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- ItemStable coherent mode-locking based on π pulse formation in single-section lasers([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Arkhipov, Rostislav; Pakhomov, Anton; Arkhipov, Mikhail; Babushkin, Ihar; Rosanov, NikolayHere we consider coherent mode-locking (CML) regimes in single-section cavity lasers, taking place for pulse durations less than atomic population and phase relaxation times, which arise due to coherent Rabi oscillations of the atomic inversion. Typically, CML is introduced for lasers with two sections, the gain and absorber ones. Here we show that, for certain combination of the cavity length and relaxation parameters, a very stable CML in a laser, containing only gain section, may arise. The mode-locking is unconditionally self-starting and appears due to balance of intra-pulse de-excitation and slow interpulse-scale pump-induced relaxation processes. We also discuss the scaling of the system to shorter pulse durations, showing a possibility of mode-locking for few-cycle pulses.
- ItemCharge‐Compensated N‐Doped π ‐Conjugated Polymers: Toward both Thermodynamic Stability of N‐Doped States in Water and High Electron Conductivity(Weinheim : Wiley-VCH, 2022) Borrmann, Fabian; Tsuda, Takuya; Guskova, Olga; Kiriy, Nataliya; Hoffmann, Cedric; Neusser, David; Ludwigs, Sabine; Lappan, Uwe; Simon, Frank; Geisler, Martin; Debnath, Bipasha; Krupskaya, Yulia; Al‐Hussein, Mahmoud; Kiriy, AntonThe understanding and applications of electron-conducting π-conjugated polymers with naphtalene diimide (NDI) blocks show remarkable progress in recent years. Such polymers demonstrate a facilitated n-doping due to the strong electron deficiency of the main polymer chain and the presence of the positively charged side groups stabilizing a negative charge of the n-doped backbone. Here, the n-type conducting NDI polymer with enhanced stability of its n-doped states for prospective “in-water” applications is developed. A combined experimental–theoretical approach is used to identify critical features and parameters that control the doping and electron transport process. The facilitated polymer reduction ability and the thermodynamic stability in water are confirmed by electrochemical measurements and doping studies. This material also demonstrates a high conductivity of 10−2 S cm−1 under ambient conditions and 10−1 S cm−1 in vacuum. The modeling explains the stabilizing effects for various dopants. The simulations show a significant doping-induced “collapse” of the positively charged side chains on the core bearing a partial negative charge. This explains a decrease in the lamellar spacing observed in experiments. This study fundamentally enables a novel pathway for achieving both thermodynamic stability of the n-doped states in water and the high electron conductivity of polymers.
- ItemTopological protection versus degree of entanglement of two-photon light in photonic topological insulators([London] : Nature Publishing Group UK, 2021) Tschernig, Konrad; Jimenez-Galán, Álvaro; Christodoulides, Demetrios N.; Ivanov, Misha; Busch, Kurt; Bandres, Miguel A.; Perez-Leija, ArmandoTopological insulators combine insulating properties in the bulk with scattering-free transport along edges, supporting dissipationless unidirectional energy and information flow even in the presence of defects and disorder. The feasibility of engineering quantum Hamiltonians with photonic tools, combined with the availability of entangled photons, raises the intriguing possibility of employing topologically protected entangled states in optical quantum computing and information processing. However, while two-photon states built as a product of two topologically protected single-photon states inherit full protection from their single-photon “parents”, a high degree of non-separability may lead to rapid deterioration of the two-photon states after propagation through disorder. In this work, we identify physical mechanisms which contribute to the vulnerability of entangled states in topological photonic lattices. Further, we show that in order to maximize entanglement without sacrificing topological protection, the joint spectral correlation map of two-photon states must fit inside a well-defined topological window of protection.
- ItemObservation of direction instability in a fiber ring laser([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Arshad, Muhammad Assad; Hartung, Alexander; Pratiwi, Arni Candra; Jäger, MatthiasWe report on the observation of a new phenomenon occurring in a fiber ring laser. This phenomenon is about the transition from an initially bidirectional emission of a reciprocal fiber ring laser to a unidirectional emission at a certain pump power threshold. In addition, the final direction is not predefined but appears to be randomly chosen every time the threshold is exceeded. Therefore, we term this new phenomenon direction instability. Furthermore, we provide a first discussion of how the instability threshold is influenced by the length and the loss of the cavity. We show that the threshold follows a power times length scaling, indicating a nonlinear origin.
- ItemQuantitative hyperspectral coherent diffractive imaging spectroscopy of a solid-state phase transition in vanadium dioxide(Washington, DC [u.a.] : Assoc., 2021) Johnson, Allan S.; Conesa, Jordi Valls; Vidas, Luciana; Perez-Salinas, Daniel; Günther, Christian M.; Pfau, Bastian; Hallman, Kent A.; Haglund, Richard F.; Eisebitt, Stefan; Wall, SimonSolid-state systems can host a variety of thermodynamic phases that can be controlled with magnetic fields, strain, or laser excitation. Many phases that are believed to exhibit exotic properties only exist on the nanoscale, coexisting with other phases that make them challenging to study, as measurements require both nanometer spatial resolution and spectroscopic information, which are not easily accessible with traditional x-ray spectromicroscopy techniques. Here, we use coherent diffractive imaging spectroscopy (CDIS) to acquire quantitative hyperspectral images of the prototypical quantum material vanadium oxide across the vanadium L2,3 and oxygen K x-ray absorption edges with nanometer-scale resolution. We extract the full complex refractive indices of the monoclinic insulating and rutile conducting phases of VO2 from a single sample and find no evidence for correlation-driven phase transitions. CDIS will enable quantitative full-field x-ray spectromicroscopy for studying phase separation in time-resolved experiments and other extreme sample environments where other methods cannot operate.
- ItemTopological transitions in ac/dc-driven superconductor nanotubes([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Fomin, Vladimir M.; Rezaev, Roman O.; Dobrovolskiy, Oleksandr V.Extending of nanostructures into the third dimension has become a major research avenue in condensed-matter physics, because of geometry- and topology-induced phenomena. In this regard, superconductor 3D nanoarchitectures feature magnetic field inhomogeneity, non-trivial topology of Meissner currents and complex dynamics of topological defects. Here, we investigate theoretically topological transitions in the dynamics of vortices and slips of the phase of the order parameter in open superconductor nanotubes under a modulated transport current. Relying upon the time-dependent Ginzburg–Landau equation, we reveal two distinct voltage regimes when (i) a dominant part of the tube is in either the normal or superconducting state and (ii) a complex interplay between vortices, phase-slip regions and screening currents determines a rich FFT voltage spectrum. Our findings unveil novel dynamical states in superconductor open nanotubes, such as paraxial and azimuthal phase-slip regions, their branching and coexistence with vortices, and allow for control of these states by superimposed dc and ac current stimuli.
- ItemImaging plasma formation in isolated nanoparticles with ultrafast resonant scattering(Melville, NY : AIP Publishing LLC, 2020) Rupp, Daniela; Flückiger, Leonie; Adolph, Marcus; Colombo, Alessandro; Gorkhover, Tais; Harmand, Marion; Krikunova, Maria; Müller, Jan Philippe; Oelze, Tim; Ovcharenko, Yevheniy; Richter, Maria; Sauppe, Mario; Schorb, Sebastian; Treusch, Rolf; Wolter, David; Bostedt, Christoph; Möller, ThomasWe have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.
- ItemHeterostructured Bismuth Telluride Selenide Nanosheets for Enhanced Thermoelectric Performance(Weinheim : Wiley-VCH GmbH, 2020) Bauer, Christoph; Veremchuk, Igor; Kunze, Christof; Benad, Albrecht; Dzhagan, Volodymyr M.; Haubold, Danny; Pohl, Darius; Schierning, Gabi; Nielsch, Kornelius; Lesnyak, Vladimir; Eychmüller, AlexanderThe n-type semiconductor system Bi2Te3Bi2Se3 is known as a low-temperature thermoelectric material with a potentially high efficiency. Herein, a facile approach is reported to synthesize core/shell heterostructured Bi2Te2Se/Bi2Te3 nanosheets (NSs) with lateral dimensions of 1-3 mu m and thickness of about 50nm. Bi2Te3 and Bi2Se3, as well as heterostructured Bi2Te2Se/Bi2Te3 NSs are obtained via colloidal synthesis. Heterostructured NSs show an inhomogeneous distribution of the chalcogen atoms forming selenium and tellurium-rich layers across the NS thickness, resulting in a core/shell structure. Detailed morphological studies reveal that these structures contain nanosized pores. These features contribute to the overall thermoelectric properties of the material, inducing strong phonon scattering at grain boundaries in compacted solids. NSs are processed into nanostructured bulks through spark plasma sintering of dry powders to form a thermoelectric material with high power factor. Electrical characterization of our materials reveals a strong anisotropic behavior in consolidated pellets. It is further demonstrated that by simple thermal annealing, core/shell structure can be controllably transformed into alloyed one. Using this approach pellets with Bi2Te2.55Se0.45 composition are obtained, which exhibit low thermal conductivity and high power factor for in-plane direction with zT of 1.34 at 400K.
- ItemOptoelectronic properties and ultrafast carrier dynamics of copper iodide thin films([London] : Nature Publishing Group UK, 2022) Li, Zhan Hua; He, Jia Xing; Lv, Xiao Hu; Chi, Ling Fei; Egbo, Kingsley O.; Li, Ming-De; Tanaka, Tooru; Guo, Qi Xin; Yu, Kin Man; Liu, Chao PingAs a promising high mobility p-type wide bandgap semiconductor, copper iodide has received increasing attention in recent years. However, the defect physics/evolution are still controversial, and particularly the ultrafast carrier and exciton dynamics in copper iodide has rarely been investigated. Here, we study these fundamental properties for copper iodide thin films by a synergistic approach employing a combination of analytical techniques. Steady-state photoluminescence spectra reveal that the emission at ~420 nm arises from the recombination of electrons with neutral copper vacancies. The photogenerated carrier density dependent ultrafast physical processes are elucidated with using the femtosecond transient absorption spectroscopy. Both the effects of hot-phonon bottleneck and the Auger heating significantly slow down the cooling rate of hot-carriers in the case of high excitation density. The effect of defects on the carrier recombination and the two-photon induced ultrafast carrier dynamics are also investigated. These findings are crucial to the optoelectronic applications of copper iodide.
- ItemThe multi-photon induced Fano effect([London] : Nature Publishing Group UK, 2021) Litvinenko, K.L.; Le, Nguyen H.; Redlich, B.; Pidgeon, C.R.; Abrosimov, N.V.; Andreev, Y.; Huang, Zhiming; Murdin, B.N.The ordinary Fano effect occurs in many-electron atoms and requires an autoionizing state. With such a state, photo-ionization may proceed via pathways that interfere, and the characteristic asymmetric resonance structures appear in the continuum. Here we demonstrate that Fano structure may also be induced without need of auto-ionization, by dressing the continuum with an ordinary bound state in any atom by a coupling laser. Using multi-photon processes gives complete, ultra-fast control over the interference. We show that a line-shape index q near unity (maximum asymmetry) may be produced in hydrogenic silicon donors with a relatively weak beam. Since the Fano lineshape has both constructive and destructive interference, the laser control opens the possibility of state-selective detection with enhancement on one side of resonance and invisibility on the other. We discuss a variety of atomic and molecular spectroscopies, and in the case of silicon donors we provide a calculation for a qubit readout application.
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