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- ItemPhase-enabled metal-organic framework homojunction for highly selective CO2 photoreduction(London : Nature Publishing Group, 2021) Liu, Yannan; Chen, Chuanshuang; Valdez, Jesus; Meira, Debora Motta; He, Wanting; Wang, Yong; Harnagea, Catalin; Lu, Qiongquiong; Guner, Tugrul; Wang, Hao; Liu, Cheng-Hao; Zhang, Qingzhe; Huang, Shengyun; Yurtsever, Aycan; Chaker, Mohamed; Ma, DonglingConversion of clean solar energy to chemical fuels is one of the promising and up-and-coming applications of metal–organic frameworks. However, fast recombination of photogenerated charge carriers in these frameworks remains the most significant limitation for their photocatalytic application. Although the construction of homojunctions is a promising solution, it remains very challenging to synthesize them. Herein, we report a well-defined hierarchical homojunction based on metal–organic frameworks via a facile one-pot synthesis route directed by hollow transition metal nanoparticles. The homojunction is enabled by two concentric stacked nanoplates with slightly different crystal phases. The enhanced charge separation in the homojunction was visualized by in-situ surface photovoltage microscopy. Moreover, the as-prepared nanostacks displayed a visible-light-driven carbon dioxide reduction with very high carbon monooxide selectivity, and excellent stability. Our work provides a powerful platform to synthesize capable metal–organic framework complexes and sheds light on the hierarchical structure-function relationships of metal–organic frameworks.
- ItemImproved kinetic behaviour of Mg(NH2)2-2LiH doped with nanostructured K-modified-LixTiyOz for hydrogen storage(London : Nature Publishing Group, 2020) Gizer, G.; Puszkiel, J.; Riglos, M.V.C.; Pistidda, C.; Ramallo-López, J.M.; Mizrahi, M.; Santoru, A.; Gemming, T.; Tseng, J.-C.; Klassen, T.; Dornheim, M.The system Mg(NH2)2 + 2LiH is considered as an interesting solid-state hydrogen storage material owing to its low thermodynamic stability of ca. 40 kJ/mol H2 and high gravimetric hydrogen capacity of 5.6 wt.%. However, high kinetic barriers lead to slow absorption/desorption rates even at relatively high temperatures (>180 °C). In this work, we investigate the effects of the addition of K-modified LixTiyOz on the absorption/desorption behaviour of the Mg(NH2)2 + 2LiH system. In comparison with the pristine Mg(NH2)2 + 2LiH, the system containing a tiny amount of nanostructured K-modified LixTiyOz shows enhanced absorption/desorption behaviour. The doped material presents a sensibly reduced (∼30 °C) desorption onset temperature, notably shorter hydrogen absorption/desorption times and reversible hydrogen capacity of about 3 wt.% H2 upon cycling. Studies on the absorption/desorption processes and micro/nanostructural characterizations of the Mg(NH2)2 + 2LiH + K-modified LixTiyOz system hint to the fact that the presence of in situ formed nanostructure K2TiO3 is the main responsible for the observed improved kinetic behaviour.
- ItemTunneling current modulation in atomically precise graphene nanoribbon heterojunctions(London : Nature Publishing Group, 2021) Senkovskiy, B.; Nenashev, A.; Alavi, S.; Falke, Y.; Hell, M.; Bampoulis, P.; Rybkovskiy, D.; Usachov, D.; Fedorov, A.; Chernov, A.; Gebhard, F.; Meerholz, K.; Hertel, D.; Arita, M.; Okuda, T.; Miyamoto, K.; Shimada, K.; Fischer, F.; Michely, T.; Baranovskii, S.; Lindfors, K.; Szkopek, T.; Grüneis, A.Lateral heterojunctions of atomically precise graphene nanoribbons (GNRs) hold promise for applications in nanotechnology, yet their charge transport and most of the spectroscopic properties have not been investigated. Here, we synthesize a monolayer of multiple aligned heterojunctions consisting of quasi-metallic and wide-bandgap GNRs, and report characterization by scanning tunneling microscopy, angle-resolved photoemission, Raman spectroscopy, and charge transport. Comprehensive transport measurements as a function of bias and gate voltages, channel length, and temperature reveal that charge transport is dictated by tunneling through the potential barriers formed by wide-bandgap GNR segments. The current-voltage characteristics are in agreement with calculations of tunneling conductance through asymmetric barriers. We fabricate a GNR heterojunctions based sensor and demonstrate greatly improved sensitivity to adsorbates compared to graphene based sensors. This is achieved via modulation of the GNR heterojunction tunneling barriers by adsorbates.
- ItemMultiple fermion scattering in the weakly coupled spin-chain compound YbAlO3(London : Nature Publishing Group, 2021) Nikitin, S.; Nishimoto, S.; Fan, Y.; Wu, J.; Wu, L.; Sukhanov, A.; Brando, M.; Pavlovskii, N.; Xu, J.; Vasylechko, L.; Yu, R.; Podlesnyak, A.The Heisenberg antiferromagnetic spin-1/2 chain, originally introduced almost a century ago, is one of the best studied models in quantum mechanics due to its exact solution, but nevertheless it continues to present new discoveries. Its low-energy physics is described by the Tomonaga-Luttinger liquid of spinless fermions, similar to the conduction electrons in one-dimensional metals. In this work we investigate the Heisenberg spin-chain compound YbAlO3 and show that the weak interchain coupling causes Umklapp scattering between the left- and right-moving fermions and stabilizes an incommensurate spin-density wave order at q = 2kF under finite magnetic fields. These Umklapp processes open a route to multiple coherent scattering of fermions, which results in the formation of satellites at integer multiples of the incommensurate fundamental wavevector Q = nq. Our work provides surprising and profound insight into bandstructure control for emergent fermions in quantum materials, and shows how neutron diffraction can be applied to investigate the phenomenon of coherent multiple scattering in metals through the proxy of quantum magnetic systems.
- ItemRoutes to control diffusive pathways and thermal expansion in Ti-alloys(London : Nature Publishing Group, 2020) Bönisch, M.; Stoica, M.; Calin, M.β-stabilized Ti-alloys present several unexplored and intriguing surprises in relation to orthorhombic α″ phases. Among them are (i) the diffusion-controlled formation of transitional α″iso, α″lean and α″rich phases and ii) the highly anisotropic thermal expansion of martensitic α″. Using the prototypical Ti-Nb system, we demonstrate that the thermodynamic energy landscape reveals formation pathways for the diffusional forms of α″ and may lead to a stable β-phase miscibility gap. In this way, we derive temperature-composition criteria for the occurrence of α″iso and resolve reaction sequences during thermal cycling. Moreover, we show that the thermal expansion anisotropy of martensitic α″ gives rise to directions of zero thermal strain depending on Nb content. Utilizing this knowledge, we propose processing routes to achieve null linear expansion in α″ containing Ti-alloys. These concepts are expected to be transferable to other Ti-alloys and offer new avenues for their tailoring and technological exploitation.
- ItemSeparate tuning of nematicity and spin fluctuations to unravel the origin of superconductivity in FeSe(London : Nature Publishing Group, 2020) Baek, S.-H.; Ok, J.M.; Kim, J.S.; Aswartham, S.; Morozov, I.; Chareev, D.; Urata, T.; Tanigaki, K.; Tanabe, Y.; Büchner, B.; Efremov, D.V.The interplay of orbital and spin degrees of freedom is the fundamental characteristic in numerous condensed matter phenomena, including high-temperature superconductivity, quantum spin liquids, and topological semimetals. In iron-based superconductors (FeSCs), this causes superconductivity to emerge in the vicinity of two other instabilities: nematic and magnetic. Unveiling the mutual relationship among nematic order, spin fluctuations, and superconductivity has been a major challenge for research in FeSCs, but it is still controversial. Here, by carrying out 77Se nuclear magnetic resonance (NMR) measurements on FeSe single crystals, doped by cobalt and sulfur that serve as control parameters, we demonstrate that the superconducting transition temperature Tc increases in proportion to the strength of spin fluctuations, while it is independent of the nematic transition temperature Tnem. Our observation therefore directly implies that superconductivity in FeSe is essentially driven by spin fluctuations in the intermediate coupling regime, while nematic fluctuations have a marginal impact on Tc.
- ItemTowards tellurium-free thermoelectric modules for power generation from low-grade heat(London : Nature Publishing Group, 2021) Ying, Pingjun; He, Ran; Mao, Jun; Zhang, Qihao; Reith, Heiko; Sui, Jiehe; Ren, Zhifeng; Nielsch, Kornelius; Schierning, GabiThermoelectric technology converts heat into electricity directly and is a promising source of clean electricity. Commercial thermoelectric modules have relied on Bi2Te3-based compounds because of their unparalleled thermoelectric properties at temperatures associated with low-grade heat (<550 K). However, the scarcity of elemental Te greatly limits the applicability of such modules. Here we report the performance of thermoelectric modules assembled from Bi2Te3-substitute compounds, including p-type MgAgSb and n-type Mg3(Sb,Bi)2, by using a simple, versatile, and thus scalable processing routine. For a temperature difference of ~250 K, whereas a single-stage module displayed a conversion efficiency of ~6.5%, a module using segmented n-type legs displayed a record efficiency of ~7.0% that is comparable to the state-of-the-art Bi2Te3-based thermoelectric modules. Our work demonstrates the feasibility and scalability of high-performance thermoelectric modules based on sustainable elements for recovering low-grade heat.
- ItemCombined structural analysis and cathodoluminescence investigations of single Pr3+-doped Ca2Nb3O10 nanosheets(London : Nature Publishing Group, 2023) Changizi, Rasa; Zaefferer, Stefan; Ziegler, Christian; Romaka, Vitaliy; Lotsch, Bettina V.; Scheu, ChristinaDue to the novel properties of both 2D materials and rare-earth elements, developing 2D rare-earth nanomaterials has a growing interest in research. To produce the most efficient rare-earth nanosheets, it is essential to find out the correlation between chemical composition, atomic structure and luminescent properties of individual sheets. In this study, 2D nanosheets exfoliated from Pr3+-doped KCa2Nb3O10 particles with different Pr concentrations were investigated. Energy dispersive X-ray spectroscopy analysis indicates that the nanosheets contain Ca, Nb and O and a varying Pr content between 0.9 and 1.8 at%. K was completely removed after exfoliation. The crystal structure is monoclinic as in the bulk. The thinnest nanosheets are 3 nm corresponding to one triple perovskite-type layer with Nb on the B sites and Ca on the A sites, surrounded by charge compensating TBA+ molecules. Thicker nanosheets of 12 nm thickness (and above) were observed too by transmission electron microscopy with the same chemical composition. This indicates that several perovskite-type triple layers remain stacked similar to the bulk. Luminescent properties of individual 2D nanosheets were studied using a cathodoluminescence spectrometer revealing additional transitions in the visible region in comparison to the spectra of different bulk phases.
- ItemPerovskite phase heterojunction solar cells(London : Nature Publishing Group, 2022) Ji, Ran; Zhang, Zongbao; Hofstetter, Yvonne J.; Buschbeck, Robin; Hänisch, Christian; Paulus, Fabian; Vaynzof, YanaModern photovoltaic devices are often based on a heterojunction structure where two components with different optoelectronic properties are interfaced. The properties of each side of the junction can be tuned by either utilizing different materials (for example, donor/acceptor) or doping (for example, p–n junction) or even varying their dimensionality (for example, 3D/2D). Here we demonstrate the concept of phase heterojunction (PHJ) solar cells by utilizing two polymorphs of the same material. We demonstrate the approach by forming γ-CsPbI3/β-CsPbI3 perovskite PHJ solar cells. We find that all of the photovoltaic parameters of the PHJ device significantly surpass those of each of the single-phase devices, resulting in a maximum power conversion efficiency of 20.1%. These improvements originate from the efficient passivation of the β-CsPbI3 by the larger bandgap γ-CsPbI3, the increase in the built-in potential of the PHJ devices enabled by the energetic alignment between the two phases and the enhanced absorption of light by the PHJ structure. The approach demonstrated here offers new possibilities for the development of photovoltaic devices based on polymorphic materials.
- ItemCalcite incorporated in silica/collagen xerogels mediates calcium release and enhances osteoblast proliferation and differentiation(London : Nature Publishing Group, 2020) Rößler, S.; Unbehau, R.; Gemming, T.; Kruppke, B.; Wiesmann, H.-P.; Hanke, T.Multiphasic silica/collagen xerogels are biomaterials designed for bone regeneration. Biphasic silica/collagen xerogels (B30) and triphasic xerogels (B30H20 or B30CK20) additionally containing hydroxyapatite or calcite were demonstrated to exhibit several structural levels. On the first level, low fibrillar collagen serves as template for silica nanoparticle agglomerates. On second level, this silica-enriched matrix phase is fiber-reinforced by collagen fibrils. In case of hydroxyapatite incorporation in B30H20, resulting xerogels exhibit a hydroxyapatite-enriched phase consisting of hydroxyapatite particle agglomerates next to silica and low fibrillar collagen. Calcite in B30CK20 is incorporated as single non-agglomerated crystal into the silica/collagen matrix phase with embedded collagen fibrils. Both the structure of multiphasic xerogels and the manner of hydroxyapatite or calcite incorporation have an influence on the release of calcium from the xerogels. B30CK20 released a significantly higher amount of calcium into a calcium-free solution over a three-week period than B30H20. In calcium containing incubation media, all xerogels caused a decrease in calcium concentration as a result of their bioactivity, which was superimposed by the calcium release for B30CK20 and B30H20. Proliferation of human bone marrow stromal cells in direct contact to the materials was enhanced on B30CK20 compared to cells on both plain B30 and B30H20.