Pub Date : 2024-08-27DOI: 10.1038/s41557-024-01617-7
Yaolong Xing, Inhwan Kim, Kyeong Tae Kang, Jinho Byun, Woo Seok Choi, Jaekwang Lee, Sang Ho Oh
Infinite-layer transition metal oxides with two-dimensional oxygen coordination exhibit intriguing electronic and magnetic properties due to strong in-plane orbital hybridization. The synthesis of this distinctive structure has primarily relied on kinetically controlled reduction of oxygen-rich phases featuring three-dimensional polyhedral oxygen coordination. Here, using in situ atomic-resolution electron microscopy, we scrutinize the intricate atomic-scale mechanisms of oxygen conduction leading to the transformation of SrFeO2.5 to infinite-layer SrFeO2. The oxygen release is highly anisotropic and governed by the lattice reorientation aligning the fast diffusion channels towards the outlet, which is facilitated by cooperative yet shuffle displacements of iron and oxygen ions. Accompanied with the oxygen release, the three-dimensional to two-dimensional reconfiguration of oxygen is facilitated by the lattice flexibility of FeOx polyhedral layers, adopting multiple discrete transient states following the sequence determined by the least energy-costing pathways. Similar transformation mechanism may operate in cuprate and nickelate superconductors, which are isostructural with SrFeO2.
{"title":"Monitoring the formation of infinite-layer transition metal oxides through in situ atomic-resolution electron microscopy.","authors":"Yaolong Xing, Inhwan Kim, Kyeong Tae Kang, Jinho Byun, Woo Seok Choi, Jaekwang Lee, Sang Ho Oh","doi":"10.1038/s41557-024-01617-7","DOIUrl":"https://doi.org/10.1038/s41557-024-01617-7","url":null,"abstract":"<p><p>Infinite-layer transition metal oxides with two-dimensional oxygen coordination exhibit intriguing electronic and magnetic properties due to strong in-plane orbital hybridization. The synthesis of this distinctive structure has primarily relied on kinetically controlled reduction of oxygen-rich phases featuring three-dimensional polyhedral oxygen coordination. Here, using in situ atomic-resolution electron microscopy, we scrutinize the intricate atomic-scale mechanisms of oxygen conduction leading to the transformation of SrFeO<sub>2.5</sub> to infinite-layer SrFeO<sub>2</sub>. The oxygen release is highly anisotropic and governed by the lattice reorientation aligning the fast diffusion channels towards the outlet, which is facilitated by cooperative yet shuffle displacements of iron and oxygen ions. Accompanied with the oxygen release, the three-dimensional to two-dimensional reconfiguration of oxygen is facilitated by the lattice flexibility of FeO<sub>x</sub> polyhedral layers, adopting multiple discrete transient states following the sequence determined by the least energy-costing pathways. Similar transformation mechanism may operate in cuprate and nickelate superconductors, which are isostructural with SrFeO<sub>2</sub>.</p>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142080974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-27DOI: 10.1038/s41557-024-01623-9
Shira Joudan
Going to conferences to share and learn about the latest science is a key part of being a researcher. Shira Joudan reflects on presenting their group’s research for the first time and guiding students through their first conference experiences.
{"title":"A new research group’s first conferences","authors":"Shira Joudan","doi":"10.1038/s41557-024-01623-9","DOIUrl":"10.1038/s41557-024-01623-9","url":null,"abstract":"Going to conferences to share and learn about the latest science is a key part of being a researcher. Shira Joudan reflects on presenting their group’s research for the first time and guiding students through their first conference experiences.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1385-1386"},"PeriodicalIF":19.2,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142080973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-26DOI: 10.1038/s41557-024-01619-5
Xiaolin Liu, Hao Yang, Hassan Harb, Rajarshi Samajdar, Toby J. Woods, Oliver Lin, Qian Chen, Adolfo I. B. Romo, Joaquín Rodríguez-López, Rajeev S. Assary, Jeffrey S. Moore, Charles M. Schroeder
Molecular electronic devices require precise control over the flow of current in single molecules. However, the electron transport properties of single molecules critically depend on dynamic molecular conformations in nanoscale junctions. Here we report a unique strategy for controlling molecular conductance using shape-persistent molecules. Chemically diverse, charged ladder molecules, synthesized via a one-pot multicomponent ladderization strategy, show a molecular conductance (d[log(G/G0)]/dx ≈ −0.1 nm−1) that is nearly independent of junction displacement, in stark contrast to the nanogap-dependent conductance (d[log(G/G0)]/dx ≈ −7 nm−1) observed for non-ladder analogues. Ladder molecules show an unusually narrow distribution of molecular conductance during dynamic junction displacement, which is attributed to the shape-persistent backbone and restricted rotation of terminal anchor groups. These principles are further extended to a butterfly-like molecule, thereby demonstrating the strategy’s generality for achieving gap-independent conductance. Overall, our work provides important avenues for controlling molecular conductance using shape-persistent molecules. Achieving robust and controllable conductance in single-molecule junctions is challenging due to the dynamic nature of molecular conformations that fluctuate over operational timescales. A strategy using shape-persistent molecules has now been developed that demonstrates nearly junction-displacement-independent conductance, providing a stable solution for single-molecule electronic properties.
{"title":"Shape-persistent ladder molecules exhibit nanogap-independent conductance in single-molecule junctions","authors":"Xiaolin Liu, Hao Yang, Hassan Harb, Rajarshi Samajdar, Toby J. Woods, Oliver Lin, Qian Chen, Adolfo I. B. Romo, Joaquín Rodríguez-López, Rajeev S. Assary, Jeffrey S. Moore, Charles M. Schroeder","doi":"10.1038/s41557-024-01619-5","DOIUrl":"10.1038/s41557-024-01619-5","url":null,"abstract":"Molecular electronic devices require precise control over the flow of current in single molecules. However, the electron transport properties of single molecules critically depend on dynamic molecular conformations in nanoscale junctions. Here we report a unique strategy for controlling molecular conductance using shape-persistent molecules. Chemically diverse, charged ladder molecules, synthesized via a one-pot multicomponent ladderization strategy, show a molecular conductance (d[log(G/G0)]/dx ≈ −0.1 nm−1) that is nearly independent of junction displacement, in stark contrast to the nanogap-dependent conductance (d[log(G/G0)]/dx ≈ −7 nm−1) observed for non-ladder analogues. Ladder molecules show an unusually narrow distribution of molecular conductance during dynamic junction displacement, which is attributed to the shape-persistent backbone and restricted rotation of terminal anchor groups. These principles are further extended to a butterfly-like molecule, thereby demonstrating the strategy’s generality for achieving gap-independent conductance. Overall, our work provides important avenues for controlling molecular conductance using shape-persistent molecules. Achieving robust and controllable conductance in single-molecule junctions is challenging due to the dynamic nature of molecular conformations that fluctuate over operational timescales. A strategy using shape-persistent molecules has now been developed that demonstrates nearly junction-displacement-independent conductance, providing a stable solution for single-molecule electronic properties.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 11","pages":"1772-1780"},"PeriodicalIF":19.2,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142073295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-23DOI: 10.1038/s41557-024-01605-x
Jooha Park, Kyoungoh Kim, Kisuk Kang
Improving battery performance requires the careful design of electrolytes. Now, high-performing lithium battery electrolytes can be produced from non-solvating solvents by using a molecular-docking solvation strategy that takes advantage of intermolecular interactions between solvents to precisely control the solvation dynamics of lithium ions.
{"title":"Expanding the diversity of lithium electrolytes","authors":"Jooha Park, Kyoungoh Kim, Kisuk Kang","doi":"10.1038/s41557-024-01605-x","DOIUrl":"10.1038/s41557-024-01605-x","url":null,"abstract":"Improving battery performance requires the careful design of electrolytes. Now, high-performing lithium battery electrolytes can be produced from non-solvating solvents by using a molecular-docking solvation strategy that takes advantage of intermolecular interactions between solvents to precisely control the solvation dynamics of lithium ions.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1390-1391"},"PeriodicalIF":19.2,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142042660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-23DOI: 10.1038/s41557-024-01613-x
Andrew R. McCluskey, Miguel Rivera, Antonia S. J. S. Mey
The role of computers in the chemical sciences is changing. Previously the domain of the theoretical or computational chemist, advanced digital skills, including data analysis, automation and simulation, are becoming extremely relevant to all. Here, we discuss the importance of integrating digital skills into an undergraduate chemistry programme and highlight some work currently being carried out to achieve this.
{"title":"Digital skills in chemical education","authors":"Andrew R. McCluskey, Miguel Rivera, Antonia S. J. S. Mey","doi":"10.1038/s41557-024-01613-x","DOIUrl":"10.1038/s41557-024-01613-x","url":null,"abstract":"The role of computers in the chemical sciences is changing. Previously the domain of the theoretical or computational chemist, advanced digital skills, including data analysis, automation and simulation, are becoming extremely relevant to all. Here, we discuss the importance of integrating digital skills into an undergraduate chemistry programme and highlight some work currently being carried out to achieve this.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1383-1384"},"PeriodicalIF":19.2,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142042643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-21DOI: 10.1038/s41557-024-01611-z
Living anionic polymerization is generally carried out using a metal-based initiator under stringent, and ideally water-free, conditions. Now, proton transfer anionic polymerization is developed using an organic compound with an acidic C–H bond as the initiator in the presence of a base catalyst. This method offers easy access to well-defined polymers under moderate conditions.
{"title":"‘Living’ anionic polymerization through reversible activation of C–H bonds with a base catalyst","authors":"","doi":"10.1038/s41557-024-01611-z","DOIUrl":"10.1038/s41557-024-01611-z","url":null,"abstract":"Living anionic polymerization is generally carried out using a metal-based initiator under stringent, and ideally water-free, conditions. Now, proton transfer anionic polymerization is developed using an organic compound with an acidic C–H bond as the initiator in the presence of a base catalyst. This method offers easy access to well-defined polymers under moderate conditions.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 10","pages":"1582-1583"},"PeriodicalIF":19.2,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142013823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-21DOI: 10.1038/s41557-024-01595-w
Jinqiao Dong, Yan Liu, Yong Cui
Research into 2D materials has been growing with impressive speed since the discovery of graphene. Such layered materials with ultrathin morphologies and extreme aspect ratios currently display a vast range of properties; however, until recently a conspicuously missing property of 2D materials was global chirality. The situation has changed over the past few years with the implementation of several distinct types of ultrathin chiral 2D crystals. Here we offer a forward-looking perspective on this field to comprehend the fundamentals of global chirality in two dimensions and develop new directions. We specifically discuss the experimental achievements of the emerging chiral 2D materials with a focus on their design strategy, synthesis, structural characterization, fundamental physical properties and possible applications. We will highlight how the molecular-scale local chirality could be significantly transmitted and amplified throughout ultrathin single-crystalline 2D structures, resulting in distinctive global chirality that brings more sophisticated functions. Chirality in extended 2D structures exhibits fundamental differences from molecular-level chirality. This Perspective discusses how local molecular chirality is transmitted and amplified to form distinctive global chirality within ultrathin, single-crystalline 2D materials; it also explores the future challenges and potential of this field.
{"title":"Emerging chiral two-dimensional materials","authors":"Jinqiao Dong, Yan Liu, Yong Cui","doi":"10.1038/s41557-024-01595-w","DOIUrl":"10.1038/s41557-024-01595-w","url":null,"abstract":"Research into 2D materials has been growing with impressive speed since the discovery of graphene. Such layered materials with ultrathin morphologies and extreme aspect ratios currently display a vast range of properties; however, until recently a conspicuously missing property of 2D materials was global chirality. The situation has changed over the past few years with the implementation of several distinct types of ultrathin chiral 2D crystals. Here we offer a forward-looking perspective on this field to comprehend the fundamentals of global chirality in two dimensions and develop new directions. We specifically discuss the experimental achievements of the emerging chiral 2D materials with a focus on their design strategy, synthesis, structural characterization, fundamental physical properties and possible applications. We will highlight how the molecular-scale local chirality could be significantly transmitted and amplified throughout ultrathin single-crystalline 2D structures, resulting in distinctive global chirality that brings more sophisticated functions. Chirality in extended 2D structures exhibits fundamental differences from molecular-level chirality. This Perspective discusses how local molecular chirality is transmitted and amplified to form distinctive global chirality within ultrathin, single-crystalline 2D materials; it also explores the future challenges and potential of this field.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1398-1407"},"PeriodicalIF":19.2,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142013829","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-20DOI: 10.1038/s41557-024-01578-x
Jeroen Royakkers, Hanbo Yang, Alexander J. Gillett, Flurin Eisner, Pratyush Ghosh, Daniel G. Congrave, Mohammed Azzouzi, Zahra Andaji-Garmaroudi, Anastasia Leventis, Akshay Rao, Jarvist Moore Frost, Jenny Nelson, Hugo Bronstein
Control of the molecular configuration at the interface of an organic heterojunction is key to the development of efficient optoelectronic devices. Due to the difficulty in characterizing these buried and (probably) disordered heterointerfaces, the interfacial structure in most systems remains a mystery. Here we demonstrate a synthetic strategy to design and control model interfaces, enabling their detailed study in isolation from the bulk material. This is achieved by the synthesis of a polymer in which a non-fullerene acceptor moiety is covalently bonded to a donor polymer backbone using dual alkyl chain links, constraining the acceptor and donor units in a through space co-facial arrangement. The constrained geometry of the acceptor relative to the electron-rich and -poor moieties in the polymer backbone can be tuned to control the kinetics of charge separation and the energy of the resultant charge-transfer state giving insight into factors that govern charge generation at organic heterojunctions. The molecular interactions at an organic heterointerface govern the performance of many optoelectronic devices. Through a combination of synthesis, spectroscopy and modelling, it has now been shown that specific molecular interactions result in improved formation of the charge-transfer state.
{"title":"Synthesis of model heterojunction interfaces reveals molecular-configuration-dependent photoinduced charge transfer","authors":"Jeroen Royakkers, Hanbo Yang, Alexander J. Gillett, Flurin Eisner, Pratyush Ghosh, Daniel G. Congrave, Mohammed Azzouzi, Zahra Andaji-Garmaroudi, Anastasia Leventis, Akshay Rao, Jarvist Moore Frost, Jenny Nelson, Hugo Bronstein","doi":"10.1038/s41557-024-01578-x","DOIUrl":"10.1038/s41557-024-01578-x","url":null,"abstract":"Control of the molecular configuration at the interface of an organic heterojunction is key to the development of efficient optoelectronic devices. Due to the difficulty in characterizing these buried and (probably) disordered heterointerfaces, the interfacial structure in most systems remains a mystery. Here we demonstrate a synthetic strategy to design and control model interfaces, enabling their detailed study in isolation from the bulk material. This is achieved by the synthesis of a polymer in which a non-fullerene acceptor moiety is covalently bonded to a donor polymer backbone using dual alkyl chain links, constraining the acceptor and donor units in a through space co-facial arrangement. The constrained geometry of the acceptor relative to the electron-rich and -poor moieties in the polymer backbone can be tuned to control the kinetics of charge separation and the energy of the resultant charge-transfer state giving insight into factors that govern charge generation at organic heterojunctions. The molecular interactions at an organic heterointerface govern the performance of many optoelectronic devices. Through a combination of synthesis, spectroscopy and modelling, it has now been shown that specific molecular interactions result in improved formation of the charge-transfer state.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1453-1461"},"PeriodicalIF":19.2,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41557-024-01578-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007637","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-20DOI: 10.1038/s41557-024-01604-y
Ai Kohata, Kazushi Kinbara
The construction of synthetic cells holds great importance for exploring complex biological systems and could potentially provide insights into the origins of life. Now, synthetic gap junctional channels have been developed as a building block to construct synthetic cells that can mediate intercellular transport of ions and bioactive species.
{"title":"Generating synthetic gap junctions using supramolecular amphiphilic giant nanotubes","authors":"Ai Kohata, Kazushi Kinbara","doi":"10.1038/s41557-024-01604-y","DOIUrl":"10.1038/s41557-024-01604-y","url":null,"abstract":"The construction of synthetic cells holds great importance for exploring complex biological systems and could potentially provide insights into the origins of life. Now, synthetic gap junctional channels have been developed as a building block to construct synthetic cells that can mediate intercellular transport of ions and bioactive species.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1387-1389"},"PeriodicalIF":19.2,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007625","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-20DOI: 10.1038/s41557-024-01579-w
The synthesis of model heterojunction interfaces allows for the study of interfacial photoinduced charge-transfer states as a function of molecular structure. This analysis provides molecular-level insight into the factors governing charge generation at organic heterointerfaces and, thus, the efficiency of organic solar cells and other optoelectronic devices.
{"title":"Synthetic model interfaces for the study of intermolecular charge-transfer states","authors":"","doi":"10.1038/s41557-024-01579-w","DOIUrl":"10.1038/s41557-024-01579-w","url":null,"abstract":"The synthesis of model heterojunction interfaces allows for the study of interfacial photoinduced charge-transfer states as a function of molecular structure. This analysis provides molecular-level insight into the factors governing charge generation at organic heterointerfaces and, thus, the efficiency of organic solar cells and other optoelectronic devices.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 9","pages":"1396-1397"},"PeriodicalIF":19.2,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007624","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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