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- ItemStrain Engineered Electrically Pumped SiGeSn Microring Lasers on Si(Washington, DC : ACS, 2022) Marzban, Bahareh; Seidel, Lukas; Liu, Teren; Wu, Kui; Kiyek, Vivien; Zoellner, Marvin Hartwig; Ikonic, Zoran; Schulze, Joerg; Grützmacher, Detlev; Capellini, Giovanni; Oehme, Michael; Witzens, Jeremy; Buca, DanSiGeSn holds great promise for enabling fully group-IV integrated photonics operating at wavelengths extending in the mid-infrared range. Here, we demonstrate an electrically pumped GeSn microring laser based on SiGeSn/GeSn heterostructures. The ring shape allows for enhanced strain relaxation, leading to enhanced optical properties, and better guiding of the carriers into the optically active region. We have engineered a partial undercut of the ring to further promote strain relaxation while maintaining adequate heat sinking. Lasing is measured up to 90 K, with a 75 K T0. Scaling of the threshold current density as the inverse of the outer circumference is linked to optical losses at the etched surface, limiting device performance. Modeling is consistent with experiments across the range of explored inner and outer radii. These results will guide additional device optimization, aiming at improving electrical injection and using stressors to increase the bandgap directness of the active material.
- ItemShort-Range Cooperative Slow-down of Water Solvation Dynamics Around SO42--Mg2+ Ion Pairs(Washington, DC : American Chemical Society, 2022) Kundu, Achintya; Mamatkulov, Shavkat I.; Brünig, Florian N.; Bonthuis, Douwe Jan; Netz, Roland R.; Elsaesser, Thomas; Fingerhut, Benjamin P.The presence of ions affects the structure and dynamics of water on a multitude of length and time scales. In this context, pairs of Mg2+ and SO42- ions in water constitute a prototypical system for which conflicting pictures of hydration geometries and dynamics have been reported. Key issues are the molecular pair and solvation shell geometries, the spatial range of electric interactions, and their impact on solvation dynamics. Here, we introduce asymmetric SO42- stretching vibrations as new and most specific local probes of solvation dynamics that allow to access ion hydration dynamics at the dilute concentration (0.2 M) of a native electrolyte environment. Highly sensitive heterodyne 2D-IR spectroscopy in the fingerprint region of the SO42- ions around 1100 cm-1 reveals a specific slow-down of solvation dynamics for hydrated MgSO4 and for Na2SO4 in the presence of Mg2+ ions, which manifests as a retardation of spectral diffusion compared to aqueous Na2SO4 solutions in the absence of Mg2+ ions. Extensive molecular dynamics and density functional theory QM/MM simulations provide a microscopic view of the observed ultrafast dephasing and hydration dynamics. They suggest a molecular picture where the slow-down of hydration dynamics arises from the structural peculiarities of solvent-shared SO42--Mg2+ ion pairs.
- 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.
- ItemAuger- and X-ray Photoelectron Spectroscopy at Metallic Li Material: Chemical Shifts Related to Sample Preparation, Gas Atmosphere, and Ion and Electron Beam Effects(Basel : MDPI, 2022) Oswald, SteffenLi-based batteries are a key element in reaching a sustainable energy economy in the near future. The understanding of the very complex electrochemical processes is necessary for the optimization of their performance. X-ray photoelectron spectroscopy (XPS) is an accepted method used to improve understanding around the chemical processes at the electrode surfaces. Nevertheless, its application is limited because the surfaces under investigation are mostly rough and inhomogeneous. Local elemental analysis, such as Auger electron spectroscopy (AES), could assist XPS to gain more insight into the chemical processes at the surfaces. In this paper, some challenges in using electron spectroscopy are discussed, such as binding energy (BE) referencing for the quantitative study of chemical shifts, gas atmospheric influences, or beam damage (including both AE and XP spectroscopy). Carefully prepared and surface-modified metallic lithium material is used as model surface, considering that Li is the key element for most battery applications.
- ItemRevealing the co-action of viscous and multistability hysteresis in an adhesive, nominally flat punch: A combined numerical and experimental study([Erscheinungsort nicht ermittelbar] : arXiv, 2022) Christian Müller, Manar Samri, René Hensel, Eduard Arzt, Martin H. MüserViscoelasticity is well known to cause a significant hysteresis of crack closure and opening when an elastomer is brought in and out of contact with a flat, rigid counterface. In contrast, the idea that adhesive hysteresis can also result under quasi-static driving due to small-scale, elastic multistability is relatively new. Here, we study a system in which both mechanisms act concurrently. Specifically, we compare the simulated and experimentally measured time evolution of the interfacial force and the real contact area between a soft elastomer and a rigid, flat punch, to which small-scale, single-sinusoidal roughness is added. To this end, we further the Green's function molecular dynamics method and extend recently developed imaging techniques to elucidate the rate- and preload-dependence of the pull-off process. Our results reveal that hysteresis is much enhanced when the saddle points of the topography come into contact, which, however, is impeded by viscoelastic forces and may require sufficiently large preloads. A similar coaction of viscous- and multistability effects is expected to occur in macroscopic polymer contacts and be relevant, e.g., for pressure-sensitive adhesives and modern adhesive gripping devices.
- ItemSilane-Mediated Expansion of Domains in Si-Doped κ-Ga2O3 Epitaxy and its Impact on the In-Plane Electronic Conduction(Weinheim : Wiley-VCH, 2022) Mazzolini, Piero; Fogarassy, Zsolt; Parisini, Antonella; Mezzadri, Francesco; Diercks, David; Bosi, Matteo; Seravalli, Luca; Sacchi, Anna; Spaggiari, Giulia; Bersani, Danilo; Bierwagen, Oliver; Janzen, Benjamin Moritz; Marggraf, Marcella Naomi; Wagner, Markus R.; Cora, Ildiko; Pécz, Béla; Tahraoui, Abbes; Bosio, Alessio; Borelli, Carmine; Leone, Stefano; Fornari, RobertoUnintentionally doped (001)-oriented orthorhombic κ-Ga2O3 epitaxial films on c-plane sapphire substrates are characterized by the presence of ≈ 10 nm wide columnar rotational domains that can severely inhibit in-plane electronic conduction. Comparing the in- and out-of-plane resistance on well-defined sample geometries, it is experimentally proved that the in-plane resistivity is at least ten times higher than the out-of-plane one. The introduction of silane during metal-organic vapor phase epitaxial growth not only allows for n-type Si extrinsic doping, but also results in the increase of more than one order of magnitude in the domain size (up to ≈ 300 nm) and mobility (highest µ ≈ 10 cm2V−1s−1, with corresponding lowest ρ ≈ 0.2 Ωcm). To qualitatively compare the mean domain dimension in κ-Ga2O3 epitaxial films, non-destructive experimental procedures are provided based on X-ray diffraction and Raman spectroscopy. The results of this study pave the way to significantly improved in-plane conduction in κ-Ga2O3 and its possible breakthrough in new generation electronics. The set of cross-linked experimental techniques and corresponding interpretation here proposed can apply to a wide range of material systems that suffer/benefit from domain-related functional properties.
- ItemTemperature dependence of the complex permittivity in microwave range of some industrial polymers(New York, NY : American Inst. of Physics, 2022) Porteanu, Horia-Eugen; Kaempf, Rudolf; Flisgen, Thomas; Heinrich, WolfgangThe microwave properties of a number of polymers common in industry are investigated. A cylindrical resonator in the TM012 mode is used. The cavity perturbation method and detailed COMSOL simulations are applied for extracting the complex permittivity as a function of temperature. The results are useful for the design of plastic processing tools by heating with electromagnetic fields. The intrinsic parameters of absorption are derived based on two exponential decays: polarization and Arrhenius dependence of the decay times on temperature.
- ItemLong-term stability of GaAs/AlAs terahertz quantum-cascade lasers(New York, NY : American Inst. of Physics, 2022) Schrottke, L.; Lü, X.; Biermann, K.; Gellie, P.; Grahn, H.T.We have investigated high-performance GaAs/AlAs terahertz (THz) quantum-cascade lasers (QCLs) with respect to the long-term stability of their operating parameters. The output power of lasers that contain an additional, thick AlAs refractive-index contrast layer underneath the cascade structure decreases after three months by about 35%. The deterioration of these lasers is attributed to the oxidation processes in this contrast layer starting from the facets. However, GaAs/AlAs THz QCLs with an Al0.9Ga0.1As refractive-index contrast layer exhibit long-term stability of the operating parameters over many years even when they are exposed to atmospheric conditions. Therefore, these lasers are promising high-power radiation sources in the terahertz spectral region for commercial applications.
- ItemHorizontal Wavenumber Spectra of Vertical Vorticity and Horizontal Divergence of Mesoscale Dynamics in the Mesosphere and Lower Thermosphere Using Multistatic Specular Meteor Radar Observations(Malden, Mass. : American Geophysical Union, 2022) Poblet, Facundo L.; Chau, Jorge L.; Conte, J. Federico; Avsarkisov, Victor; Vierinen, Juha; Charuvil Asokan, HarikrishnanSpecular meteor radars (SMRs) have significantly contributed to the understanding of wind dynamics in the mesosphere and lower thermosphere (MLT). We present a method to estimate horizontal correlations of vertical vorticity (Qzz) and horizontal divergence (P) in the MLT, using line-of-sight multistatic SMRs velocities, that consists of three steps. First, we estimate 2D, zonal, and meridional correlation functions of wind fluctuations (with periods less than 4 hr and vertical wavelengths smaller than 4 km) using the wind field correlation function inversion (WCFI) technique. Then, the WCFI's statistical estimates are converted into longitudinal and transverse components. The conversion relation is obtained by considering the rotation about the vertical direction of two velocity vectors, from an east-north-up system to a meteor-pair-dependent cylindrical system. Finally, following a procedure previously applied in the upper troposphere and lower stratosphere to airborne wind measurements, the longitudinal and transverse spatial correlations are fitted, from which Qzz, P, and their spectra are directly estimated. The method is applied to a special Spread spectrum Interferometric Multistatic meteor radar Observing Network data set, obtained over northern Germany for seven days in November 2018. The results show that in a quasi-axisymmetric scenario, P was more than five times larger than Qzz for the horizontal wavelengths range given by ∼50–400 km, indicating a predominance of internal gravity waves over vortical modes of motion as a possible explanation for the MLT mesoscale dynamics during this campaign.
- ItemDeveloping a Laser Induced Liquid Beam Ion Desorption Spectral Database as Reference for Spaceborne Mass Spectrometers(Malden, Mass. : American Geophysical Union, 2022) Klenner, Fabian; Umair, Muhammad; Walter, Sebastian H. G.; Khawaja, Nozair; Hillier, Jon; Nölle, Lenz; Zou, Zenghui; Napoleoni, Maryse; Sanderink, Arnaud; Zuschneid, Wilhelm; Abel, Bernd; Postberg, FrankSpaceborne impact ionization mass spectrometers, such as the Cosmic Dust Analyzer on board the past Cassini spacecraft or the SUrface Dust Analyzer being built for NASA's upcoming Europa Clipper mission, are of crucial importance for the exploration of icy moons in the Solar System, such as Saturn's moon Enceladus or Jupiter's moon Europa. For the interpretation of data produced by these instruments, analogue experiments on Earth are essential. To date, thousands of laboratory mass spectra have been recorded with an analogue experiment for impact ionization mass spectrometers. Simulation of mass spectra of ice grains in space is achieved by a Laser Induced Liquid Beam Ion Desorption (LILBID) approach. The desorbed cations or anions are analyzed in a time-of-flight mass spectrometer. The amount of unstructured raw data is increasingly challenging to sort, process, interpret and compare with data from space. Thus far this has been achieved manually for individual mass spectra because no database containing the recorded reference spectra was available. Here we describe the development of a comprehensive, extendable database containing cation and anion mass spectra from the laboratory LILBID facility. The database is based on a Relational Database Management System with a web server interface and enables filtering of the laboratory data using a wide range of parameters. The mass spectra can be compared not only with data from past and future space missions but also mass spectral data generated by other, terrestrial, techniques. The validated and approved subset of the database is available for general public (https://lilbid-db.planet.fu-berlin.de).