“Control of switching between metastable superconducting states in delta-MoN nanowires”. Buh J, Kabanov V, Baranov V, Mrzel A, Kovic A, Mihailovic D, Nature communications 6, 10250 (2015). http://doi.org/10.1038/ncomms10250
Abstract: The superconducting state in one-dimensional nanosystems is very delicate. While fluctuations of the phase of the superconducting wave function lead to the spontaneous decay of persistent supercurrents in thin superconducting wires and nanocircuits, discrete phase-slip fluctuations can also lead to more exotic phenomena, such as the appearance of metastable superconducting states in current-bearing wires. Here we show that switching between different metastable superconducting states in d-MoN nanowires can be very effectively manipulated by introducing small amplitude electrical noise. Furthermore, we show that deterministic switching between metastable superconducting states with different numbers of phase-slip centres can be achieved in both directions with small electrical current pulse perturbations of appropriate polarity. The observed current-controlled bi-stability is in remarkable agreement with theoretically predicted trajectories of the system switching between different limit cycle solutions of a model one-dimensional superconductor.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
Times cited: 8
DOI: 10.1038/ncomms10250
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“Insertion compounds and composites made by ball milling for advanced sodium-ion batteries”. Zhang B, Dugas R, Rousse G, Rozier P, Abakumov AM, Tarascon J-M, Nature communications 7, 10308 (2016). http://doi.org/10.1038/ncomms10308
Abstract: Sodium-ion batteries have been considered as potential candidates for stationary energy storage because of the low cost and wide availability of Na sources. However, their future commercialization depends critically on control over the solid electrolyte interface formation, as well as the degree of sodiation at the positive electrode. Here we report an easily scalable ball milling approach, which relies on the use of metallic sodium, to prepare a variety of sodium-based alloys, insertion layered oxides and polyanionic compounds having sodium in excess such as the Na4V2(PO4)(2)F-3 phase. The practical benefits of preparing sodium-enriched positive electrodes as reservoirs to compensate for sodium loss during solid electrolyte interphase formation are demonstrated by assembling full C/P'2-Na-1[Fe0.5Mn0.5]O-2 and C/'Na3+xV2(PO4)(2)F-3' sodium-ion cells that show substantial increases (>10%) in energy storage density. Our findings may offer electrode design principles for accelerating the development of the sodium-ion technology.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 104
DOI: 10.1038/ncomms10308
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“Unusual lattice vibration characteristics in whiskers of the pseudo-one-dimensional titanium trisulfide TiS3”. Wu K, Torun E, Sahin H, Chen B, Fan X, Pant A, Wright DP, Aoki T, Peeters FM, Soignard E, Tongay S, Nature communications 7, 12952 (2016). http://doi.org/10.1038/NCOMMS12952
Abstract: Transition metal trichalcogenides form a class of layered materials with strong in-plane anisotropy. For example, titanium trisulfide (TiS3) whiskers are made out of weakly interacting TiS3 layers, where each layer is made of weakly interacting quasi-one-dimensional chains extending along the b axis. Here we establish the unusual vibrational properties of TiS3 both experimentally and theoretically. Unlike other two-dimensional systems, the Raman active peaks of TiS3 have only out-of-plane vibrational modes, and interestingly some of these vibrations involve unique rigid-chain vibrations and S-S molecular oscillations. High-pressure Raman studies further reveal that the A(g)(S-S) S-S molecular mode has an unconventional negative pressure dependence, whereas other peaks stiffen as anticipated. Various vibrational modes are doubly degenerate at ambient pressure, but the degeneracy is lifted at high pressures. These results establish the unusual vibrational properties of TiS3 with strong in-plane anisotropy, and may have relevance to understanding of vibrational properties in other anisotropic two-dimensional material systems.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
Times cited: 50
DOI: 10.1038/NCOMMS12952
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“Imaging of super-fast dynamics and flow instabilities of superconducting vortices”. Embon L, Anahory Y, Jelić, ZL, Lachman EO, Myasoedov Y, Huber ME, Mikitik GP, Silhanek AV, Milošević, MV, Gurevich A, Zeldov E, Nature communications 8, 85 (2017). http://doi.org/10.1038/S41467-017-00089-3
Abstract: Quantized magnetic vortices driven by electric current determine key electromagnetic properties of superconductors. While the dynamic behavior of slow vortices has been thoroughly investigated, the physics of ultrafast vortices under strong currents remains largely unexplored. Here, we use a nanoscale scanning superconducting quantum interference device to image vortices penetrating into a superconducting Pb film at rates of tens of GHz and moving with velocities of up to tens of km/s, which are not only much larger than the speed of sound but also exceed the pair-breaking speed limit of superconducting condensate. These experiments reveal formation of mesoscopic vortex channels which undergo cascades of bifurcations as the current and magnetic field increase. Our numerical simulations predict metamorphosis of fast Abrikosov vortices into mixed Abrikosov-Josephson vortices at even higher velocities. This work offers an insight into the fundamental physics of dynamic vortex states of superconductors at high current densities, crucial for many applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
Times cited: 124
DOI: 10.1038/S41467-017-00089-3
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“Asymmetry and non-dispersivity in the Aharonov-Bohm effect”. Becker M, Guzzinati G, Béché, A, Verbeeck J, Batelaan H, Nature communications 10, 1700 (2019). http://doi.org/10.1038/S41467-019-09609-9
Abstract: Decades ago, Aharonov and Bohm showed that electrons are affected by electromagnetic potentials in the absence of forces due to fields. Zeilinger's theorem describes this absence of classical force in quantum terms as the “dispersionless” nature of the Aharonov-Bohm effect. Shelankov predicted the presence of a quantum “force” for the same Aharonov-Bohm physical system as elucidated by Berry. Here, we report an experiment designed to test Shelankov's prediction and we provide a theoretical analysis that is intended to elucidate the relation between Shelankov's prediction and Zeilinger's theorem. The experiment consists of the Aharonov-Bohm physical system; free electrons pass a magnetized nanorod and far-field electron diffraction is observed. The diffraction pattern is asymmetric confirming one of Shelankov's predictions and giving indirect experimental evidence for the presence of a quantum “force”. Our theoretical analysis shows that Zeilinger's theorem and Shelankov's result are both special cases of one theorem.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 12
DOI: 10.1038/S41467-019-09609-9
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“A highly conductive fibre network enables centimetre-scale electron transport in multicellular cable bacteria”. Meysman FJR, Cornelissen R, Trashin S, Bonne R, Hidalgo-Martinez S, van der Veen J, Blom CJ, Karman C, Hou J-L, Eachambadi RT, Geelhoed JS, De Wael K, Beaumont HJE, Cleuren B, Valcke R, van der Zant HSJ, Boschker HTS, Manca JV, Nature communications 10, 4120 (2019). http://doi.org/10.1038/S41467-019-12115-7
Abstract: Biological electron transport is classically thought to occur over nanometre distances, yet recent studies suggest that electrical currents can run along centimetre-long cable bacteria. The phenomenon remains elusive, however, as currents have not been directly measured, nor have the conductive structures been identified. Here we demonstrate that cable bacteria conduct electrons over centimetre distances via highly conductive fibres embedded in the cell envelope. Direct electrode measurements reveal nanoampere currents in intact filaments up to 10.1 mm long (>2000 adjacent cells). A network of parallel periplasmic fibres displays a high conductivity (up to 79 S cm(-1)), explaining currents measured through intact filaments. Conductance rapidly declines upon exposure to air, but remains stable under vacuum, demonstrating that charge transfer is electronic rather than ionic. Our finding of a biological structure that efficiently guides electrical currents over long distances greatly expands the paradigm of biological charge transport and could enable new bio-electronic applications.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 12.124
Times cited: 10
DOI: 10.1038/S41467-019-12115-7
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“A redox signalling globin is essential for reproduction in Caenorhabditis elegans”. De Henau S, Tilleman L, Vangheel M, Luyckx E, Trashin S, Pauwels M, Germani F, Vlaeminck C, Vanfleteren JR, Bert W, Pesce A, Nardini M, Bolognesi M, De Wael K, Moens L, Dewilde S, Braeckman BP, Nature communications 6, 8782 (2015). http://doi.org/10.1038/NCOMMS9782
Abstract: Moderate levels of reactive oxygen species (ROS) are now recognized as redox signalling molecules. However, thus far, only mitochondria and NADPH oxidases have been identified as cellular sources of ROS in signalling. Here we identify a globin (GLB-12) that produces superoxide, a type of ROS, which serves as an essential signal for reproduction in C. elegans. We find that GLB-12 has an important role in the regulation of multiple aspects in germline development, including germ cell apoptosis. We further describe how GLB-12 displays specific molecular, biochemical and structural properties that allow this globin to act as a superoxide generator. In addition, both an intra- and extracellular superoxide dismutase act as key partners of GLB-12 to create a transmembrane redox signal. Our results show that a globin can function as a driving factor in redox signalling, and how this signal is regulated at the subcellular level by multiple control layers.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 12.124
Times cited: 20
DOI: 10.1038/NCOMMS9782
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“Singlet oxygen-based electrosensing by molecular photosensitizers”. Trashin S, Rahemi V, Ramji K, Neven L, Gorun SM, De Wael K, Nature communications 8, 16108 (2017). http://doi.org/10.1038/NCOMMS16108
Abstract: Enzyme-based electrochemical biosensors are an inspiration for the development of (bio)analytical techniques. However, the instability and reproducibility of the reactivity of enzymes, combined with the need for chemical reagents for sensing remain challenges for the construction of useful devices. Here we present a sensing strategy inspired by the advantages of enzymes and photoelectrochemical sensing, namely the integration of aerobic photocatalysis and electrochemical analysis. The photosensitizer, a bioinspired perfluorinated Zn phthalocyanine, generates singlet-oxygen from air under visible light illumination and oxidizes analytes, yielding electrochemically-detectable products while resisting the oxidizing species it produces. Compared with enzymatic detection methods, the proposed strategy uses air instead of internally added reactive reagents, features intrinsic baseline correction via on/off light switching and shows C-F bonds-type enhanced stability. It also affords selectivity imparted by the catalytic process and nano-level detection, such as 20 nM amoxicillin in μl sample volumes.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 12.124
Times cited: 26
DOI: 10.1038/NCOMMS16108
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“Manipulating topological transformations of polar structures through real-time observation of the dynamic polarization evolution”. Du K, Zhang M, Dai C, Zhou ZN, Xie YW, Ren ZH, Tian H, Chen LQ, Van Tendeloo G, Zhang Z, Nature communications 10, 4864 (2019). http://doi.org/10.1038/S41467-019-12864-5
Abstract: Topological structures based on controllable ferroelectric or ferromagnetic domain configurations offer the opportunity to develop microelectronic devices such as high-density memories. Despite the increasing experimental and theoretical insights into various domain structures (such as polar spirals, polar wave, polar vortex) over the past decade, manipulating the topological transformations of polar structures and comprehensively understanding its underlying mechanism remains lacking. By conducting an in-situ non-contact bias technique, here we systematically investigate the real-time topological transformations of polar structures in PbTiO3/SrTiO3 multilayers at an atomic level. The procedure of vortex pair splitting and the transformation from polar vortex to polar wave and out-of-plane polarization are observed step by step. Furthermore, the redistribution of charge in various topological structures has been demonstrated under an external bias. This provides new insights for the symbiosis of polar and charge and offers an opportunity for a new generation of microelectronic devices.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
DOI: 10.1038/S41467-019-12864-5
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“High temperature rise dominated cracking mechanisms in ultra-ductile and tough titanium alloy”. Choisez L, Ding L, Marteleur M, Idrissi H, Pardoen T, Jacques PJ, Nature Communications 11, 2110 (2020). http://doi.org/10.1038/S41467-020-15772-1
Abstract: Extensive use of titanium alloys is partly hindered by a lack of ductility, strain hardening, and fracture toughness. Recently, several beta -metastable titanium alloys were designed to simultaneously activate both transformation-induced plasticity and twinning-induced plasticity effects, resulting in significant improvements to their strain hardening capacity and resistance to plastic localization. Here, we report an ultra-large fracture resistance in a Ti-12Mo alloy (wt.%), that results from a high resistance to damage nucleation, with an unexpected fracture phenomenology under quasi-static loading. Necking develops at a large uniform true strain of 0.3 while fracture initiates at a true fracture strain of 1.0 by intense through-thickness shear within a thin localized shear band. Transmission electron microscopy reveals that dynamic recrystallization occurs in this band, while local partial melting is observed on the fracture surface. Shear band temperatures of 1250-2450 degrees C are estimated by the fusible coating method. The reported high ductility combined to the unconventional fracture process opens alternative avenues toward Ti alloys toughening. Specific titanium alloys combine transformation-induced plasticity and twinning-induced plasticity for improved work hardening. Here, the authors show that these alloys also have an ultra-large fracture resistance and an unexpected fracture mechanism via dynamic recrystallization and local melting in a deformation band.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 1
DOI: 10.1038/S41467-020-15772-1
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“Transforming solid-state precipitates via excess vacancies”. Bourgeois L, Zhang Y, Zhang Z, Chen Y, Medhekar N V, Nature Communications 11, 1248 (2020). http://doi.org/10.1038/S41467-020-15087-1
Abstract: Many phase transformations associated with solid-state precipitation look structurally simple, yet, inexplicably, take place with great difficulty. A classic case of difficult phase transformations is the nucleation of strengthening precipitates in high-strength lightweight aluminium alloys. Here, using a combination of atomic-scale imaging, simulations and classical nucleation theory calculations, we investigate the nucleation of the strengthening phase theta' onto a template structure in the aluminium-copper alloy system. We show that this transformation can be promoted in samples exhibiting at least one nanoscale dimension, with extremely high nucleation rates for the strengthening phase as well as for an unexpected phase. This template-directed solid-state nucleation pathway is enabled by the large influx of surface vacancies that results from heating a nanoscale solid. Template-directed nucleation is replicated in a bulk alloy as well as under electron irradiation, implying that this difficult transformation can be facilitated under the general condition of sustained excess vacancy concentrations.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 5
DOI: 10.1038/S41467-020-15087-1
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“Deciphering the interactions between single arm dislocation sources and coherent twin boundary in nickel bi-crystal”. Samaee V, Dupraz M, Pardoen T, VAn Swygenhoven H, Schryvers D, Idrissi H, Nature Communications 12, 962 (2021). http://doi.org/10.1038/S41467-021-21296-Z
Abstract: The introduction of a well-controlled population of coherent twin boundaries (CTBs) is an attractive route to improve the strength ductility product in face centered cubic (FCC) metals. However, the elementary mechanisms controlling the interaction between single arm dislocation sources (SASs), often present in nanotwinned FCC metals, and CTB are still not well understood. Here, quantitative in-situ transmission electron microscopy (TEM) observations of these mechanisms under tensile loading are performed on submicron Ni bi-crystal. We report that the absorption of curved screw dislocations at the CTB leads to the formation of constriction nodes connecting pairs of twinning dislocations at the CTB plane in agreement with large scale 3D atomistic simulations. The coordinated motion of the twinning dislocation pairs due to the presence of the nodes leads to a unique CTB sliding mechanism, which plays an important role in initiating the fracture process at a CTB ledge. TEM observations of the interactions between non-screw dislocations and the CTB highlight the importance of the synergy between the repulsive force of the CTB and the back stress from SASs when the interactions occur in small volumes. Interactions of dislocations with coherent twin boundaries contribute to strength and ductility in metals, but investigating the interaction mechanisms is challenging. Here the authors unravel these mechanisms through quantitative in-situ transmission electron microscopy observations in nickel bi-crystal samples under tensile loading.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
DOI: 10.1038/S41467-021-21296-Z
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“Early deformation mechanisms in the shear affected region underneath a copper sliding contact”. Haug C, Ruebeling F, Kashiwar A, Gumbsch P, Kübel C, Greiner C, Nature Communications 11, 839 (2020). http://doi.org/10.1038/S41467-020-14640-2
Abstract: Dislocation mediated plastic deformation decisively influences the friction coefficient and the microstructural changes at many metal sliding interfaces during tribological loading. This work explores the initiation of a tribologically induced microstructure in the vicinity of a copper twin boundary. Two distinct horizontal dislocation traces lines (DTL) are observed in their interaction with the twin boundary beneath the sliding interface. DTL formation seems unaffected by the presence of the twin boundary but the twin boundary acts as an indicator of the occurring deformation mechanisms. Three concurrent elementary processes can be identified: simple shear of the subsurface area in sliding direction, localized shear at the primary DTL and crystal rotation in the layers above and between the DTLs around axes parallel to the transverse direction. Crystal orientation analysis demonstrates a strong compatibility of these proposed processes. Quantitatively separating these different deformation mechanisms is crucial for future predictive modeling of tribological contacts.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
DOI: 10.1038/S41467-020-14640-2
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“Acoustic cavities in 2D heterostructures”. Zalalutdinov MK, Robinson JT, Fonseca JJ, LaGasse SW, Pandey T, Lindsay LR, Reinecke TL, Photiadis DM, Culbertson JC, Cress CD, Houston BH, Nature Communications 12, 3267 (2021). http://doi.org/10.1038/S41467-021-23359-7
Abstract: Two-dimensional (2D) materials offer unique opportunities in engineering the ultrafast spatiotemporal response of composite nanomechanical structures. In this work, we report on high frequency, high quality factor (Q) 2D acoustic cavities operating in the 50-600GHz frequency (f) range with f x Q up to 1 x 10(14). Monolayer steps and material interfaces expand cavity functionality, as demonstrated by building adjacent cavities that are isolated or strongly-coupled, as well as a frequency comb generator in MoS2/h-BN systems. Energy dissipation measurements in 2D cavities are compared with attenuation derived from phonon-phonon scattering rates calculated using a fully microscopic ab initio approach. Phonon lifetime calculations extended to low frequencies (<1THz) and combined with sound propagation analysis in ultrathin plates provide a framework for designing acoustic cavities that approach their fundamental performance limit. These results provide a pathway for developing platforms employing phonon-based signal processing and for exploring the quantum nature of phonons. Here, authors report on acoustic cavities in 2D materials operating in the 50-600GHz range and show that quality factors approach the limit set by lattice anharmonicity. Functionality expanded by heterogeneities (steps and interfaces) is demonstrated through coupled cavities and frequency comb generation.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
DOI: 10.1038/S41467-021-23359-7
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“Exponentially selective molecular sieving through angstrom pores”. Sun PZ, Yagmurcukardes M, Zhang R, Kuang WJ, Lozada-Hidalgo M, Liu BL, Cheng H-M, Wang FC, Peeters FM, Grigorieva IV, Geim AK, Nature Communications 12, 7170 (2021). http://doi.org/10.1038/S41467-021-27347-9
Abstract: Two-dimensional crystals with angstrom-scale pores are widely considered as candidates for a next generation of molecular separation technologies aiming to provide extreme, exponentially large selectivity combined with high flow rates. No such pores have been demonstrated experimentally. Here we study gas transport through individual graphene pores created by low intensity exposure to low kV electrons. Helium and hydrogen permeate easily through these pores whereas larger species such as xenon and methane are practically blocked. Permeating gases experience activation barriers that increase quadratically with molecules' kinetic diameter, and the effective diameter of the created pores is estimated as similar to 2 angstroms, about one missing carbon ring. Our work reveals stringent conditions for achieving the long sought-after exponential selectivity using porous two-dimensional membranes and suggests limits on their possible performance. Two-dimensional membranes with angstrom-sized pores are predicted to combine high permeability with exceptional selectivity, but experimental demonstration has been challenging. Here the authors realize angstrom-sized pores in monolayer graphene and demonstrate gas transport with activation barriers increasing quadratically with the molecular kinetic diameter.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
Times cited: 28
DOI: 10.1038/S41467-021-27347-9
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“Superconducting diode effect via conformal-mapped nanoholes”. Lyu Y-Y, Jiang J, Wang Y-L, Xiao Z-L, Dong S, Chen Q-H, Milošević, MV, Wang H, Divan R, Pearson JE, Wu P, Peeters FM, Kwok W-K, Nature Communications 12, 2703 (2021). http://doi.org/10.1038/S41467-021-23077-0
Abstract: A superconducting diode is an electronic device that conducts supercurrent and exhibits zero resistance primarily for one direction of applied current. Such a dissipationless diode is a desirable unit for constructing electronic circuits with ultralow power consumption. However, realizing a superconducting diode is fundamentally and technologically challenging, as it usually requires a material structure without a centre of inversion, which is scarce among superconducting materials. Here, we demonstrate a superconducting diode achieved in a conventional superconducting film patterned with a conformal array of nanoscale holes, which breaks the spatial inversion symmetry. We showcase the superconducting diode effect through switchable and reversible rectification signals, which can be three orders of magnitude larger than that from a flux-quantum diode. The introduction of conformal potential landscapes for creating a superconducting diode is thereby proven as a convenient, tunable, yet vastly advantageous tool for superconducting electronics. This could be readily applicable to any superconducting materials, including cuprates and iron-based superconductors that have higher transition temperatures and are desirable in device applications. A superconducting diode is dissipationless and desirable for electronic circuits with ultralow power consumption, yet it remains challenging to realize it. Here, the authors achieve a superconducting diode in a conventional superconducting film patterned with a conformal array of nanoscale holes.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
Times cited: 71
DOI: 10.1038/S41467-021-23077-0
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“Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals”. Toso S, Imran M, Mugnaioli E, Moliterni A, Caliandro R, Schrenker NJ, Pianetti A, Zito J, Zaccaria F, Wu Y, Gemmi M, Giannini C, Brovelli S, Infante I, Bals S, Manna L, Nature communications 13, 3976 (2022). http://doi.org/10.1038/S41467-022-31699-1
Abstract: Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 15
DOI: 10.1038/S41467-022-31699-1
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“Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement”. Wang D, Hermes M, Najmr S, Tasios N, Grau-Carbonell A, Liu Y, Bals S, Dijkstra M, Murray CB, van Blaaderen A, Nature communications 13, 6001 (2022). http://doi.org/10.1038/S41467-022-33616-Y
Abstract: Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 7
DOI: 10.1038/S41467-022-33616-Y
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“Wien effect in interfacial water dissociation through proton-permeable graphene electrodes”. Cai J, Griffin E, Guarochico-Moreira VH, Barry D, Xin B, Yagmurcukardes M, Zhang S, Geim AK, Peeters FM, Lozada-Hidalgo M, Nature communications 13, 5776 (2022). http://doi.org/10.1038/S41467-022-33451-1
Abstract: Strong electric fields can accelerate molecular dissociation reactions. The phenomenon known as the Wien effect was previously observed using high-voltage electrolysis cells that produced fields of about 10(7) V m(-1), sufficient to accelerate the dissociation of weakly bound molecules (e.g., organics and weak electrolytes). The observation of the Wien effect for the common case of water dissociation (H2O reversible arrow H+ + OH-) has remained elusive. Here we study the dissociation of interfacial water adjacent to proton-permeable graphene electrodes and observe strong acceleration of the reaction in fields reaching above 10(8) V m(-1). The use of graphene electrodes allows measuring the proton currents arising exclusively from the dissociation of interfacial water, while the electric field driving the reaction is monitored through the carrier density induced in graphene by the same field. The observed exponential increase in proton currents is in quantitative agreement with Onsager's theory. Our results also demonstrate that graphene electrodes can be valuable for the investigation of various interfacial phenomena involving proton transport.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 16.6
Times cited: 14
DOI: 10.1038/S41467-022-33451-1
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“Gas permeation through graphdiyne-based nanoporous membranes”. Zhou Z, Tan Y, Yang Q, Bera A, Xiong Z, Yagmurcukardes M, Kim M, Zou Y, Wang G, Mishchenko A, Timokhin I, Wang C, Wang H, Yang C, Lu Y, Boya R, Liao H, Haigh S, Liu H, Peeters FM, Li Y, Geim AK, Hu S, Nature communications 13, 4031 (2022). http://doi.org/10.1038/S41467-022-31779-2
Abstract: Nanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeance. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of similar to 0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 16.6
Times cited: 21
DOI: 10.1038/S41467-022-31779-2
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“Boosting quantum yields in two-dimensional semiconductors via proximal metal plates”. Lee Y, Forte JD'arf S, Chaves A, Kumar A, Tran TT, Kim Y, Roy S, Taniguchi T, Watanabe K, Chernikov A, Jang JI, Low T, Kim J, Nature Communications 12, 7095 (2021). http://doi.org/10.1038/S41467-021-27418-X
Abstract: The short exciton lifetime and strong exciton-exciton interaction in transition metal dichalcogenides limit the efficiency of exciton emission. Here, the authors show that exciton-exciton interaction in monolayer WS2 can be screened using proximal metal plates, leading to an improved quantum yield. Monolayer transition metal dichalcogenides (1L-TMDs) have tremendous potential as atomically thin, direct bandgap semiconductors that can be used as convenient building blocks for quantum photonic devices. However, the short exciton lifetime due to the defect traps and the strong exciton-exciton interaction in TMDs has significantly limited the efficiency of exciton emission from this class of materials. Here, we show that exciton-exciton interaction in 1L-WS2 can be effectively screened using an ultra-flat Au film substrate separated by multilayers of hexagonal boron nitride. Under this geometry, induced dipolar exciton-exciton interaction becomes quadrupole-quadrupole interaction because of effective image dipoles formed within the metal. The suppressed exciton-exciton interaction leads to a significantly improved quantum yield by an order of magnitude, which is also accompanied by a reduction in the exciton-exciton annihilation (EEA) rate, as confirmed by time-resolved optical measurements. A theoretical model accounting for the screening of the dipole-dipole interaction is in a good agreement with the dependence of EEA on exciton densities. Our results suggest that fundamental EEA processes in the TMD can be engineered through proximal metallic screening, which represents a practical approach towards high-efficiency 2D light emitters.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
DOI: 10.1038/S41467-021-27418-X
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“Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production”. Chen H, Xiong Y, Li J, Abed J, Wang D, Pedrazo-Tardajos A, Cao Y, Zhang Y, Wang Y, Shakouri M, Xiao Q, Hu Y, Bals S, Sargent EHH, Su C-Y, Yang Z, Nature communications 14, 1719 (2023). http://doi.org/10.1038/S41467-023-37401-3
Abstract: Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas. Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon's rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H-2 yields of 4.7 mol g((Co))(-1) and 4.4 mol g((Co))(-1), respectively. Moreover, the H-2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 6
DOI: 10.1038/S41467-023-37401-3
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“Prediction of hyperbolic exciton-polaritons in monolayer black phosphorus”. Wang F, Wang C, Chaves A, Song C, Zhang G, Huang S, Lei Y, Xing Q, Mu L, Xie Y, Yan H, Nature Communications 12, 5628 (2021). http://doi.org/10.1038/S41467-021-25941-5
Abstract: Hyperbolic polaritons exhibit large photonic density of states and can be collimated in certain propagation directions. The majority of hyperbolic polaritons are sustained in man-made metamaterials. However, natural-occurring hyperbolic materials also exist. Particularly, natural in-plane hyperbolic polaritons in layered materials have been demonstrated in MoO3 and WTe2, which are based on phonon and plasmon resonances respectively. Here, by determining the anisotropic optical conductivity (dielectric function) through optical spectroscopy, we predict that monolayer black phosphorus naturally hosts hyperbolic exciton-polaritons due to the pronounced in-plane anisotropy and strong exciton resonances. We simultaneously observe a strong and sharp ground state exciton peak and weaker excited states in high quality monolayer samples in the reflection spectrum, which enables us to determine the exciton binding energy of similar to 452 meV. Our work provides another appealing platform for the in-plane natural hyperbolic polaritons, which is based on excitons rather than phonons or plasmons.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 12.124
DOI: 10.1038/S41467-021-25941-5
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“Anion redox as a means to derive layered manganese oxychalcogenides with exotic intergrowth structures”. Sasaki S, Giri S, Cassidy SJ, Dey S, Batuk M, Vandemeulebroucke D, Cibin G, Smith RI, Holdship P, Grey CP, Hadermann J, Clarke SJ, Nature communications 14, 2917 (2023). http://doi.org/10.1038/S41467-023-38489-3
Abstract: Topochemistry enables step-by-step conversions of solid-state materials often leading to metastable structures that retain initial structural motifs. Recent advances in this field revealed many examples where relatively bulky anionic constituents were actively involved in redox reactions during (de)intercalation processes. Such reactions are often accompanied by anion-anion bond formation, which heralds possibilities to design novel structure types disparate from known precursors, in a controlled manner. Here we present the multistep conversion of layered oxychalcogenides Sr(2)MnO(2)Cu(1.5)Ch(2) (Ch=S, Se) into Cu-deintercalated phases where antifluorite type [Cu(1.5)Ch(2)](2.5-) slabs collapsed into two-dimensional arrays of chalcogen dimers. The collapse of the chalcogenide layers on deintercalation led to various stacking types of Sr(2)MnO(2)Ch(2) slabs, which formed polychalcogenide structures unattainable by conventional high-temperature syntheses. Anion-redox topochemistry is demonstrated to be of interest not only for electrochemical applications but also as a means to design complex layered architectures. Low temperature chemical transformations of solids using high-energy intermediates have enabled the synthesis of a new series of layered oxide chalcogenide containing oxidised chalcogenide dimers promising a new range of solids.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
DOI: 10.1038/S41467-023-38489-3
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“Direct observation of cation diffusion driven surface reconstruction at van der Waals gaps”. Cui W, Lin W, Lu W, Liu C, Gao Z, Ma H, Zhao W, Van Tendeloo G, Zhao W, Zhang Q, Sang X, Nature communications 14, 554 (2023). http://doi.org/10.1038/S41467-023-35972-9
Abstract: Weak interlayer van der Waals (vdW) bonding has significant impact on the surface/interface structure, electronic properties, and transport properties of vdW layered materials. Unraveling the complex atomistic dynamics and structural evolution at vdW surfaces is therefore critical for the design and synthesis of the next-generation vdW layered materials. Here, we show that Ge/Bi cation diffusion along the vdW gap in layered GeBi2Te4 (GBT) can be directly observed using in situ heating scanning transmission electron microscopy (STEM). The cation concentration variation during diffusion was correlated with the local Te-6 octahedron distortion based on a quantitative analysis of the atomic column intensity and position in time-elapsed STEM images. The in-plane cation diffusion leads to out-of-plane surface etching through complex structural evolutions involving the formation and propagation of a non-centrosymmetric GeTe2 triple layer surface reconstruction on fresh vdW surfaces, and GBT subsurface reconstruction from a septuple layer to a quintuple layer. Our results provide atomistic insight into the cation diffusion and surface reconstruction in vdW layered materials. Weak interlayer van der Waals (vdW) bonding has significant impact on the structure and properties of vdW layered materials. Here authors use in-situ aberration-corrected ADF-STEM for an atomistic insight into the cation diffusion in the vdW gaps and the etching of vdW surfaces at high temperatures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
DOI: 10.1038/S41467-023-35972-9
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“Gate-controlled suppression of light-driven proton transport through graphene electrodes”. Huang S, Griffin E, Cai J, Xin B, Tong J, Fu Y, Kravets V, Peeters FM, Lozada-Hidalgo M, Nature communications 14, 6932 (2023). http://doi.org/10.1038/S41467-023-42617-4
Abstract: Recent experiments demonstrated that proton transport through graphene electrodes can be accelerated by over an order of magnitude with low intensity illumination. Here we show that this photo-effect can be suppressed for a tuneable fraction of the infra-red spectrum by applying a voltage bias. Using photocurrent measurements and Raman spectroscopy, we show that such fraction can be selected by tuning the Fermi energy of electrons in graphene with a bias, a phenomenon controlled by Pauli blocking of photo-excited electrons. These findings demonstrate a dependence between graphene's electronic and proton transport properties and provide fundamental insights into molecularly thin electrode-electrolyte interfaces and their interaction with light. Recent experiments have shown that proton transport through graphene electrodes can be promoted by light, but the understanding of this phenomenon remains unclear. Here, the authors report the electrical tunability of this photo-effect, showing a connection between graphene electronic and proton transport properties.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 16.6
DOI: 10.1038/S41467-023-42617-4
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