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- ItemA Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer(Weinheim : Wiley-VCH, 2021) Liu, Kejun; Li, Jiang; Qi, Haoyuan; Hambsch, Mike; Rawle, Jonathan; Vázquez, Adrián Romaní; Nia, Ali Shaygan; Pashkin, Alexej; Schneider, Harald; Polozij, Mirosllav; Heine, Thomas; Helm, Manfred; Mannsfeld, Stefan C.B.; Kaiser, Ute; Dong, Renhao; Feng, XinliangTwo-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm2), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene. © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
- ItemElectron Population Dynamics in Optically Pumped Asymmetric Coupled Ge/SiGe Quantum Wells: Experiment and Models(Basel : MDPI, 2020) Ciano, Chiara; Virgilio, Michele; Bagolini, Luigi; Baldassarre, Leonetta; Rossetti, Andrea; Pashkin, Alexej; Helm, Manfred; Montanari, Michele; Persichetti, Luca; Di Gaspare, Luciana; Capellini, Giovanni; Paul, Douglas J.; Scalari, Giacomo; Faist, Jèrome; De Seta, Monica; Ortolani, Michelen-type doped Ge quantum wells with SiGe barriers represent a promising heterostructure system for the development of radiation emitters in the terahertz range such as electrically pumped quantum cascade lasers and optically pumped quantum fountain lasers. The nonpolar lattice of Ge and SiGe provides electron-phonon scattering rates that are one order of magnitude lower than polar GaAs. We have developed a self-consistent numerical energy-balance model based on a rate equation approach which includes inelastic and elastic inter-and intra-subband scattering events and takes into account a realistic two-dimensional electron gas distribution in all the subband states of the Ge/SiGe quantum wells by considering subband-dependent electronic temperatures and chemical potentials. This full-subband model is compared here to the standard discrete-energy-level model, in which the material parameters are limited to few input values (scattering rates and radiative cross sections). To provide an experimental case study, we have epitaxially grown samples consisting of two asymmetric coupled quantum wells forming a three-level system, which we optically pump with a free electron laser. The benchmark quantity selected for model testing purposes is the saturation intensity at the 1!3 intersubband transition. The numerical quantum model prediction is in reasonable agreement with the experiments and therefore outperforms the discrete-energy-level analytical model, of which the prediction of the saturation intensity is off by a factor 3. © 2019 by the authors.
- ItemTerahertz absorption-saturation and emission from electron-doped germanium quantum wells(Washington, DC : Soc., 2020) Ciano, Chiara; Virgilio, Michele; Bagolini, Luigi; Baldassarre, Leonetta; Pashkin, Alexej; Helm, Manfred; Montanari, Michele; Persichetti, Luca; Di Gaspare, Luciana; Capellini, Giovanni; Paul, Douglas J.; Scalari, Giacomo; Faist, Jèrome; De Seta, Monica; Ortolani, MicheleWe study radiative relaxation at terahertz frequencies in n-type Ge/SiGe quantum wells, optically pumped with a terahertz free electron laser. Two wells coupled through a tunneling barrier are designed to operate as a three-level laser system with non-equilibrium population generated by optical pumping around the 1→3 intersubband transition at 10 THz. The non-equilibrium subband population dynamics are studied by absorption-saturation measurements and compared to a numerical model. In the emission spectroscopy experiment, we observed a photoluminescence peak at 4 THz, which can be attributed to the 3→2 intersubband transition with possible contribution from the 2→1 intersubband transition. These results represent a step towards silicon-based integrated terahertz emitters.
- ItemFlexomagnetism and vertically graded Néel temperature of antiferromagnetic Cr2O3 thin films([London] : Nature Publishing Group UK, 2022) Makushko, Pavlo; Kosub, Tobias; Pylypovskyi, Oleksandr V.; Hedrich, Natascha; Li, Jiang; Pashkin, Alexej; Avdoshenko, Stanislav; Hübner, René; Ganss, Fabian; Wolf, Daniel; Lubk, Axel; Liedke, Maciej Oskar; Butterling, Maik; Wagner, Andreas; Wagner, Kai; Shields, Brendan J.; Lehmann, Paul; Veremchuk, Igor; Fassbender, Jürgen; Maletinsky, Patrick; Makarov, DenysAntiferromagnetic insulators are a prospective materials platform for magnonics, spin superfluidity, THz spintronics, and non-volatile data storage. A magnetomechanical coupling in antiferromagnets offers vast advantages in the control and manipulation of the primary order parameter yet remains largely unexplored. Here, we discover a new member in the family of flexoeffects in thin films of Cr2O3. We demonstrate that a gradient of mechanical strain can impact the magnetic phase transition resulting in the distribution of the Néel temperature along the thickness of a 50-nm-thick film. The inhomogeneous reduction of the antiferromagnetic order parameter induces a flexomagnetic coefficient of about 15 μB nm−2. The antiferromagnetic ordering in the inhomogeneously strained films can persist up to 100 °C, rendering Cr2O3 relevant for industrial electronics applications. Strain gradient in Cr2O3 thin films enables fundamental research on magnetomechanics and thermodynamics of antiferromagnetic solitons, spin waves and artificial spin ice systems in magnetic materials with continuously graded parameters.
- ItemStretchable Thin Film Mechanical-Strain-Gated Switches and Logic Gate Functions Based on a Soft Tunneling Barrier(Weinheim : Wiley-VCH, 2021) Chae, Soosang; Choi, Won Jin; Fotev, Ivan; Bittrich, Eva; Uhlmann, Petra; Schubert, Mathias; Makarov, Denys; Wagner, Jens; Pashkin, Alexej; Fery, AndreasMechanical-strain-gated switches are cornerstone components of material-embedded circuits that perform logic operations without using conventional electronics. This technology requires a single material system to exhibit three distinct functionalities: strain-invariant conductivity and an increase or decrease of conductivity upon mechanical deformation. Herein, mechanical-strain-gated electric switches based on a thin-film architecture that features an insulator-to-conductor transition when mechanically stretched are demonstrated. The conductivity changes by nine orders of magnitude over a wide range of tunable working strains (as high as 130%). The approach relies on a nanometer-scale sandwiched bilayer Au thin film with an ultrathin poly(dimethylsiloxane) elastomeric barrier layer; applied strain alters the electron tunneling currents through the barrier. Mechanical-force-controlled electric logic circuits are achieved by realizing strain-controlled basic (AND and OR) and universal (NAND and NOR) logic gates in a single system. The proposed material system can be used to fabricate material-embedded logics of arbitrary complexity for a wide range of applications including soft robotics, wearable/implantable electronics, human-machine interfaces, and Internet of Things.