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Start date: 2022 × Subject: electron ×

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Now showing 1 - 10 of 25
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    Single molecule level plasmonic catalysis – a dilution study of p-nitrothiophenol on gold dimers
    (Cambridge : Soc., 2015) Zhang, Zhenglong; Deckert-Gaudig, Tanja; Singh, Pushkar; Deckert, Volker
    Surface plasmons on isolated gold dimers can initiate intermolecular reactions of adsorbed p-nitrothiophenol. At the single molecule level when dimerization is not possible an intramolecular reaction can be observed. Experimental evidence indicates that plasmon-induced hot electrons provide the required activation energy.
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    Excited-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, Andrea
    Time-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.
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    Defect-free Naphthalene Diimide Bithiophene Copolymers with Controlled Molar Mass and High Performance via Direct Arylation Polycondensation
    (Washington, DC : ACS Publications, 2015) Matsidik, Rukiya; Komber, Hartmut; Luzio, Alessandro; Caironi, Mario; Sommer, Michael
    A highly efficient, simple, and environmentally friendly protocol for the synthesis of an alternating naphthalene diimide bithiophene copolymer (PNDIT2) via direct arylation polycondensation (DAP) is presented. High molecular weight (MW) PNDIT2 can be obtained in quantitative yield using aromatic solvents. Most critical is the suppression of two major termination reactions of NDIBr end groups: nucleophilic substitution and solvent end-capping by aromatic solvents via C–H activation. In situ solvent end-capping can be used to control MW by varying monomer concentration, whereby end-capping is efficient and MW is low for low concentration and vice versa. Reducing C–H reactivity of the solvent at optimized conditions further increases MW. Chain perfection of PNDIT2 is demonstrated in detail by NMR spectroscopy, which reveals PNDIT2 chains to be fully linear and alternating. This is further confirmed by investigating the optical and thermal properties as a function of MW, which saturate at Mn ≈ 20 kDa, in agreement with controls made by Stille coupling. Field-effect transistor (FET) electron mobilities μsat up to 3 cm2/(V·s) are measured using off-center spin-coating, with FET devices made from DAP PNDIT2 exhibiting better reproducibility compared to Stille controls.
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    (BB)-Carboryne Complex of Ruthenium: Synthesis by Double B-H Activation at a Single Metal Center
    (Washington, DC : ACS Publications, 2016) Eleazer, Bennett J.; Smith, Mark D.; Popov, Alexey A.; Peryshkov, Dmitry V.
    The first example of a transition metal (BB)-carboryne complex containing two boron atoms of the icosahedral cage connected to a single exohedral metal center (POBBOP)Ru(CO)2 (POBBOP = 1,7-OP(i-Pr)2-2,6-dehydro-m-carborane) was synthesized by double B-H activation within the strained m-carboranyl pincer framework. Theoretical calculations revealed that the unique three-membered (BB)>Ru metalacycle is formed by two bent B-Ru σ-bonds with the concomitant increase of the bond order between the two metalated boron atoms. The reactivity of the highly strained electron-rich (BB)-carboryne fragment with small molecules was probed by reactions with electrophiles. The carboryne-carboranyl transformations reported herein represent a new mode of cooperative metal-ligand reactivity of boron-based complexes.
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    Multidimensional 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, Olga
    High 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.
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    Tunable positions of Weyl nodes via magnetism and pressure in the ferromagnetic Weyl semimetal CeAlSi
    ([London] : Nature Publishing Group UK, 2024) Cheng, Erjian; Yan, Limin; Shi, Xianbiao; Lou, Rui; Fedorov, Alexander; Behnami, Mahdi; Yuan, Jian; Yang, Pengtao; Wang, Bosen; Cheng, Jin-Guang; Xu, Yuanji; Xu, Yang; Xia, Wei; Pavlovskii, Nikolai; Peets, Darren C.; Zhao, Weiwei; Wan, Yimin; Burkhardt, Ulrich; Guo, Yanfeng; Li, Shiyan; Felser, Claudia; Yang, Wenge; Büchner, Bernd
    The noncentrosymmetric ferromagnetic Weyl semimetal CeAlSi with simultaneous space-inversion and time-reversal symmetry breaking provides a unique platform for exploring novel topological states. Here, by employing multiple experimental techniques, we demonstrate that ferromagnetism and pressure can serve as efficient parameters to tune the positions of Weyl nodes in CeAlSi. At ambient pressure, a magnetism-facilitated anomalous Hall/Nernst effect (AHE/ANE) is uncovered. Angle-resolved photoemission spectroscopy (ARPES) measurements demonstrated that the Weyl nodes with opposite chirality are moving away from each other upon entering the ferromagnetic phase. Under pressure, by tracing the pressure evolution of AHE and band structure, we demonstrate that pressure could also serve as a pivotal knob to tune the positions of Weyl nodes. Moreover, multiple pressure-induced phase transitions are also revealed. These findings indicate that CeAlSi provides a unique and tunable platform for exploring exotic topological physics and electron correlations, as well as catering to potential applications, such as spintronics.
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    Enhancing laser beam performance by interfering intense laser beamlets
    ([London] : Nature Publishing Group UK, 2019) Morace, A.; Iwata, N.; Sentoku, Y.; Mima, K.; Arikawa, Y.; Yogo, A.; Andreev, A.; Tosaki, S.; Vaisseau, X.; Abe, Y.; Kojima, S.; Sakata, S.; Hata, M.; Lee, S.; Matsuo, K.; Kamitsukasa, N.; Norimatsu, T.; Kawanaka, J.; Tokita, S.; Miyanaga, N.; Shiraga, H.; Sakawa, Y.; Nakai, M.; Nishimura, H.; Azechi, H.; Fujioka, S.; Kodama, R.
    Increasing the laser energy absorption into energetic particle beams represents a longstanding quest in intense laser-plasma physics. During the interaction with matter, part of the laser energy is converted into relativistic electron beams, which are the origin of secondary sources of energetic ions, γ-rays and neutrons. Here we experimentally demonstrate that using multiple coherent laser beamlets spatially and temporally overlapped, thus producing an interference pattern in the laser focus, significantly improves the laser energy conversion efficiency into hot electrons, compared to one beam with the same energy and nominal intensity as the four beamlets combined. Two-dimensional particle-in-cell simulations support the experimental results, suggesting that beamlet interference pattern induces a periodical shaping of the critical density, ultimately playing a key-role in enhancing the laser-to-electron energy conversion efficiency. This method is rather insensitive to laser pulse contrast and duration, making this approach robust and suitable to many existing facilities.
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    Observation of correlated electronic decay in expanding clusters triggered by near-infrared fields
    ([London] : Nature Publishing Group UK, 2015) Schütte, B.; Arbeiter, M.; Fennel, T.; Jabbari, G.; Kuleff, A.I.; Vrakking, M.J.J.; Rouzée, A.
    When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme-ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano-scale system to intense laser light.
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    Anharmonic strong-coupling effects at the origin of the charge density wave in CsV3Sb5
    ([London] : Nature Publishing Group UK, 2024) He, Ge; Peis, Leander; Cuddy, Emma Frances; Zhao, Zhen; Li, Dong; Zhang, Yuhang; Stumberger, Romona; Moritz, Brian; Yang, Haitao; Gao, Hongjun; Devereaux, Thomas Peter; Hackl, Rudi
    The formation of charge density waves is a long-standing open problem, particularly in dimensions higher than one. Various observations in the vanadium antimonides discovered recently further underpin this notion. Here, we study the Kagome metal CsV3Sb5 using polarized inelastic light scattering and density functional theory calculations. We observe a significant gap anisotropy with 2Δmax/kBTCDW≈20, far beyond the prediction of mean-field theory. The analysis of the A1g and E2g phonons, including those emerging below TCDW, indicates strong phonon-phonon coupling, presumably mediated by a strong electron-phonon interaction. Similarly, the asymmetric Fano-type lineshape of the A1g amplitude mode suggests strong electron-phonon coupling below TCDW. The large electronic gap, the enhanced anharmonic phonon-phonon coupling, and the Fano shape of the amplitude mode combined are more supportive of a strong-coupling phonon-driven charge density wave transition than of a Fermi surface instability or an exotic mechanism in CsV3Sb5.
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    Sound-driven single-electron transfer in a circuit of coupled quantum rails
    ([London] : Nature Publishing Group UK, 2019) Takada, Shintaro; Edlbauer, Hermann; Lepage, Hugo V.; Wang, Junliang; Mortemousque, Pierre-André; Georgiou, Giorgos; Barnes, Crispin H. W.; Ford, Christopher J. B.; Yuan, Mingyun; Santos, Paulo V.; Waintal, Xavier; Ludwig, Arne; Wieck, Andreas D.; Urdampilleta, Matias; Meunier, Tristan; Bäuerle, Christopher
    Surface acoustic waves (SAWs) strongly modulate the shallow electric potential in piezoelectric materials. In semiconductor heterostructures such as GaAs/AlGaAs, SAWs can thus be employed to transfer individual electrons between distant quantum dots. This transfer mechanism makes SAW technologies a promising candidate to convey quantum information through a circuit of quantum logic gates. Here we present two essential building blocks of such a SAW-driven quantum circuit. First, we implement a directional coupler allowing to partition a flying electron arbitrarily into two paths of transportation. Second, we demonstrate a triggered single-electron source enabling synchronisation of the SAW-driven sending process. Exceeding a single-shot transfer efficiency of 99%, we show that a SAW-driven integrated circuit is feasible with single electrons on a large scale. Our results pave the way to perform quantum logic operations with flying electron qubits. © 2019, The Author(s).