouzée, Arnaud; Stapelfeldt, Henrik; Rolles, Daniel; Boll, RebeccaWe explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon-iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.
- ItemMonitoring conical intersections in the ring opening of furan by attosecond stimulated X-ray Raman spectroscopy(Melville, NY : AIP Publishing LLC, 2015) Hua, Weijie; Oesterling, Sven; Biggs, Jason D.; Zhang, Yu; Ando, Hideo; de Vivie-Riedle, Regina; Fingerhut, Benjamin P.; Mukamel, ShaulAttosecond X-ray pulses are short enough to capture snapshots of molecules undergoing nonadiabatic electron and nuclear dynamics at conical intersections (CoIns). We show that a stimulated Raman probe induced by a combination of an attosecond and a femtosecond pulse has a unique temporal and spectral resolution for probing the nonadiabatic dynamics and detecting the ultrafast (∼4.5 fs) passage through a CoIn. This is demonstrated by a multiconfigurational self-consistent-field study of the dynamics and spectroscopy of the furan ring-opening reaction. Trajectories generated by surface hopping simulations were used to predict Attosecond Stimulated X-ray Raman Spectroscopy signals at reactant and product structures as well as representative snapshots along the conical intersection seam. The signals are highly sensitive to the changes in nonadiabatically coupled electronic structure and geometry.