Pub Date : 2024-06-04DOI: 10.1038/s41563-024-01924-x
Stacked atomic layers that interact via van der Waals forces offer a confined interlayer space for stabilizing unconventional materials or physical states, enabling a versatile platform for engineering structural configurations and properties at the atomic level.
{"title":"Exploring interlayer space","authors":"","doi":"10.1038/s41563-024-01924-x","DOIUrl":"10.1038/s41563-024-01924-x","url":null,"abstract":"Stacked atomic layers that interact via van der Waals forces offer a confined interlayer space for stabilizing unconventional materials or physical states, enabling a versatile platform for engineering structural configurations and properties at the atomic level.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":41.2,"publicationDate":"2024-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41563-024-01924-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141246567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-03DOI: 10.1038/s41563-024-01910-3
Zhizhan Qiu, Yixuan Han, Keian Noori, Zhaolong Chen, Mikhail Kashchenko, Li Lin, Thomas Olsen, Jing Li, Hanyan Fang, Pin Lyu, Mykola Telychko, Xingyu Gu, Shaffique Adam, Su Ying Quek, Aleksandr Rodin, A. H. Castro Neto, Kostya S. Novoselov, Jiong Lu
The coexistence of correlated electron and hole crystals enables the realization of quantum excitonic states, capable of hosting counterflow superfluidity and topological orders with long-range quantum entanglement. Here we report evidence for imbalanced electron–hole crystals in a doped Mott insulator, namely, α-RuCl3, through gate-tunable non-invasive van der Waals doping from graphene. Real-space imaging via scanning tunnelling microscopy reveals two distinct charge orderings at the lower and upper Hubbard band energies, whose origin is attributed to the correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru–Ru bonds, respectively. Moreover, a gate-induced transition of electron–hole crystals is directly visualized, further corroborating their nature as correlation-driven charge crystals. The realization and atom-resolved visualization of imbalanced electron–hole crystals in a doped Mott insulator opens new doors in the search for correlated bosonic states within strongly correlated materials. Scanning tunnelling microscopy of doped RuCl3 shows distinct charge orderings at the lower and upper Hubbard bands, which can be attributed to a correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and a rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru–Ru bonds.
{"title":"Evidence for electron–hole crystals in a Mott insulator","authors":"Zhizhan Qiu, Yixuan Han, Keian Noori, Zhaolong Chen, Mikhail Kashchenko, Li Lin, Thomas Olsen, Jing Li, Hanyan Fang, Pin Lyu, Mykola Telychko, Xingyu Gu, Shaffique Adam, Su Ying Quek, Aleksandr Rodin, A. H. Castro Neto, Kostya S. Novoselov, Jiong Lu","doi":"10.1038/s41563-024-01910-3","DOIUrl":"10.1038/s41563-024-01910-3","url":null,"abstract":"The coexistence of correlated electron and hole crystals enables the realization of quantum excitonic states, capable of hosting counterflow superfluidity and topological orders with long-range quantum entanglement. Here we report evidence for imbalanced electron–hole crystals in a doped Mott insulator, namely, α-RuCl3, through gate-tunable non-invasive van der Waals doping from graphene. Real-space imaging via scanning tunnelling microscopy reveals two distinct charge orderings at the lower and upper Hubbard band energies, whose origin is attributed to the correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru–Ru bonds, respectively. Moreover, a gate-induced transition of electron–hole crystals is directly visualized, further corroborating their nature as correlation-driven charge crystals. The realization and atom-resolved visualization of imbalanced electron–hole crystals in a doped Mott insulator opens new doors in the search for correlated bosonic states within strongly correlated materials. Scanning tunnelling microscopy of doped RuCl3 shows distinct charge orderings at the lower and upper Hubbard bands, which can be attributed to a correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and a rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru–Ru bonds.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141235970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-03DOI: 10.1038/s41563-024-01917-w
Shihao Zang, Adam W. Hauser, Sanjib Paul, Glen M. Hocky, Stefano Sacanna
Structures of molecular crystals are identified using scattering techniques because we cannot see inside them. Micrometre-sized colloidal particles enable the real-time observation of crystallization with optical microscopy, but in practice this is still hampered by a lack of ‘X-ray vision’. Here we introduce a system of index-matched fluorescently labelled colloidal particles and demonstrate the robust formation of ionic crystals in aqueous solution, with structures that can be controlled by size ratio and salt concentration. Full three-dimensional coordinates of particles are distinguished through in situ confocal microscopy, and the crystal structures are identified via comparison of their simulated scattering pattern with known atomic arrangements. Finally, we leverage our ability to look inside colloidal crystals to observe the motion of defects and crystal melting in time and space and to reveal the origin of crystal twinning. Using this platform, the path to real-time analysis of ionic colloidal crystallization is now ‘crystal clear’. Index-matched fluorescent particles provide a system that directly visualizes ionic crystallization using confocal microscopy, and offers insight into the structure, nucleation and growth of ionic solids.
{"title":"Enabling three-dimensional real-space analysis of ionic colloidal crystallization","authors":"Shihao Zang, Adam W. Hauser, Sanjib Paul, Glen M. Hocky, Stefano Sacanna","doi":"10.1038/s41563-024-01917-w","DOIUrl":"10.1038/s41563-024-01917-w","url":null,"abstract":"Structures of molecular crystals are identified using scattering techniques because we cannot see inside them. Micrometre-sized colloidal particles enable the real-time observation of crystallization with optical microscopy, but in practice this is still hampered by a lack of ‘X-ray vision’. Here we introduce a system of index-matched fluorescently labelled colloidal particles and demonstrate the robust formation of ionic crystals in aqueous solution, with structures that can be controlled by size ratio and salt concentration. Full three-dimensional coordinates of particles are distinguished through in situ confocal microscopy, and the crystal structures are identified via comparison of their simulated scattering pattern with known atomic arrangements. Finally, we leverage our ability to look inside colloidal crystals to observe the motion of defects and crystal melting in time and space and to reveal the origin of crystal twinning. Using this platform, the path to real-time analysis of ionic colloidal crystallization is now ‘crystal clear’. Index-matched fluorescent particles provide a system that directly visualizes ionic crystallization using confocal microscopy, and offers insight into the structure, nucleation and growth of ionic solids.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141236023","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-23DOI: 10.1038/s41563-024-01897-x
Eric Grelet, Maxime M. C. Tortora
Chirality is ubiquitous in nature across all length scales, with major implications spanning fields from biology, chemistry and physics to materials science. How chirality propagates from nanoscale building blocks to meso- and macroscopic helical structures remains an open issue. Here, working with a canonical system of filamentous viruses, we demonstrate that their self-assembly into chiral liquid crystal phases quantitatively results from the interplay between two main mechanisms of chirality transfer: electrostatic interactions from the helical charge patterns on the virus surface, and fluctuation-based helical deformations leading to viral backbone helicity. Our experimental and theoretical approach provides a comprehensive framework for deciphering how chirality is hierarchically and quantitatively propagated across spatial scales. Our work highlights the ways in which supramolecular helicity may arise from subtle chiral contributions of opposite handedness that act either cooperatively or competitively, thus accounting for the multiplicity of chiral behaviours observed for nearly identical molecular systems. The authors investigate the origins of chirality transfer across length scales, quantitatively demonstrating how chirality propagates from the molecular to liquid crystal level in filamentous virus systems.
{"title":"Elucidating chirality transfer in liquid crystals of viruses","authors":"Eric Grelet, Maxime M. C. Tortora","doi":"10.1038/s41563-024-01897-x","DOIUrl":"10.1038/s41563-024-01897-x","url":null,"abstract":"Chirality is ubiquitous in nature across all length scales, with major implications spanning fields from biology, chemistry and physics to materials science. How chirality propagates from nanoscale building blocks to meso- and macroscopic helical structures remains an open issue. Here, working with a canonical system of filamentous viruses, we demonstrate that their self-assembly into chiral liquid crystal phases quantitatively results from the interplay between two main mechanisms of chirality transfer: electrostatic interactions from the helical charge patterns on the virus surface, and fluctuation-based helical deformations leading to viral backbone helicity. Our experimental and theoretical approach provides a comprehensive framework for deciphering how chirality is hierarchically and quantitatively propagated across spatial scales. Our work highlights the ways in which supramolecular helicity may arise from subtle chiral contributions of opposite handedness that act either cooperatively or competitively, thus accounting for the multiplicity of chiral behaviours observed for nearly identical molecular systems. The authors investigate the origins of chirality transfer across length scales, quantitatively demonstrating how chirality propagates from the molecular to liquid crystal level in filamentous virus systems.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141085616","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-23DOI: 10.1038/s41563-024-01907-y
Hao Pan, Menglin Zhu, Ella Banyas, Louis Alaerts, Megha Acharya, Hongrui Zhang, Jiyeob Kim, Xianzhe Chen, Xiaoxi Huang, Michael Xu, Isaac Harris, Zishen Tian, Francesco Ricci, Brendan Hanrahan, Jonathan E. Spanier, Geoffroy Hautier, James M. LeBeau, Jeffrey B. Neaton, Lane W. Martin
Thin-film materials with large electromechanical responses are fundamental enablers of next-generation micro-/nano-electromechanical applications. Conventional electromechanical materials (for example, ferroelectrics and relaxors), however, exhibit severely degraded responses when scaled down to submicrometre-thick films due to substrate constraints (clamping). This limitation is overcome, and substantial electromechanical responses in antiferroelectric thin films are achieved through an unconventional coupling of the field-induced antiferroelectric-to-ferroelectric phase transition and the substrate constraints. A detilting of the oxygen octahedra and lattice-volume expansion in all dimensions are observed commensurate with the phase transition using operando electron microscopy, such that the in-plane clamping further enhances the out-of-plane expansion, as rationalized using first-principles calculations. In turn, a non-traditional thickness scaling is realized wherein an electromechanical strain (1.7%) is produced from a model antiferroelectric PbZrO3 film that is just 100 nm thick. The high performance and understanding of the mechanism provide a promising pathway to develop high-performance micro-/nano-electromechanical systems. Here, the authors observe that in thin films of antiferroelectric PbZrO3, substrate clamping enhances the electromechanical response, with expansion purely in the out-of-plane direction, achieving 1.7% strain for 100-nm-thick films.
{"title":"Clamping enables enhanced electromechanical responses in antiferroelectric thin films","authors":"Hao Pan, Menglin Zhu, Ella Banyas, Louis Alaerts, Megha Acharya, Hongrui Zhang, Jiyeob Kim, Xianzhe Chen, Xiaoxi Huang, Michael Xu, Isaac Harris, Zishen Tian, Francesco Ricci, Brendan Hanrahan, Jonathan E. Spanier, Geoffroy Hautier, James M. LeBeau, Jeffrey B. Neaton, Lane W. Martin","doi":"10.1038/s41563-024-01907-y","DOIUrl":"10.1038/s41563-024-01907-y","url":null,"abstract":"Thin-film materials with large electromechanical responses are fundamental enablers of next-generation micro-/nano-electromechanical applications. Conventional electromechanical materials (for example, ferroelectrics and relaxors), however, exhibit severely degraded responses when scaled down to submicrometre-thick films due to substrate constraints (clamping). This limitation is overcome, and substantial electromechanical responses in antiferroelectric thin films are achieved through an unconventional coupling of the field-induced antiferroelectric-to-ferroelectric phase transition and the substrate constraints. A detilting of the oxygen octahedra and lattice-volume expansion in all dimensions are observed commensurate with the phase transition using operando electron microscopy, such that the in-plane clamping further enhances the out-of-plane expansion, as rationalized using first-principles calculations. In turn, a non-traditional thickness scaling is realized wherein an electromechanical strain (1.7%) is produced from a model antiferroelectric PbZrO3 film that is just 100 nm thick. The high performance and understanding of the mechanism provide a promising pathway to develop high-performance micro-/nano-electromechanical systems. Here, the authors observe that in thin films of antiferroelectric PbZrO3, substrate clamping enhances the electromechanical response, with expansion purely in the out-of-plane direction, achieving 1.7% strain for 100-nm-thick films.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141085614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-22DOI: 10.1038/s41563-024-01904-1
Tianxiang Dai, Anqi Ma, Jun Mao, Yutian Ao, Xinyu Jia, Yun Zheng, Chonghao Zhai, Yan Yang, Zhihua Li, Bo Tang, Jun Luo, Baile Zhang, Xiaoyong Hu, Qihuang Gong, Jianwei Wang
Controlling topological phases of light allows the observation of abundant topological phenomena and the development of robust photonic devices. The prospect of more sophisticated control with topological photonic devices for practical implementations requires high-level programmability. Here we demonstrate a fully programmable topological photonic chip with large-scale integration of silicon photonic nanocircuits and microresonators. Photonic artificial atoms and their interactions in our compound system can be individually addressed and controlled, allowing the arbitrary adjustment of structural parameters and geometrical configurations for the observation of dynamic topological phase transitions and diverse photonic topological insulators. Individual programming of artificial atoms on the generic chip enables the comprehensive statistical characterization of topological robustness against relatively weak disorders, and counterintuitive topological Anderson phase transitions induced by strong disorders. This generic topological photonic chip can be rapidly reprogrammed to implement multifunctionalities, providing a flexible and versatile platform for applications across fundamental science and topological technologies. The authors demonstrate a programmable topological photonic chip with large-scale integration of silicon photonic nanocircuits and microresonators that can be rapidly reprogrammed to implement diverse multifunctionalities.
{"title":"A programmable topological photonic chip","authors":"Tianxiang Dai, Anqi Ma, Jun Mao, Yutian Ao, Xinyu Jia, Yun Zheng, Chonghao Zhai, Yan Yang, Zhihua Li, Bo Tang, Jun Luo, Baile Zhang, Xiaoyong Hu, Qihuang Gong, Jianwei Wang","doi":"10.1038/s41563-024-01904-1","DOIUrl":"10.1038/s41563-024-01904-1","url":null,"abstract":"Controlling topological phases of light allows the observation of abundant topological phenomena and the development of robust photonic devices. The prospect of more sophisticated control with topological photonic devices for practical implementations requires high-level programmability. Here we demonstrate a fully programmable topological photonic chip with large-scale integration of silicon photonic nanocircuits and microresonators. Photonic artificial atoms and their interactions in our compound system can be individually addressed and controlled, allowing the arbitrary adjustment of structural parameters and geometrical configurations for the observation of dynamic topological phase transitions and diverse photonic topological insulators. Individual programming of artificial atoms on the generic chip enables the comprehensive statistical characterization of topological robustness against relatively weak disorders, and counterintuitive topological Anderson phase transitions induced by strong disorders. This generic topological photonic chip can be rapidly reprogrammed to implement multifunctionalities, providing a flexible and versatile platform for applications across fundamental science and topological technologies. The authors demonstrate a programmable topological photonic chip with large-scale integration of silicon photonic nanocircuits and microresonators that can be rapidly reprogrammed to implement diverse multifunctionalities.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41563-024-01904-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141079118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Elucidating the mechanism of photoinduced water splitting on TiO2 is important for advancing the understanding of photocatalysis and the ability to control photocatalytic surface reactions. However, incomplete experimental information and complex coupled electron–nuclear motion make the microscopic understanding challenging. Here we analyse the atomic-scale pathways of photogenerated charge carrier transport and photoinduced water dissociation at the prototypical water–rutile TiO2(110) interface using first-principles dynamics simulations. Two distinct mechanisms are observed. Field-initiated electron migration leads to adsorbed water dissociation via proton transfer to a surface bridging oxygen. In the other pathway, adsorbed water dissociation occurs via proton donation to a second-layer water molecule coupled to photoexcited-hole transfer promoted by in-plane surface lattice distortions. Two stages of non-adiabatic in-plane lattice motion—expansion and recovery—are observed, which are closely associated with population changes in Ti3d orbitals. Controlling such highly correlated electron–nuclear dynamics may provide opportunities for boosting the performance of photocatalytic materials. Understanding the origin of photoinduced water splitting on TiO2 is crucial to control photocatalytic surface reactions. A photoexcited-hole-transfer-driven mechanism now shows that water dissociation is strongly coupled with dynamic lattice distortion (photoexcited phonons) on TiO2 surfaces.
{"title":"Correlated electron–nuclear dynamics of photoinduced water dissociation on rutile TiO2","authors":"Peiwei You, Daqiang Chen, Xinbao Liu, Cui Zhang, Annabella Selloni, Sheng Meng","doi":"10.1038/s41563-024-01900-5","DOIUrl":"10.1038/s41563-024-01900-5","url":null,"abstract":"Elucidating the mechanism of photoinduced water splitting on TiO2 is important for advancing the understanding of photocatalysis and the ability to control photocatalytic surface reactions. However, incomplete experimental information and complex coupled electron–nuclear motion make the microscopic understanding challenging. Here we analyse the atomic-scale pathways of photogenerated charge carrier transport and photoinduced water dissociation at the prototypical water–rutile TiO2(110) interface using first-principles dynamics simulations. Two distinct mechanisms are observed. Field-initiated electron migration leads to adsorbed water dissociation via proton transfer to a surface bridging oxygen. In the other pathway, adsorbed water dissociation occurs via proton donation to a second-layer water molecule coupled to photoexcited-hole transfer promoted by in-plane surface lattice distortions. Two stages of non-adiabatic in-plane lattice motion—expansion and recovery—are observed, which are closely associated with population changes in Ti3d orbitals. Controlling such highly correlated electron–nuclear dynamics may provide opportunities for boosting the performance of photocatalytic materials. Understanding the origin of photoinduced water splitting on TiO2 is crucial to control photocatalytic surface reactions. A photoexcited-hole-transfer-driven mechanism now shows that water dissociation is strongly coupled with dynamic lattice distortion (photoexcited phonons) on TiO2 surfaces.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141079063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-20DOI: 10.1038/s41563-024-01887-z
Hannah L. Stern, Carmem M. Gilardoni, Qiushi Gu, Simone Eizagirre Barker, Oliver F. J. Powell, Xiaoxi Deng, Stephanie A. Fraser, Louis Follet, Chi Li, Andrew J. Ramsay, Hark Hoe Tan, Igor Aharonovich, Mete Atatüre
Solid-state spin–photon interfaces that combine single-photon generation and long-lived spin coherence with scalable device integration—ideally under ambient conditions—hold great promise for the implementation of quantum networks and sensors. Despite rapid progress reported across several candidate systems, those possessing quantum coherent single spins at room temperature remain extremely rare. Here we report quantum coherent control under ambient conditions of a single-photon-emitting defect spin in a layered van der Waals material, namely, hexagonal boron nitride. We identify that the carbon-related defect has a spin-triplet electronic ground-state manifold. We demonstrate that the spin coherence is predominantly governed by coupling to only a few proximal nuclei and is prolonged by decoupling protocols. Our results serve to introduce a new platform to realize a room-temperature spin qubit coupled to a multiqubit quantum register or quantum sensor with nanoscale sample proximity.
{"title":"A quantum coherent spin in hexagonal boron nitride at ambient conditions","authors":"Hannah L. Stern, Carmem M. Gilardoni, Qiushi Gu, Simone Eizagirre Barker, Oliver F. J. Powell, Xiaoxi Deng, Stephanie A. Fraser, Louis Follet, Chi Li, Andrew J. Ramsay, Hark Hoe Tan, Igor Aharonovich, Mete Atatüre","doi":"10.1038/s41563-024-01887-z","DOIUrl":"https://doi.org/10.1038/s41563-024-01887-z","url":null,"abstract":"<p>Solid-state spin–photon interfaces that combine single-photon generation and long-lived spin coherence with scalable device integration—ideally under ambient conditions—hold great promise for the implementation of quantum networks and sensors. Despite rapid progress reported across several candidate systems, those possessing quantum coherent single spins at room temperature remain extremely rare. Here we report quantum coherent control under ambient conditions of a single-photon-emitting defect spin in a layered van der Waals material, namely, hexagonal boron nitride. We identify that the carbon-related defect has a spin-triplet electronic ground-state manifold. We demonstrate that the spin coherence is predominantly governed by coupling to only a few proximal nuclei and is prolonged by decoupling protocols. Our results serve to introduce a new platform to realize a room-temperature spin qubit coupled to a multiqubit quantum register or quantum sensor with nanoscale sample proximity.</p>","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":41.2,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141069319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-20DOI: 10.1038/s41563-024-01901-4
Jiashun Liang, Yangyang Wan, Houfu Lv, Xuan Liu, Fan Lv, Shenzhou Li, Jia Xu, Zhi Deng, Junyi Liu, Siyang Zhang, Yingjun Sun, Mingchuan Luo, Gang Lu, Jiantao Han, Guoxiong Wang, Yunhui Huang, Shaojun Guo, Qing Li
Structurally ordered L10-PtM (M = Fe, Co, Ni and so on) intermetallic nanocrystals, benefiting from the chemically ordered structure and higher stability, are one of the best electrocatalysts used for fuel cells. However, their practical development is greatly plagued by the challenge that the high-temperature (>600 °C) annealing treatment necessary for realizing the ordered structure usually leads to severe particle sintering, morphology change and low ordering degree, which makes it very difficult for the gram-scale preparation of desirable PtM intermetallic nanocrystals with high Pt content for practical fuel cell applications. Here we report a new concept involving the low-melting-point-metal (M′ = Sn, Ga, In)-induced bond strength weakening strategy to reduce Ea and promote the ordering process of PtM (M = Ni, Co, Fe, Cu and Zn) alloy catalysts for a higher ordering degree. We demonstrate that the introduction of M′ can reduce the ordering temperature to extremely low temperatures (≤450 °C) and thus enable the preparation of high-Pt-content (≥40 wt%) L10-Pt-M-M′ intermetallic nanocrystals as well as ten-gram-scale production. X-ray spectroscopy studies, in situ electron microscopy and theoretical calculations reveal the fundamental mechanism of the Sn-facilitated ordering process at low temperatures, which involves weakened bond strength and consequently reduced Ea via Sn doping, the formation and fast diffusion of low-coordinated surface free atoms, and subsequent L10 nucleation. The developed L10-Ga-PtNi/C catalysts display outstanding performance in H2–air fuel cells under both light- and heavy-duty vehicle conditions. Under the latter condition, the 40% L10-Pt50Ni35Ga15/C catalyst delivers a high current density of 1.67 A cm−2 at 0.7 V and retains 80% of the current density after extended 90,000 cycles, which exceeds the United States Department of Energy performance metrics and represents among the best cathodic electrocatalysts for practical proton-exchange membrane fuel cells. Although structurally ordered intermetallic nanocrystals are promising electrocatalysts for fuel cells, their high-temperature large-scale preparation has proved challenging. A low-melting-point-metal-induced bond strength weakening strategy to promote alloy catalyst ordering is now proposed.
{"title":"Metal bond strength regulation enables large-scale synthesis of intermetallic nanocrystals for practical fuel cells","authors":"Jiashun Liang, Yangyang Wan, Houfu Lv, Xuan Liu, Fan Lv, Shenzhou Li, Jia Xu, Zhi Deng, Junyi Liu, Siyang Zhang, Yingjun Sun, Mingchuan Luo, Gang Lu, Jiantao Han, Guoxiong Wang, Yunhui Huang, Shaojun Guo, Qing Li","doi":"10.1038/s41563-024-01901-4","DOIUrl":"10.1038/s41563-024-01901-4","url":null,"abstract":"Structurally ordered L10-PtM (M = Fe, Co, Ni and so on) intermetallic nanocrystals, benefiting from the chemically ordered structure and higher stability, are one of the best electrocatalysts used for fuel cells. However, their practical development is greatly plagued by the challenge that the high-temperature (>600 °C) annealing treatment necessary for realizing the ordered structure usually leads to severe particle sintering, morphology change and low ordering degree, which makes it very difficult for the gram-scale preparation of desirable PtM intermetallic nanocrystals with high Pt content for practical fuel cell applications. Here we report a new concept involving the low-melting-point-metal (M′ = Sn, Ga, In)-induced bond strength weakening strategy to reduce Ea and promote the ordering process of PtM (M = Ni, Co, Fe, Cu and Zn) alloy catalysts for a higher ordering degree. We demonstrate that the introduction of M′ can reduce the ordering temperature to extremely low temperatures (≤450 °C) and thus enable the preparation of high-Pt-content (≥40 wt%) L10-Pt-M-M′ intermetallic nanocrystals as well as ten-gram-scale production. X-ray spectroscopy studies, in situ electron microscopy and theoretical calculations reveal the fundamental mechanism of the Sn-facilitated ordering process at low temperatures, which involves weakened bond strength and consequently reduced Ea via Sn doping, the formation and fast diffusion of low-coordinated surface free atoms, and subsequent L10 nucleation. The developed L10-Ga-PtNi/C catalysts display outstanding performance in H2–air fuel cells under both light- and heavy-duty vehicle conditions. Under the latter condition, the 40% L10-Pt50Ni35Ga15/C catalyst delivers a high current density of 1.67 A cm−2 at 0.7 V and retains 80% of the current density after extended 90,000 cycles, which exceeds the United States Department of Energy performance metrics and represents among the best cathodic electrocatalysts for practical proton-exchange membrane fuel cells. Although structurally ordered intermetallic nanocrystals are promising electrocatalysts for fuel cells, their high-temperature large-scale preparation has proved challenging. A low-melting-point-metal-induced bond strength weakening strategy to promote alloy catalyst ordering is now proposed.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141069345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-17DOI: 10.1038/s41563-024-01903-2
Klas Tybrandt
Integrating electrochemically actuated soft robotics with ultra-flexible microelectrodes enables reversible and gentle wrapping around nerves for high-quality recordings.
将电化学致动软机器人技术与超柔性微电极相结合，可对神经进行可逆的轻柔包裹，从而实现高质量的记录。
{"title":"A gentle nerve wrapper","authors":"Klas Tybrandt","doi":"10.1038/s41563-024-01903-2","DOIUrl":"10.1038/s41563-024-01903-2","url":null,"abstract":"Integrating electrochemically actuated soft robotics with ultra-flexible microelectrodes enables reversible and gentle wrapping around nerves for high-quality recordings.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":null,"pages":null},"PeriodicalIF":37.2,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140953575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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