| {"title": "Direct Time-domain Observation of Conformational Relaxation in Gas-phase\n Cold Collisions", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Garrett K. Drayna", "Christian Hallas", "Kenneth Wang", "S\\'ergio R.\n Domingos", "Sandra Eibenberger", "John M. Doyle", "David Patterson"], "abstract": " Cooling molecules in the gas phase is important for precision spectroscopy,\ncold molecule physics, and physical chemistry. Measurements of conformational\nrelaxation cross sections shed important light on potential energy surfaces and\nenergy flow within a molecule. However, gas-phase conformational cooling has\nnot been previously observed directly. In this work, we directly observe\nconformational dynamics of 1,2-propanediol in cold (6K) collisions with atomic\nhelium using microwave spectroscopy and buffer-gas cooling. Precise knowledge\nand control of the collisional environment in the buffer-gas allows us to\nmeasure the absolute collision cross-section for conformational relaxation.\nSeveral conformers of 1,2-propanediol are investigated and found to have\nrelaxation cross-sections with He ranging from\n$\\sigma=4.7(3.0)\\times10^{-18}\\:\\mathrm{cm}^{2}$ to\n$\\sigma>5\\times10^{-16}\\:\\mathrm{cm}^{2}$. Our method is applicable to a broad\nclass of molecules and could be used to provide information about the potential\nenergy surfaces of previously uninvestigated molecules.\n", "doi": "10.1002/anie.201600030", "arxiv_id": "1601.03359", "pdf_urls": ["https://arxiv.org/pdf/1601.03359"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 55, 4957 (2016)", "categories": "physics.chem-ph physics.atom-ph"} |
| {"title": "Structure and Composition of the 200 K-Superconducting Phase of H2S\n under Ultrahigh Pressure: The Perovskite (SH-)(H3S+)", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Elijah E. Gordon{\\S}", "Ke Xu{\\S}", "Hongjun Xiang", "Annette\n Bussmann-Holder", "Reinhard K. Kremer", "Arndt Simon", "J\\\"urgen K\\\"ohler and\n Myung-Hwan Whangbo"], "abstract": " H2S is converted under ultrahigh pressure (> 110 GPa) to a metallic phase\nthat becomes superconducting with a record Tc of 200 K. It has been proposed\nthat the superconducting phase is body-centered cubic H3S ( Im3m , a = 3.089\n{\\AA}) resulting from a decomposition reaction 3H2S --> 2H3S + S. The analogy\nof H2S and H2O leads us to a very different conclusion. The well-known\ndissociation of water into H3O+ and OH- increases by orders of magnitude under\npressure. An equivalent behavior of H2S is anticipated under pressure with the\ndissociation, 2H2S --> H3S+ + SH- forming a perovskite structure (SH-)(H3S+),\nwhich consists of corner-sharing SH6 octahedra with SH- at each A-site (i.e.,\nthe center of each S8 cube). Our DFT calculations show that the perovskite\n(SH-)(H3S+) is thermodynamically more stable than the Im3m structure of H3S,\nand suggest that the A-site H atoms are most likely fluxional even at Tc.\n", "doi": "10.1002/anie.201511347", "arxiv_id": "1602.02686", "pdf_urls": ["https://arxiv.org/pdf/1602.02686"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed., 2016, 128, 3746-3748", "categories": "cond-mat.supr-con"} |
| {"title": "Boron Nitride Nanosheets Improve Sensitivity and Reusability of Surface\n Enhanced Raman Spectroscopy", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Qiran Cai", "Srikanth Mateti", "Wenrong Yang", "Rob Jones", "Kenji Watanabe", "Takashi Taniguchi", "Shaoming Huang", "Ying Chen and Lu Hua Li"], "abstract": " Surface enhanced Raman spectroscopy (SERS) is a useful multidisciplinary\nanalytic technique. However, it is still a challenge to produce SERS substrates\nthat are highly sensitive, reproducible, stable, reusable, and scalable. Here,\nwe demonstrate that atomically thin boron nitride (BN) nanosheets have many\nunique and desirable properties to help solve this challenge. The synergic\neffect of the atomic thickness, high flexibility, stronger surface adsorption\ncapability, electrical insulation, impermeability, high thermal and chemical\nstability of BN nanosheets can increase the Raman sensitivity by up to two\norders, and in the meantime attain long-term stability and extraordinary\nreusability not achievable by other materials. These advances will greatly\nfacilitate the wider use of SERS in many fields.\n", "doi": "10.1002/anie.201600517", "arxiv_id": "1607.03555", "pdf_urls": ["https://arxiv.org/pdf/1607.03555"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2016, 55, 8405-8409", "categories": "cond-mat.mes-hall cond-mat.mtrl-sci"} |
| {"title": "Self-Organized Stationary Patterns in Networks of Bistable Chemical\n Reactions", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["N. E. Kouvaris", "M. Sebek", "A. S. Mikhailov and I. Z. Kiss"], "abstract": " Experiments with networks of discrete reactive bistable electrochemical\nelements organized in regular and nonregular tree networks are presented to\nconfirm an alternative to the Turing mechanism for the formation of\nself-organized stationary patterns. The results show that the pattern formation\ncan be described by the identification of domains that can be activated\nindividually or in combinations. The method also enabled the localization of\nchemical reactions to network substructures and the identification of critical\nsites whose activation results in complete activation of the system. Although\nthe experiments were performed with a specific nickel electrodissolution\nsystem, they reproduced all the salient dynamic behavior of a general network\nmodel with a single nonlinearity parameter. Thus, the considered\npattern-formation mechanism is very robust, and similar behavior can be\nexpected in other natural or engineered networked systems that exhibit, at\nleast locally, a treelike structure.\n", "doi": "10.1002/anie.201607030", "arxiv_id": "1609.07783", "pdf_urls": ["https://arxiv.org/pdf/1609.07783"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2016, 55, 13267-13270", "categories": "nlin.PS nlin.AO"} |
| {"title": "Stable Co-Catalyst-Free Photocatalytic H2 Evolution From Oxidized\n Titanium Nitride Nanopowders", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Xuemei Zhou", "Eva M. Zolnhofer", "Nhat Truong Nguyen", "Ning Liu", "Karsten\n Meyer", "Patrik Schmuki"], "abstract": " In the present work, a simple strategy is used to thermally oxidize TiN\nnanopowder (ca. 20 nm) to an anatase phase of a TiO2:Ti3+:N compound. In\ncontrast to the rutile phase of such a compound this photocatalyst provides\nphotocatalytic activity for hydrogen evolution under AM1.5 conditions - this\nwithout the use of any noble metal co-catalyst. Moreover the photocatalyst is\nactive and stable over extended periods of time (tested for 4 months).\nImportantly, to achieve successful conversion to the active anatase polymorph,\nsufficiently small starting particles of TiN are needed. The key factor for\ncatalysis is the stabilization of the co-catalytically active Ti3+ species\nagainst oxidation by nitrogen present in the starting material.\n", "doi": "10.1002/anie.201506797", "arxiv_id": "1610.06335", "pdf_urls": ["https://arxiv.org/pdf/1610.06335"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition Volume 54, Issue 45, pages\n 13385-13389, November 2, 2015", "categories": "cond-mat.mtrl-sci"} |
| {"title": "Self-ordered Mo-oxide Nanotube Arrays as Precursor for Aligned MoOx/MoS2\n Core-Shell Nanotubular Structures with a High Density of Reactive Sites", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Bowen Jin", "Xuemei Zhou", "Li Huang", "Markus Licklederer", "Min Yang", "Patrik\n Schmuki"], "abstract": " In the present work we demonstrate the self-organized formation of anodic\nMo-oxide nanotube arrays grown on a Mo sheet under suitable electrochemical\nconditions in glycerol/NH4F electrolytes. The resulting amorphous tubes can be\ncrystallized by annealing to MoO2 or MoO3. The tube walls then can be further\nsulfurized fully or partially to Mo-sulfide to form well-ordered arrays of\nvertically aligned MoOx/MoS2 nanotubes. Under optimized conditions, defined\nMoS2 sheets form on the oxide walls in a layer by layer low angle zig-zag\narrangement that provide a high density of reactive stacking faults. These\ncore-shell nanotube arrays, consisting of tubes with a conductive suboxide core\nand a functional high defect density MoS2 coating, are highly promising for\napplications such as electrocatalysis (hydrogen evolution) or ion insertion\ndevices.\n", "doi": "10.1002/anie.201605551", "arxiv_id": "1610.06350", "pdf_urls": ["https://arxiv.org/pdf/1610.06350"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Volume 55, Issue 40,\n pages 12252-12256, September 26, 2016", "categories": "cond-mat.mtrl-sci"} |
| {"title": "TiO2 nanotubes: N-ion implantation at low-dose provides noble-metal-free\n photocatalytic H2-evolution activity", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Xuemei Zhou", "Volker H\\\"aublein", "Ning Liu", "Nhat Truong Nguyen", "Eva M.\n Zolnhofer", "Hiroaki Tsuchiya", "Manuela S. Killian", "Karsten Meyer", "Lothar Frey", "Patrik Schmuki"], "abstract": " Low-dose nitrogen implantation induces in TiO2 nanotubes a co-catalytic\nactivity for photocatalytic H2-evolution. The use of an ion implantation\nprocess leads to a N-implanted zone only at the top part of the tubes. The\ncoupling of this top layer and the underlying non-implanted part of the\nnanotubes strongly contributes to an efficient carrier separation and thus to a\nsignificantly enhanced H2 generation.\n", "doi": "10.1002/anie.201511580", "arxiv_id": "1610.06562", "pdf_urls": ["https://arxiv.org/pdf/1610.06562"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Volume 55, Issue 11,\n pages 3763-3767, March 7, 2016", "categories": "physics.chem-ph"} |
| {"title": "Hydrogenated anatase: Strong photocatalytic H2 evolution without the use\n of a co-catalyst", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Ning Liu", "Christopher Schneider", "Detlef Freitag", "Umamaheswari\n Venkatesan", "V. R. Reddy Marthala", "Martin Hartmann", "Benjamin Winter", "Erdmann\n Spiecker", "Eva Zolnhofer", "Karsten Meyer", "Patrik Schmuki"], "abstract": " In the present work we show, how a high pressure hydrogenation of commercial\nanatase or anatase/rutile powder can create a photocatalyst for hydrogen\nevolution that is highly effective and stable without the need of any\nadditional co-catalyst. This activation effect can not be observed for rutile.\nFor anatase/rutile mixtures, however, a strong synergistic effect is found\n(similar to findings commonly observed for noble metal decorated TiO2). ESR\nmeasurements indicate the intrinsic co-catalytic activation of anatase TiO2 to\nbe due to specific defect centers formed during hydrogenation.\n", "doi": "10.1002/anie.201408493", "arxiv_id": "1610.06564", "pdf_urls": ["https://arxiv.org/pdf/1610.06564"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Volume 53, Issue 51,\n pages 14201-14205, December 15, 2014", "categories": "physics.chem-ph"} |
| {"title": "Visible Light Triggered Drug Release from TiO2 Nanotube Arrays: A Novel\n Controllable Antibacterial Platform", "year": 2016, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jingwen Xu", "Xuemei Zhou", "Zhida Gao", "Yan-Yan Song", "Patrik Schmuki"], "abstract": " In this work, we use a double-layered stack of TiO2 nanotubes (TiNTs) to\nconstruct a visible-light triggered drug delivery system. Key for visible-light\ndrug release is a hydrophobic cap on the nanotubes containing Au nanoparticles\n(AuNPs). The AuNPs allow for a photocatalytic scission of the hydrophobic chain\nunder visible light. To demonstrate the principle, we loaded antibiotic\n(ampicillin sodium (AMP)) in the lower part of the TiO2 nanotube stack,\ntriggered visible light induced release, and carried out antibacterial studies.\nThe release from the platform becomes most controllable if the drug is\nsilane-grafted in hydrophilic bottom layer for drug storage. Thus visible-light\nphotocatalysis can also determine the release kinetics of the active drug from\nthe nanotube wall.\n", "doi": "10.1002/anie.201508710", "arxiv_id": "1611.03520", "pdf_urls": ["https://arxiv.org/pdf/1611.03520"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Volume 55, Issue 2, pages\n 593-597, January 11, 2016", "categories": "physics.chem-ph cond-mat.mtrl-sci"} |
| {"title": "An Atomic-Scale View of CO and H2 Oxidation on a Pt-Fe3O4 Model Catalyst", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Roland Bliem", "Jessi van der Hoeven", "Adam Zavodny", "Oscar Gamba", "Jiri\n Pavelec", "Petra de Jongh", "Michael Schmid", "Ulrike Diebold", "and Gareth S.\n Parkinson"], "abstract": " Metal-support interactions are frequently invoked to explain the enhanced\ncatalytic activity of metal nanoparticles dispersed over reducible metal-oxide\nsupports, yet the atomic scale mechanisms are rarely known. Here, we use\nscanning tunneling microscopy to study a Pt1-6/Fe3O4 model catalyst exposed to\nCO, H2, O2, and mixtures thereof, at 550 K. CO extracts lattice oxygen at the\ncluster perimeter to form CO2, creating large holes in the metal-oxide surface.\nH2 and O2 dissociate on the metal clusters and spill over onto the support. The\nformer creates create surface hydroxyl groups, which react with the support to\ndesorb water, while atomic oxygen reacts with Fe from the bulk to create new\nFe3O4(001) islands. The presence of the Pt is crucial because it catalyses\nreactions that already occur on the bare iron-oxide surface, but at higher\ntemperatures.\n", "doi": "10.1002/anie.201507368", "arxiv_id": "1702.03998", "pdf_urls": ["https://arxiv.org/pdf/1702.03998"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Volume 54, Issue 47,\n November 16, 2015, Page 13999", "categories": "physics.chem-ph cond-mat.mtrl-sci"} |
| {"title": "The intriguing mechanism of phosphorus anodes for sodium ion batteries\n revealed by operando pair distribution function and X-ray diffraction\n computed tomography", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jonas Sottmann", "Marco Di Michiel", "Helmer Fjellv{\\aa}g", "Lorenzo\n Malavasi", "Serena Margadonna", "Ponniah Vajeeston", "Gavin Vaughan", "David S. Wragg"], "abstract": " Phosphorus is one of the most promising anodes for sodium ion batteries\n(SIBs). Little is known about the structural mechanism of Na/P cycling due to\nthe fact that only one of the structures involved (Na3P) is crystalline. Using\noperando X-ray diffraction computed tomography (XRD-CT) analysed by Rietveld\nand pair distribution (PDF) methods combined with density functional theory\n(DFT) calculations we show that the sodiation and desodiation mechanisms of\nphosphorus are very different. Sodiation follows the thermodynamic path of\nlowest energy from P via NaP to Na3P while desodiation follows a kinetically\ncontrolled deintercalation mechanism in which the layered Na3-xP type structure\nis maintained until P nanoclusters form. Using XRD-CT allows analysis of the 3D\nstructure of the anode, but most importantly, removes the contributions from\nthe sample container and other battery components, particularly important for\nPDF analysis.\n", "doi": "10.1002/anie.201704271", "arxiv_id": "1703.04337", "pdf_urls": ["https://arxiv.org/pdf/1703.04337"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2017, 56, 11385", "categories": "cond-mat.mtrl-sci"} |
| {"title": "The Structural Fate of Individual Multicomponent Metal-Oxide\n Nanoparticles in Polymer Nanoreactors", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jingshan S. Du", "Peng-Cheng Chen", "Brian Meckes", "Zhuang Xie", "Jinghan\n Zhu", "Yuan Liu", "Vinayak P. Dravid", "and Chad A. Mirkin"], "abstract": " Multicomponent nanoparticles can be synthesized with either homogeneous or\nphase-segregated architectures depending on the synthesis conditions and\nelements incorporated. To understand the parameters that determine their\nstructural fate, multicomponent metal-oxide nanoparticles consisting of\ncombinations of Co, Ni, and Cu were synthesized via scanning probe block\ncopolymer lithography and characterized using correlated electron microscopy.\nThese studies revealed that the miscibility, ratio of the metallic components,\nand the synthesis temperature determine the crystal structure and architecture\nof the nanoparticles. A Co-Ni-O system forms a rock salt structure largely due\nto the miscibility of CoO and NiO, while Cu-Ni-O, which has large miscibility\ngaps, forms either homogeneous oxides, heterojunctions, or alloys depending on\nthe annealing temperature and composition. Moreover, a higher ordered\nstructure, Co-Ni-Cu-O, was found to follow the behavior of lower ordered\nsystems.\n", "doi": "10.1002/anie.201703296", "arxiv_id": "1705.05760", "pdf_urls": ["https://arxiv.org/pdf/1705.05760"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2017, 56, 7625", "categories": "physics.chem-ph cond-mat.mtrl-sci"} |
| {"title": "Magic Graphene Clusters Formation in the graphene CVD growth process on\n Ru and Rh", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Junfeng Gao and Feng Ding"], "abstract": " To improve atomically controlled chemical vapor deposition (CVD) growth of\ngraphene, understanding the evolution from various carbon species to a graphene\nnuclei on various catalyst surfaces is essential. Experimentally, an\nultra-stable carbon cluster on Ru(0001), Rh(111) surfaces was observed, while\nits structure and formation process were still under highly debate. Using ab\ninitio calculations and kinetic analyses, we disclosed a specific type of\ncarbon clusters, composed of a C21 core and a few dangling C atoms around, were\nexceptional stable in the size range from 21 to 27. The most stable one of\nthem, an isomer of C24 characterized as three dangling C atoms attached to the\nC21 (denoted as C21-3C), is the most promising candidate for the experimental\nobservation. The ultra-stability of C21-3C originates from both the stable core\nand the appropriate passivation of dangling carbon atoms by the catalyst\nsurface.\n", "doi": "10.1002/anie.201406570", "arxiv_id": "1707.04396", "pdf_urls": ["https://arxiv.org/pdf/1707.04396"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition 53, 14031-14035 (2014)", "categories": "cond-mat.mtrl-sci physics.atm-clus physics.chem-ph"} |
| {"title": "Charge Transport and Conductance Switching of Redox-active Azulene\n Derivatives", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Florian Schwarz", "Michael Koch", "Georg Kastlunger", "Heinz Berke", "Robert\n Stadler", "Koushik Venkatesan and Emanuel Loertscher"], "abstract": " Azulene (Az) is a non-alternating, aromatic hydrocarbon composed of a\nfive-membered, electron-rich and a seven-membered, electron-poor ring; an\nelectron distribution that provides intrinsic redox activity. By varying the\nattachment points of the two electrode-bridging substituents to the Az centre,\nthe influence of the redox functionality on charge transport is evaluated. The\nconductance of the 1,3 Az derivative is at least one order of magnitude lower\nthan those of the 2,6 Az and 4,7 Az derivatives, in agreement with density\nfunctional theory (DFT) calculations. In addition, only 1,3 Az exhibits\npronounced nonlinear current-voltage characteristics with hysteresis,\nindicating a bias-dependent conductance switching. DFT identifies the LUMO to\nbe nearest to the Fermi energy of the electrodes, but to be an active transport\nchannel only in the case of the 2,6 and the 4,7 Az derivatives, whereas the 1,3\nAz derivative uses the HOMO at low and the LUMO+1 at high bias. In return, the\nlocalized, weakly coupled LUMO of 1,3 Az creates a slow electron-hopping\nchannel responsible for the voltage-induced switching due to the occupation of\na single MO.\n", "doi": "10.1002/anie.201605559", "arxiv_id": "1709.00277", "pdf_urls": ["https://arxiv.org/pdf/1709.00277"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "English version: Angew. Chem. Int. Ed. 55, 11781 (2016), German\n version: Angew. Chem. 128, 11956 (2016)", "categories": "cond-mat.mes-hall"} |
| {"title": "Experimentally Probing 'Hydrophobic' Water at the Gold Electrode/Aqueous\n Interface", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Yujin Tong and Fran\\c{c}ois Lapointe and Matin Th\\\"amer and Martin\n Wolf and R. Kramer Campen (Fritz Haber Institute of the Max Planck Society", "Berlin", "Germany)"], "abstract": " Quantitative description of reaction mechanisms in aqueous phase\nelectrochemistry requires experimental characterization of local water\nstructure at the electrode/aqueous interface and its evolution with changing\npotential. Gaining such insight experimentally under electrochemical conditions\nis a formidable task. Here we characterize the potential dependent structure of\na sub-population of interfacial water that have one OH group pointing towards a\ngold working electrode using interface specific vibrational spectroscopy in a\nthin film electrochemical cell. Such 'free-OH' groups are the molecular level\nobservable of an extended hydrophobic interface. This 'free-OH' interacts only\nweakly with the Au surface at all potentials, has an orientational distribution\nthat narrows as one approaches the potential of zero charge and disappears on\nthe oxidation of the gold electrode.\n", "doi": null, "arxiv_id": "1711.01376", "pdf_urls": ["https://arxiv.org/pdf/1711.01376"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew Chem Int Ed (2017) 4211-4214", "categories": "physics.chem-ph"} |
| {"title": "Electron--Proton Decoupling in Excited-State Hydrogen Atom Transfer in\n the Gas Phase", "year": 2017, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Mitsuhiko Miyazaki", "Ryuhei Ohara", "Kota Daigoku", "Kenro Hashimoto", "Jonathan R.Woodward", "Claude Dedonder (PIIM)", "Christophe Jouvet (PIIM)", "Masaaki Fujii"], "abstract": " Hydrogen-release by photoexcitation, excited-state- hydrogen-transfer (ESHT),\nis one of the important photo- chemical processes that occur in aromatic acids\nand is responsible for photoprotection of biomolecules. The mecha- nism is\ndescribed by conversion of the initial state to a charge- separated state along\nthe O(N)-H bond elongation, leading to dissociation. Thus ESHT is not a simple\nH-atom transfer in which a proton and a 1s electron move together. Here we show\nthat the electron-transfer and the proton-motion are decoupled in gas-phase\nESHT. We monitor electron and proton transfer independently by picosecond\ntime-resolved near-infrared and infrared spectroscopy for isolated\nphenol--(ammonia)5, a benchmark molecular cluster. Electron transfer from\nphenol to ammonia occurred in less than 3 picoseconds, while the overall H-atom\ntransfer took 15 picoseconds. The observed electron-proton decoupling will\nallow for a deeper understanding and control of of photochemistry in\nbiomolecules\n", "doi": "10.1002/anie.201506467", "arxiv_id": "1712.02993", "pdf_urls": ["https://arxiv.org/pdf/1712.02993"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Wiley-VCH Verlag, 2015,\n 54", "categories": "physics.atm-clus"} |
| {"title": "Large second harmonic generation of LiCs2PO4 caused by the metal-cation-centered groups", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Xiyue Cheng", "Myung-Hwan Whangbo", "Guo-Cong Guo", "Maochun Hong", "Shuiquan Deng"], "abstract": "We evaluated the individual atom contributions to the second harmonic generation (SHG) coefficients of LiCs2PO4 (LCPO) by introducing the partial response functionals on the basis of first principles calculations. The SHG response of LCPO is dominated by the metal-cation-centered groups CsO6 and LiO4, not by the nonmetal-cation-centered groups PO4 one expects from the existing models and theories. The SHG coefficients of LCPO are determined mainly by the occupied orbitals O-2p and Cs-5p as well as by the unoccupied orbitals Cs-5d and Li-2p. For the SHG response of a material, the polarizable atomic orbitals of the occupied and the unoccupied states are both important.", "doi": "10.1002/anie.201711465", "arxiv_id": "1803.00748", "pdf_urls": ["https://arxiv.org/pdf/1803.00748"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2018, 57, 3933-3937", "categories": "cond-mat.mtrl-sci"} |
| {"title": "Maximum spin polarization in chromium dimer cations as demonstrated by\n x-ray magnetic circular dichroism spectroscopy", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Vicente Zamudio-Bayer", "Konstantin Hirsch", "Andreas Langenberg", "Markus\n Niemeyer", "Marlene Vogel", "Arkadiusz {\\L}awicki", "Akira Terasaki", "J. Tobias Lau", "and Bernd von Issendorff"], "abstract": " X-ray magnetic circular dichroism spectroscopy has been used to characterize\nthe electronic structure and magnetic moment of Cr$_2^+$. Our results indicate\nthat the removal of a single electron from the $4s\\sigma_g$ bonding orbital of\nCr$_2$ drastically changes the preferred coupling of the $3d$ electronic spins.\nWhile the neutral molecule has a zero-spin ground state with a very short bond\nlength, the molecular cation exhibits a ferromagnetically coupled ground state\nwith the highest possible spin of $S=11/2$, and almost twice the bond length of\nthe neutral molecule. This spin configuration can be interpreted as a result of\nindirect exchange coupling between the $3d$ electrons of the two atoms that is\nmediated by the single $4s$ electron through a strong intraatomic $3d$-$4s$\nexchange interaction. Our finding allows an estimate of the relative energies\nof two states that are often discussed as ground-state candidates, the\nferromagnetically coupled $^{12}\\Sigma$ and the low-spin $^2\\Sigma$ state.\n", "doi": "10.1002/anie.201411018", "arxiv_id": "1804.03866", "pdf_urls": ["https://arxiv.org/pdf/1804.03866"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 54, 4498 (2015)", "categories": "physics.chem-ph physics.atm-clus"} |
| {"title": "Chemistry with Graphene and Graphene Oxide - Challenges for Synthetic\n Chemists", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Siegfried Eigler", "Andreas Hirsch"], "abstract": " The chemical production of graphene as well as its controlled wet- chemical\nmodification is a challenge for synthetic chemists and the characterization of\nreaction products requires sophisticated analytic methods. In this review we\nfirst describe the structure of graphene and graphene oxide. We then outline\nthe most important synthetic methods which are used for the production of these\ncarbon based nanomaterials. We summarize the state-of-the-art for their\nchemical functionalization by non-covalent and covalent approaches. We put\nspecial emphasis on the differentiation of the terms graphite, graphene,\ngraphite oxide and graphene oxide. An improved fundamental knowledge about the\nstructure and the chemical properties of graphene and graphene oxide is an\nimportant prerequisite for the development of practical applications.\n", "doi": "10.1002/anie.201402780", "arxiv_id": "1805.03088", "pdf_urls": ["https://arxiv.org/pdf/1805.03088"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2014, 53, 7720-7738", "categories": "physics.chem-ph"} |
| {"title": "Double- and Single-Sided bis-Functionalization of Graphene", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Kathrin C. Knirsch", "Ricarda A. Sch\\\"afer", "Frank Hauke", "Andreas Hirsch"], "abstract": " For the first time bis-functionalization of graphene employing two successive\nreduction and covalent bond formation steps are reported. Both bulk\nfunctionalization in solution and functionalization of individual sheets\ndeposited on surfaces have been carried out. Whereas in the former case attacks\nfrom both sides of the basal plane are possible and can lead to strain-free\narchitectures, in the latter case, retro-functionalizations can get important\nwhen the corresponding anion of the addend represents a sufficiently good\nleaving group.\n", "doi": "10.1002/anie.201511807", "arxiv_id": "1805.09128", "pdf_urls": ["https://arxiv.org/pdf/1805.09128"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2016, 55, 5861-5864", "categories": "physics.chem-ph cond-mat.mtrl-sci"} |
| {"title": "Noncovalent Functionalization of Black Phosphorus", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Gonzalo Abell\\'an", "Vicent Lloret", "Udo Mundloch", "Mario Marcia", "Christian Neiss", "Andreas G\\\"orling", "Maria Varela", "Frank Hauke", "Andreas Hirsch"], "abstract": " The first non-covalent functionalization of black phosphorus (BP) is\npresented. The treatment of BP with electron- withdrawing\n7,7,8,8-tetracyano-p-quinodimethane (TCNQ) leads to electron transfer from BP\nto the organic dopant. On the other hand, the non-covalent interaction of BP\nwith perylene diimide is mainly due to van-der-Waals interactions but also\nleads to a considerable stabilization of the BP flakes against oxygen\ndegradation.\n", "doi": "10.1002/anie.201604784", "arxiv_id": "1805.09130", "pdf_urls": ["https://arxiv.org/pdf/1805.09130"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2016, 55, 14557-14562", "categories": "physics.chem-ph cond-mat.mtrl-sci"} |
| {"title": "Substrate-Modulated Reductive Graphene Functionalization", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Ricarda A. Sch\\\"afer", "Konstantin Weber", "Frank Hauke", "Vojislav Krstic", "Bernd Meyer", "Andreas Hirsch"], "abstract": " Covalently functionalizing mechanical exfoliated monolayer and bilayer\ngraphenides with {\\lambda}-iodanes led to the discovery that the monolayers\nsupported on a SiO2 substrate are considerably more reactive than bilayers as\ndemonstrated by statistical Raman spectroscopy/microscopy. Supported by DFT\ncalculations we show that ditopic addend binding leads to much more stable\nproducts than the corresponding monotopic reactions due to much lower lattice\nstrain of the reactions products. The chemical nature of the substrate\n(graphene versus SiO2) plays a crucial role.14858-14862.\n", "doi": "10.1002/anie.201607427", "arxiv_id": "1805.09131", "pdf_urls": ["https://arxiv.org/pdf/1805.09131"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2016, 55, 14858-14862", "categories": "physics.chem-ph cond-mat.mtrl-sci"} |
| {"title": "Poly(ionic liquid)-Derived Carbon with Site-Specific N-Doping and\n Biphasic Heterojunction for Enhanced CO2 Capture and Sensing", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jiang Gong", "Markus Antonietti and Jiayin Yuan"], "abstract": " CO2 capture is a pressing global environmental issue that drives scientists\nto develop creative strategies for tackling this challenge. The concept in this\ncontribution is to produce site specific nitrogen doping in microporous carbon\nfibers. It creates a carbon/carbon heterojunction by using poly(ionic liquid)\n(PIL) as soft activation agent that deposits nitrogen species exclusively on\nthe skin of commercial microporous carbon fibers. Such carbon-based biphasic\nheterojunction amplifies the interaction between carbon fiber and CO2 molecule\nfor unusually high CO2 uptake and resistive sensing.\n", "doi": "10.1002/anie.201702453", "arxiv_id": "1810.06418", "pdf_urls": ["https://arxiv.org/pdf/1810.06418"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Volume56, Issue26, June\n 19, 2017,Pages 7557-7563", "categories": "physics.app-ph cond-mat.mtrl-sci"} |
| {"title": "Ambient Electro-Synthesis of Ammonia - Electrode Porosity and\n Composition Engineering", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Hong Wang", "Lu Wang", "Qiang Wang", "Shuyang Ye", "Wei Sun", "Yue Shao", "Zhiping\n Jiang", "Qiao Qiao", "Yimei Zhu", "Pengfei Song", "Debao Li", "Le He", "Xiaohong Zhang", "Jiayin Yuan", "Tom Wu", "Geoffrey A. Ozin"], "abstract": " Ammonia, key precursor for fertilizer production, convenient hydrogen carrier\nand emerging clean fuel, plays a pivotal role in sustaining life on earth.\nCurrently, the main route for NH3 synthesis is via the heterogeneous catalytic\nHaber-Bosch process (N2+3H2 - 2NH3), which proceeds under extreme conditions of\ntemperature and pressure with a very large carbon footprint. Herein we report\nthat a pristine nitrogen-doped nanoporous graphitic carbon membrane (NCM) can\nelectrochemically convert N2 into NH3 in an aqueous acidic solution under\nambient conditions. The Faradaic efficiency and rate of production of NH3 on\nthe NCM electrode reach 5.2% and 0.08 g m-2 h-1, respectively. After\nfunctionalization of the NCM with Au nanoparticles (Au NPs) these performance\nmetrics are dramatically enhanced to 22% and 0.36 g m-2 h-1, respectively.\nThese efficiencies and rates for the production of NH3 at room temperature and\natmospheric pressure are unprecedented. As this system offers the potential to\nbe scaled to industrial proportions there is a high likelihood it might\ndisplace the century old Haber-Bosch process.\n", "doi": "10.1002/anie.201805514", "arxiv_id": "1810.13007", "pdf_urls": ["https://arxiv.org/pdf/1810.13007"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Publication cover image,\n Volume57, Issue38, September 17, 2018 Pages 12360-12364", "categories": "physics.chem-ph"} |
| {"title": "Quantifying Chemical Structure and Atomic Energies in Amorphous Silicon\n Networks", "year": 2018, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Noam Bernstein", "Bishal Bhattarai", "G\\'abor Cs\\'anyi", "David A. Drabold", "Stephen R. Elliott", "Volker L. Deringer"], "abstract": " Amorphous materials are coming within reach of realistic computer\nsimulations, but new approaches are needed to fully understand their intricate\natomic structures. Here, we show how machine-learning (ML)-based techniques can\ngive new, quantitative chemical insight into the atomic-scale structure of\namorphous silicon (a-Si). Based on a similarity function (\"kernel\"), we define\na structural metric that unifies the description of nearest- and\nnext-nearest-neighbor environments in the amorphous state. We apply this to an\nensemble of a-Si networks, generated in melt-quench simulations with an\nML-based interatomic potential, in which we tailor the degree of ordering by\nvarying the quench rates down to $10^{10}$ K/s (leading to a structural model\nthat is lower in energy than the established WWW network). We then show how\n\"machine-learned\" atomic energies permit a chemical interpretation, associating\ncoordination defects in a-Si with distinct energetic stability regions. The\napproach is straightforward and inexpensive to apply to arbitrary structural\nmodels, and it is therefore expected to have more general significance for\ndeveloping a quantitative understanding of the amorphous state.\n", "doi": "10.1002/anie.201902625", "arxiv_id": "1811.11069", "pdf_urls": ["https://arxiv.org/pdf/1811.11069"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 58, 7057 (2019)", "categories": "cond-mat.mtrl-sci"} |
| {"title": "Electron-proton Co-doping Induced Metal-insulator Transition in VO2 Film\n via Surface Self-assembled Ascorbic Acid Molecules", "year": 2019, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Bowen Lia", "Liyan Xieb", "Zhaowu Wang", "Shi Chen", "Hui Ren", "Yuliang Chen", "Chengming Wang", "Guobin Zhang", "Jun Jiang and Chongwen Zou"], "abstract": " Charge doping is an effective way to induce metal-insulate transition (MIT)\nin correlated materials for many important utilizations, which is however\npractically limited by problem of low stability. In this study, we have\nachieved pronounced phase modulation and stabilized the metallic state of\nmonoclinic vanadium dioxide (VO2) at room temperature, via a novel\nelectron-proton co-doping mechanism driven by surface absorption of\nself-assembled L-ascorbic acid (AA) molecules. The ionized AA- species in\nsolution donate effective electrons to the adsorbed VO2 surface, which then\nelectrostatically attract surrounding protons to penetrate, and eventually\nresults in stable hydrogen-doped metallic VO2. The variations of phase and\nelectronic structures as well as the electron occupancy of V-3d/O-2p hybrid\norbitals were examined by synchrotron characterizations and first-principle\ntheoretical simulations, which explain the formation of stable metallic state.\nImportantly, the adsorbed molecules protect hydrogen dopants from escaping out\nof lattice and thereby stabilize the metallic phase for VO2. Such an\nelectron-proton co-doping mechanism driven by suitable molecules absorption\nwould open a new door for engineering properties of correlated oxide materials.\n", "doi": "10.1002/ange.201904148", "arxiv_id": "1901.05597", "pdf_urls": ["https://arxiv.org/pdf/1901.05597"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 58 (2019)13711", "categories": "physics.app-ph cond-mat.str-el"} |
| {"title": "Post Graphene 2D Chemistry: The Emerging Field of Molybdenum Disulfide\n and Black Phosphorus Functionalization", "year": 2019, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Andreas Hirsch", "Frank Hauke"], "abstract": " The current state of the chemical functionalization of three types of single\nsheet 2D materials, namely, graphene, molybdenum disulfide (MoS2), and black\nphosphorus (BP) is summarized. Such 2D sheet polymers represent currently an\nemerging field at the interface of synthetic chemistry, physics, and materials\nscience. Both covalent and non-covalent functionalization of sheet\narchitectures allows for a systematic modification of their properties, i.e. an\nimprovement of solubility and processability, the prevention of re-aggregation\nor a band gap tuning. Next to successful functionalization concepts also\nfundamental challenges are addressed. These include the insolubility and\npolydispersity of most 2D sheet polymers, the development of suitable\ncharacterization tools, the identification of effective binding strategies, the\nchemical activation of the usually rather unreactive basal planes for covalent\naddend binding, and the regioselectivity of plane addition reactions. Although\na number of these questions remain elusive in this review, the first promising\nconcepts to overcome such hurdles have been listed.\n", "doi": "10.1002/anie.201708211", "arxiv_id": "1903.06460", "pdf_urls": ["https://arxiv.org/pdf/1903.06460"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2018, 57, 4338-4354", "categories": "physics.chem-ph physics.app-ph"} |
| {"title": "Efficient Electrocatalytic Reduction of CO2 by Nitrogen-Doped Nanoporous\n Carbon-Carbon Nanotube Membranes - A Step Towards the Electrochemical CO2\n Refinery", "year": 2019, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Hong Wang", "Jia Jia", "Pengfei Song", "Qiang Wang", "Debao Li", "Shixiong Min", "Chenxi Qian", "Lu Wang", "Young Feng Li", "Chun Ma", "Tom Wu", "Jiayin Yuan", "Markus\n Antonietti", "Geoffrey A. Ozin"], "abstract": " The search for earth abundant, efficient and stable electrocatalysts that can\nenable the chemical reduction of CO2 to value-added chemicals and fuels at an\nindustrially relevant scale, is a high priority for the development of a global\nnetwork of renewable energy conversion and storage systems that can\nmeaningfully impact greenhouse gas induced climate change. Here we introduce a\nstraightforward, low cost, scalable and technologically relevant method to\nmanufacture an all-carbon, electroactive, nitrogen-doped nanoporous\ncarbon-carbon nanotube composite membrane, dubbed \"HNCM-CNT\". The membrane is\ndemonstrated to function as a binder-free, high-performance electrode for the\nelectrocatalytic reduction of CO2 to formate. The Faradaic efficiency for the\nproduction of formate is 81%. Furthermore, the robust structural and\nelectrochemical properties of the membrane endow it with excellent long-term\nstability.\n", "doi": null, "arxiv_id": "1905.01466", "pdf_urls": ["https://arxiv.org/pdf/1905.01466"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "angewandte Chemie International Edition, Volume56, Issue27, June\n 26, 2017, Pages 7847-7852", "categories": "physics.chem-ph"} |
| {"title": "SERS discrimination of single amino acid residue in single peptide by\n plasmonic nanocavities", "year": 2019, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jian-An Huang", "Mansoureh Z. Mousavi", "Giorgia Giovannini", "Yingqi Zhao", "Aliaksandr Hubarevich", "Denis Garoli", "Francesco De Angelis"], "abstract": " Surface-enhanced Raman spectroscopy (SERS) is a sensitive label-free optical\nmethod that can provide fingerprint Raman spectra of biomolecules such as DNA,\namino acids and proteins. While SERS of single DNA molecule has been recently\ndemonstrated, Raman analysis of single protein sequence was not possible\nbecause the SERS spectra of proteins are usually dominated by signals of\naromatic amino acid residues. Here, we used electroplasmonic approach to trap\nsingle gold nanoparticle in a nanohole for generating a plasmonic nanocavity\nbetween the trapped nanoparticle and the nanopore wall. The giant field\ngenerated in the nanocavity was so sensitive and localized that it enables SERS\ndiscrimination of 10 distinct amino acids at single-molecule level. The\nobtained spectra are used to analyze the spectra of 2 biomarkers (Vasopressin\nand Oxytocin) made of a short sequence of 9 amino-acids. Significantly, we\ndemonstrated identification of single non-aromatic amino acid residues in a\nsingle short peptide chain as well as discrimination between two peptides with\nsequences distinguishable in 2 specific amino-acids. Our result demonstrate the\nhigh sensitivity of our method to identify single amino acid residue in a\nprotein chain and a potential for further applications in proteomics and\nsingle-protein sequencing.\n", "doi": "10.1002/anie.202000489", "arxiv_id": "1908.04206", "pdf_urls": ["https://arxiv.org/pdf/1908.04206"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, 59, 11423-11431 (2020)", "categories": "q-bio.QM physics.optics"} |
| {"title": "Rapid one-step synthesis and compaction of high-performance n-type\n Mg3Sb2 thermoelectrics", "year": 2019, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jiawei Zhang", "Lirong Song", "Bo Brummerstedt Iversen"], "abstract": " n-type Mg3Sb2-based compounds are emerging as a promising class of low-cost\nthermoelectric materials due to their extraordinary performance at low and\nintermediate temperatures. However, so far high thermoelectric performance has\nmerely been reported in n-type Mg3Sb2-Mg3Bi2 alloys with a large amount of Bi.\nMoreover, current synthesis methods of n-type Mg3Sb2 bulk thermoelectrics\ninvolve multi-step processes that are time- and energy-consuming. Here we\nreport a fast and straightforward approach to fabricate n-type Mg3Sb2\nthermoelectrics using spark plasma sintering, which combines the synthesis and\ncompaction in one step. Using this method, we achieve a high thermoelectric\nfigure of merit zT of ~0.4-1.5 at 300-725 K in n-type (Sc, Te)-doped Mg3Sb2\nwithout alloying with Mg3Bi2. In comparison with the currently reported\nsynthesis methods, the complexity, process time, and cost of the new method are\nsignificantly reduced. This work demonstrates a simple, low-cost route for the\npotential large-scale production of n-type Mg3Sb2 thermoelectrics.\n", "doi": "10.1002/anie.201912909", "arxiv_id": "1911.10549", "pdf_urls": ["https://arxiv.org/pdf/1911.10549"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 10.1002/anie.201912909, 2019", "categories": "cond-mat.mtrl-sci"} |
| {"title": "Colloidal Quantum Nanostructures: Emerging Materials for Display\n Applications", "year": 2019, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Yossef E. Panfil", "Meirav Oded", "Uri Banin"], "abstract": " Colloidal semiconductor nanocrystals (SCNCs) or, more broadly, colloidal\nquantum nanostructures constitute outstanding model systems for investigating\nsize and dimensionality effects. Their nanoscale dimensions lead to quantum\nconfinement effects that enable tuning of their optical and electronic\nproperties. Thus, emission color control with narrow photoluminescence spectra,\nwide absorbance spectra, and outstanding photostability, combined with their\nchemical processability through control of their surface chemistry leads to the\nemergence of SCNCs as outstanding materials for present and next-generation\ndisplays. In this Review, we present the fundamental chemical and physical\nproperties of SCNCs, followed by a description of the advantages of different\ncolloidal quantum nanostructures for display applications. The open challenges\nwith respect to their optical activity are addressed. Both photoluminescent and\nelectroluminescent display scenarios utilizing SCNCs are described.\n", "doi": "10.1002/anie.201708510", "arxiv_id": "1912.04667", "pdf_urls": ["https://arxiv.org/pdf/1912.04667"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2018, 57, 4274", "categories": "physics.app-ph cond-mat.mes-hall"} |
| {"title": "Spectroscopies and electron microscopies unravel the origin of the first\n colour photographs", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Victor de Seauve", "Marie-Ang\\'elique Languille", "Mathieu Kociak", "St\\'ephanie Belin", "James Ablett", "Christine Andraud", "Odile St\\'ephan", "Jean-Pascal Rueff", "Emiliano Fonda", "Bertrand Lav\\'edrine"], "abstract": " The first colours photographs were created by a process introduced by Edmond\nBecquerel in 1848. The nature of these photochromatic images colours motivated\na debate between scientists during the 19th century, which is still not\nsettled. We present the results of chemical analysis (EDX, HAXPES and EXAFS)\nand morphology studies (SEM, STEM) aiming at explaining the optical properties\nof the photochromatic images (UV-visible spectroscopy and low loss EELS). We\nrule out the two hypotheses (pigment and interferences) that have prevailed\nsince 1848, respectively based on variations in the oxidation degree of the\ncompound forming the sensitized layer and periodically spaced photolytic silver\nplanes. A study of the silver nanoparticles dispersions contained in the\ncoloured layers showed specific localizations and size distributions of the\nnanoparticles for each colour. These results allow us to formulate a plasmonic\nhypothesis on the origin of the photochromatic images colours.\n", "doi": "10.1002/anie.202001241", "arxiv_id": "2001.08078", "pdf_urls": ["https://arxiv.org/pdf/2001.08078"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 59 (2020) 9113-9119", "categories": "physics.app-ph cond-mat.mtrl-sci"} |
| {"title": "Collective All-Carbon Magnetism in Triangulene Dimers", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Shantanu Mishra", "Doreen Beyer", "Kristjan Eimre", "Ricardo Ortiz", "Joaquin\n Fernandez-Rossier", "Reinhard Berger", "Oliver Groening", "Carlo A. Pignedoli", "Roman Fasel", "Xinliang Feng", "Pascal Ruffieux"], "abstract": " Triangular zigzag nanographenes, such as triangulene and its pi-extended\nhomologues, have received widespread attention as organic nanomagnets for\nmolecular spintronics, and may serve as building blocks for high-spin networks\nwith long-range magnetic order - of immense fundamental and technological\nrelevance. As a first step toward these lines, we present the on-surface\nsynthesis and a proof-of-principle experimental study of magnetism in\ncovalently bonded triangulene dimers. On-surface reactions of\nrationally-designed precursor molecules on Au(111) lead to the selective\nformation of triangulene dimers in which the triangulene units are either\ndirectly connected through their minority sublattice atoms, or are separated\nvia a 1,4-phenylene spacer. The chemical structures of the dimers have been\ncharacterized by bond-resolved scanning tunneling microscopy. Scanning\ntunneling spectroscopy and inelastic electron tunneling spectroscopy\nmeasurements reveal collective singlet-triplet spin excitations in the dimers,\ndemonstrating efficient inter-triangulene magnetic coupling.\n", "doi": "10.1002/anie.202002687", "arxiv_id": "2003.00753", "pdf_urls": ["https://arxiv.org/pdf/2003.00753"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 59, 12041-12047 (2020)", "categories": "cond-mat.mes-hall"} |
| {"title": "The Influence of Elastic Strain on Catalytic Activity Towards the\n Hydrogen Evolution Reaction", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Kai Yan", "Tuhina Adit Maark", "Alireza Khorshidi", "Vijay A. Sethuraman", "Andrew Peterson", "Pradeep R. Guduru"], "abstract": " Understanding the role of elastic strain in modifying catalytic reaction\nrates is crucial for catalyst design, but experimentally, this effect is often\ncoupled with a ligand effect. To isolate the strain effect, we have\ninvestigated the influence of externally applied elastic strain on the\ncatalytic activity of metal films towards the hydrogen evolution reaction\n(HER). We show that elastic strain tunes the catalytic activity in a controlled\nand predictable way. Both theory and experiment show strain controls reactivity\nin a controlled manner consistent with the qualitative predictions of the HER\nvolcano plot and the d-band theory: Ni and Pt activity were accelerated by\ncompression, while Cu activity was accelerated by tension. By isolating the\nelastic strain effect from the ligand effect, this study provides a greater\ninsight into the role of elastic strain in controlling electrocatalytic\nactivity.\n", "doi": "10.1002/anie.201508613", "arxiv_id": "2003.04085", "pdf_urls": ["https://arxiv.org/pdf/2003.04085"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, 55, 6175-6181, 2016", "categories": "physics.app-ph cond-mat.mtrl-sci"} |
| {"title": "Pressure-induced inverse order-disorder transition in double perovskites", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Zheng Deng", "Chang-Jong Kang", "Mark Croft", "Wenmin Li", "Xi Shen", "Jianfa\n Zhao", "Richeng Yu", "Changqing Jin", "Gabi Kotliar", "Sizhan Liu", "T. A. Tyson", "Ryan\n Tappero", "Martha Greenblatt"], "abstract": " Given the consensus that pressure improves cation order in most of known\nmaterials, a discovery of pressure-induced disorder could require\nreconsideration of order-disorder transition in solid state physics/chemistry\nand geophysics. Double perovskites Y2CoIrO6 and Y2CoRuO6 synthesized at ambient\npressure show B-site order, while the polymorphs synthesized at 6 and 15 GPa\nare partially-ordered and disordered respectively. With the decrease of\nordering degrees, the lattices are shrunken and the crystal structures alter\nfrom monoclinic to orthorhombic symmetry. Correspondingly, long-range\nferrimagnetic order in the B-site ordered phases are gradually overwhelmed by\nB-site disorder. Theoretical calculations suggest that unusual unit cell\ncompressions under external pressures unexpectedly stabilize the disordered\nphases of Y2CoIrO6 and Y2CoRuO6.\n", "doi": "10.1002/anie.202001922", "arxiv_id": "2003.08025", "pdf_urls": ["https://arxiv.org/pdf/2003.08025"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition 59, 8240 (2020)", "categories": "cond-mat.mtrl-sci cond-mat.str-el"} |
| {"title": "A cyanine dye rotaxane porphyrin nanoring complex as a model light\n harvesting system", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jiratheep Pruchyathamkorn", "William J. Kendrick", "Andrew T. Frawley", "Andrea Mattioni", "Felipe Caycedo-Soler", "Susana F. Huelga", "Martin B. Plenio", "and Harry L. Anderson"], "abstract": " A nanoring-rotaxane supramolecular assembly, with a Cy7 cyanine dye\n(hexamethylindotricarbocyanine) threaded along the axis of the nanoring, has\nbeen synthesized as a model for the energy transfer between the light\nharvesting complex LH1 and the reaction center in purple bacteria\nphotosynthesis. The complex displays efficient energy transfer from the central\ncyanine dye to the surrounding zinc porphyrin nanoring. We present a\ntheoretical model that reproduces the absorption spectrum of the nanoring and\nquantifies the excitonic coupling between the nanoring and the central dye,\nexplaining the efficient energy transfer and elucidating the similarity with\nstructurally related natural light harvesting systems.\n", "doi": "10.1002/anie.202006644 10.1002/ange.202006644", "arxiv_id": "2006.08349", "pdf_urls": ["https://arxiv.org/pdf/2006.08349"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 59, 16455-16458 (2020)", "categories": "physics.chem-ph cond-mat.mtrl-sci quant-ph"} |
| {"title": "Amperometric Measurements and Dynamic Models Reveal a Mechanism for How\n Zinc Alters Neurotransmitter Release", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Lin Ren", "Alexander Oleinick (PASTEUR)", "Irina Svir (PASTEUR)", "Christian\n Amatore (PASTEUR)", "Andrew Ewing"], "abstract": " Zinc, a suspected potentiator of learning and memory, is shown to affect\nexocytotic release and storage in neurotransmitter-containing vesicles.\nStructural and size analysis of the vesicular dense core and halo using\ntransmission electron microscopy was combined with single-cell amperometry to\nstudy the vesicle size changes induced after zinc treatment and to compare\nthese changes to theoretical predictions based on the concept of partial\nrelease as opposed to full quantal release. This powerful combined analytical\napproach establishes the existence of an unsuspected strong link between\nvesicle structure and exocytotic dynamics which can be used to explain the\nmechanism of regulation of synaptic plasticity by Zn 2+ through modulation of\nneurotransmitter release.\n", "doi": "10.1002/anie.201913184", "arxiv_id": "2007.03243", "pdf_urls": ["https://arxiv.org/pdf/2007.03243"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Wiley-VCH Verlag, 2020,\n 59 (8), pp.3083-3087", "categories": "q-bio.NC q-bio.SC"} |
| {"title": "Intracellular Electrochemical Nanomeasurements Reveal that Exocytosis of\n Molecules at Living Neurons is Subquantal and Complex", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Anna Larsson", "Soodabeh Majdi", "Alexander Oleinick (PASTEUR)", "Irina Svir\n (PASTEUR)", "Johan Dunevall", "Christian Amatore (PASTEUR)", "Andrew Ewing"], "abstract": " Since the early work of Bernard Katz, the process of cellular chemical\ncommunication via exocytosis, quantal release, has been considered to be all or\nnone. Recent evidence has shown exocytosis to be partial or 'subquantal' at\nsingle-cell model systems, but there is a need to understand this at\ncommunicating nerve cells. Partial release allows nerve cells to control the\nsignal at the site of release during individual events, where the smaller the\nfraction released, the greater the range of regulation. Here we show that the\nfraction of the vesicular octopamine content released from a living Drosophila\nlarval neuromuscular neuron is very small. The percentage of released molecules\nwas found to be only 4.5% for simple events and 10.7% for complex (i.e.,\noscillating or flickering) events. This large content, combined with partial\nrelease controlled by fluctuations of the fusion pore, offers presynaptic\nplasticity that can be widely regulated. Two works published in 2010 suggested\nthat the Katz principle, [1] was incorrect for all-or-none release and that\nonly part of the chemical load of vesicles was released during exocytosis, at\nleast as measured as a full spike during amperometry. [2] The combination of\nelectrochemical methods to measure both release and vesicle content in 2015\nadded a wealth of information to support the concept of partial release in\nexocytosis. [3] Additionally, this has recently been supported by work with\nTIRF microscopy showing 'subquantal' release from vesicles in adrenal\nchromaffin cells and using super-resolution STED microscopy. [4] It appears\nthat the full event generally involves release of only part of the load of\nchemical messenger in single-cell model systems like adrenal chromaffin and\nPC12 cells. Is this also true at living neurons in a nervous system and to what\nextent? To answer this critical question, we quantified the number of\noctopamine molecules in the neuromuscular neurons of Drosophila larvae by\nadapting an amperometric technique developed in our\n", "doi": "10.1002/anie.201914564", "arxiv_id": "2007.03246", "pdf_urls": ["https://arxiv.org/pdf/2007.03246"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Wiley-VCH Verlag, 2020,\n 59 (17), pp.6711-6714", "categories": "q-bio.NC"} |
| {"title": "Atom-Tunneling in Chemistry", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jan Meisner", "Johannes K\\\"astner"], "abstract": " Quantum mechanical tunneling of atoms is increasingly found to play an\nimportant role in many chemical transformations. Experimentally, atom-tunneling\ncan be indirectly detected by temperature-independent rate constants at low\ntemperature or by enhanced kinetic isotope effects. On the contrary, using\ncomputational investigations the influence of tunneling on the reaction rates\ncan directly be monitored. The tunnel effect, for example, changes reaction\npaths and branching ratios, enables chemical reactions in an astrochemical\nenvironment that would be impossible by thermal transition, and influences\nbiochemical processes.\n", "doi": "10.1002/anie.201511028", "arxiv_id": "2009.04303", "pdf_urls": ["https://arxiv.org/pdf/2009.04303"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2016, 55, 5400", "categories": "physics.chem-ph astro-ph.GA"} |
| {"title": "Predicting Berborite as Potential Deep-Ultraviolet Nonlinear Optical\n Crystal from First Principles", "year": 2020, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Lei Kang", "Pifu Gong", "Zheshuai Lin", "Bing Huang"], "abstract": " Following our ab initio nonlinear optical (NLO) materials design guidelines,\nin this Letter, we discovered a novel type of structure to realize potential\ndeep-ultraviolet (DUV) NLO performance in the classical beryllium borate\nsystem. By densely stacking the NLO-active layered frameworks, the key design\nscheme for the structural evolution from the (Be2BO3F2) layers in KBe2BO3F2\n(KBBF) to the novel (Be2BO5H3) layers in berborite is illustrated. Based on\navailable experimental results and systematical theoretical evaluation from\nfirst principles, the NLO properties of berborite are further obtained as\ncomparable as the only pratical DUV NLO crystal KBBF. It is demonstrated that\nberborite can achieve available DUV phase-matched output with strong NLO effect\nfor the practically important 177.3 nm and 193.7 nm lasers. Once obtained with\nsizable single crystal, it can be applied as a promising DUV NLO crystal.\n", "doi": "10.1002/anie.202105789", "arxiv_id": "2012.07260", "pdf_urls": ["https://arxiv.org/pdf/2012.07260"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 2021", "categories": "cond-mat.mtrl-sci physics.optics"} |
| {"title": "Na9Bi5Os3O24: A Unique Diamagnetic Oxide Featuring a Pronouncedly\n Jahn-Teller Compressed Octahedral Coordination of Osmium(VI)", "year": 2021, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Gohil S. Thakur", "Hans Reuter", "Alexey V. Ushakov", "Gianpiero Gallo", "Jueurgen Nuss", "Robert E. Dinnebier", "Sergey V. Streltsov", "Daniel I. Khomskii", "and Martin Jansen"], "abstract": " The Jahn-Teller theorem constitutes one of the most popular and stringent\nconcepts, applicable to all fields of chemistry. In open shell transition\nelements chemistry and physics, 3d4, 3d9, and 3d7(low-spin) configurations in\noctahedral complexes serve as particular illustrative and firm examples, where\na striking change (distortion) in local geometry is associated to a substantial\nreduction of electronic energy. However, there has been a lasting debate, about\nthe fact that the octahedra are found to exclusively elongate, (at least for eg\nelectrons). Against this background, the title compound displays two marked\nfeatures, (1) the octahedron of oxygen atoms around Os6+ (d2) is drastically\ncompressed, in contrast to the standard JT expectations, and (2) the splitting\nof the t2g set induced by this compression is extreme, such that a diamagnetic\nground state results. What we see is obviously a Jahn-Teller distortion\nresulting in a compression of the respective octahedron and acting on the t2g\nset of orbitals. Both these issues are unprecedented. Noteworthy, the splitting\ninto a lower dxy (hosting two d electrons with opposite spin) and two higher\ndxz and dyz orbitals is so large that for the first time ever the Hund's\ncoupling for t2g electrons is overcome. We show that these effects are not\nforced by structural frustration, the structure offers sufficient space for Os\nto shift the apical oxygen atoms to a standard distance. Local electronic\neffects appear to be responsible, instead. The relevance of these findings is\nfar reaching, since they provide insights in the hierarchy of perturbations\ndefining ground states of open shell electronic systems. The system studied\nhere, offers substantially more structural and compositional degrees of\nfreedom, such that a configuration could form that enables Os6+ to adopt its\napparently genuine diamagnetic ground state.\n", "doi": "10.1002/anie.202103295", "arxiv_id": "2103.06065", "pdf_urls": ["https://arxiv.org/pdf/2103.06065"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 60 (2021) 16500-16505", "categories": "cond-mat.mtrl-sci"} |
| {"title": "On-surface synthesis and collective spin excitations of a\n triangulene-based nanostar", "year": 2021, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Jeremy Hieulle", "Silvia Castro", "Niklas Friedrich", "Alessio Vegliante", "Francisco Romero Lara", "Sof\\'ia Sanz", "Dulce Rey", "Martina Corso", "Thomas\n Frederiksen", "Jose Ignacio Pascual", "and Diego Pe\\~na"], "abstract": " Triangulene nanographenes are open-shell molecules with predicted high spin\nstate due to the frustration of their conjugated network. Their long-sought\nsynthesis became recently possible over a metal surface. Here, we present a\nmacrocycle formed by six [3]triangulenes, which was obtained by combining the\nsolution synthesis of a dimethylphenyl-anthracene cyclic hexamer and the\non-surface cyclodehydrogenation of this precursor over a gold substrate. The\nresulting triangulene nanostar exhibits a collective spin state generated by\nthe interaction of its 12 unpaired {\\pi}-electrons along the conjugated\nlattice, corresponding to the antiferromagnetic ordering of six S = 1 sites\n(one per triangulene unit). Inelastic electron tunneling spectroscopy resolved\nthree spin excitations connecting the singlet ground state with triplet states.\nThe nanostar behaves close to predictions from the Heisenberg model of a S = 1\nspin ring, representing a unique system to test collective spin modes in cyclic\nsystems.\n", "doi": "10.1002/anie.202108301", "arxiv_id": "2107.02198", "pdf_urls": ["https://arxiv.org/pdf/2107.02198"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angew. Chem. Int. Ed. 60, 25224-25229 (2021)", "categories": "cond-mat.mes-hall physics.chem-ph"} |
| {"title": "On-Surface Decarboxylation Coupling Facilitated by Lock-to-Unlock\n Variation of Molecules upon the Reaction", "year": 2021, "venue_abbr": "Angew. Chem. Int. Ed.", "venue_name": "Angewandte Chemie International Edition", "authors": ["Shaoshan Wang", "Zhuo Li", "Pengcheng Ding", "Cristina Mattioli", "Wujun\n Huang", "Yang Wang", "Andr\\'e Gourdon (CEMES-GNS)", "Ye Sun", "Mingshu Chen", "Lev\n Kantorovich", "Xueming Yang", "Federico Rosei", "Miao Yu"], "abstract": " On-surface synthesis (OSS) involving relatively high energy barriers remains\nchallenging due to a typical dilemma: firm molecular anchor is required to\nprevent molecular desorption upon the reaction, whereas sufficient lateral\nmobility is crucial for subsequent coupling and assembly. By locking the\nmolecular precursors on the substrate then unlocking them during the reaction,\nwe present a strategy to address this challenge. High-yield synthesis based on\nwell-defined decarboxylation, intermediate transition and hexamerization is\ndemonstrated, resulting in an extended and ordered network exclusively composed\nof the newly-synthesized macrocyclic compound. Thanks to the steric hindrance\nof its maleimide group, we attain a preferential selection of the coupling.\nThis work unlocks a promising path to enrich the reaction types and improve the\ncoupling selectivity hence the structual homogeneity of the final product for\nOSS.\n", "doi": null, "arxiv_id": "2109.06499", "pdf_urls": ["https://arxiv.org/pdf/2109.06499"], "github": [], "is_oa": true, "sources": ["open-arxiv"], "type": "journal", "journal_ref": "Angewandte Chemie International Edition, Wiley-VCH Verlag, 2021", "categories": "physics.chem-ph"} |
|
|
