High-performance memristors have emerged as efficient hardware for integrating noisy image recognition and noise reduction. Herein, we report a fast-switching memristor featuring tens of nanoseconds switching time fabricated using a vacancy-ordered double perovskite, Cs2TiBr6 nanocrystals. The spatially ordered vacancies in the double perovskite facilitate the predictable formation and rupture of conductive filaments, which are explored through a comprehensive simulation using the finite element analysis physical model. These unique microscopic features suppress random conducting filament growth and enhance bromine vacancy diffusion, boosting memristor switching speed. A further study of synapse-like behaviors reveals that Cs2TiBr6-based memristors exhibit high robustness and reproducibility. We further developed the crossbar-array memristors as artificial neural networks for image denoising and classification, achieving a 10% increase in recognition accuracy for pre-denoised images over non-denoised samples. Our work highlights the potential of intrinsic vacancy-ordered memristive materials for advancing efficient, real-time, robust visual recognition.
{"title":"Vacancy-ordered double-perovskite-based memristors for image processing and pattern recognition","authors":"Wentong Li, Yanyun Ren, Tianwei Duan, Hao Tang, Hao Li, Kaihuan Zhang, Yu Sun, Xiaoyu Zhang, Weitao Zheng, Martyn A. McLachlan, Zhongrui Wang, Yuanyuan Zhou, Jiaqi Zhang","doi":"10.1016/j.matt.2024.10.006","DOIUrl":"https://doi.org/10.1016/j.matt.2024.10.006","url":null,"abstract":"High-performance memristors have emerged as efficient hardware for integrating noisy image recognition and noise reduction. Herein, we report a fast-switching memristor featuring tens of nanoseconds switching time fabricated using a vacancy-ordered double perovskite, Cs<sub>2</sub>TiBr<sub>6</sub> nanocrystals. The spatially ordered vacancies in the double perovskite facilitate the predictable formation and rupture of conductive filaments, which are explored through a comprehensive simulation using the finite element analysis physical model. These unique microscopic features suppress random conducting filament growth and enhance bromine vacancy diffusion, boosting memristor switching speed. A further study of synapse-like behaviors reveals that Cs<sub>2</sub>TiBr<sub>6</sub>-based memristors exhibit high robustness and reproducibility. We further developed the crossbar-array memristors as artificial neural networks for image denoising and classification, achieving a 10% increase in recognition accuracy for pre-denoised images over non-denoised samples. Our work highlights the potential of intrinsic vacancy-ordered memristive materials for advancing efficient, real-time, robust visual recognition.","PeriodicalId":388,"journal":{"name":"Matter","volume":"213 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142562154","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 : 2024-10-25DOI: 10.1016/j.matt.2024.09.014
Wenbing Wu, Alain Kadar, Sang Hyun Lee, Hong Ju Jung, Bum Chul Park, Jeffery E. Raymond, Thomas K. Tsotsis, Carlos E.S. Cesnik, Sharon C. Glotzer, Valerie Goss, Nicholas A. Kotov
Complex multifunctional coatings combining order and disorder are central for information, biomedical, transportation, and energy technologies. Their scalable fabrication is possible using nanostructured composites made by layer-by-layer assembly (LBL). Here, we show that structural descriptions encompassing their nonrandom disorder and related property-focused design are possible using graph theory (GT). Two-dimensional images of LBL films of silver and gold nanowires (NWs) were used to calculate GT representations. We found that random stick computational models often used to describe NW, nanofiber, and nanotube materials give inaccurate predictions of their structure. Concurrently, image-informed GT models accurately predict the structure and properties of the LBL films, including the unexpected nonlinearity of charge transport vs. LBL cycles. The conductivity anisotropy in LBL composites, not readily detectable with microscopy, was accurately predicted using GT models. Spray-assisted LBL offers the direct translation of GT predictions to additive, scalable coatings for drones and potentially other technologies.
{"title":"Layer-by-layer assembled nanowire networks enable graph-theoretical design of multifunctional coatings","authors":"Wenbing Wu, Alain Kadar, Sang Hyun Lee, Hong Ju Jung, Bum Chul Park, Jeffery E. Raymond, Thomas K. Tsotsis, Carlos E.S. Cesnik, Sharon C. Glotzer, Valerie Goss, Nicholas A. Kotov","doi":"10.1016/j.matt.2024.09.014","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.014","url":null,"abstract":"Complex multifunctional coatings combining order and disorder are central for information, biomedical, transportation, and energy technologies. Their scalable fabrication is possible using nanostructured composites made by layer-by-layer assembly (LBL). Here, we show that structural descriptions encompassing their nonrandom disorder and related property-focused design are possible using graph theory (GT). Two-dimensional images of LBL films of silver and gold nanowires (NWs) were used to calculate GT representations. We found that random stick computational models often used to describe NW, nanofiber, and nanotube materials give inaccurate predictions of their structure. Concurrently, image-informed GT models accurately predict the structure and properties of the LBL films, including the unexpected nonlinearity of charge transport vs. LBL cycles. The conductivity anisotropy in LBL composites, not readily detectable with microscopy, was accurately predicted using GT models. Spray-assisted LBL offers the direct translation of GT predictions to additive, scalable coatings for drones and potentially other technologies.","PeriodicalId":388,"journal":{"name":"Matter","volume":"2 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490187","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 : 2024-10-17DOI: 10.1016/j.matt.2024.09.022
Hao Huang, Haoyu Zhang, Ningjie Du, Yidan Lyu, Jiahang Xu, Haoran Fu, Yixin Guan, Kewang Nan
Despite the prolonged therapeutic benefits offered by many existing extended-release oral drug formulations, their inability to conform to circadian rhythms and specific pathological profiles remains a critical limitation. Here, we report drug origami, a computation-guided, origami-inspired approach for modulating the drug release kinetics of oral formulations. By harnessing the precise folding patterns of origami, the drug origami demonstrates characteristics of pulsatile and multiphasic release that can be tailored to match specific medication regimens. By employing computational models guided by control equations, both in vitro and in vivo drug release kinetics can be predicted and modulated with good quantitative agreement. This and other evidence suggest drug origami to be “do-it-yourself” drugs in personalized medicine where patients can create their own formulations according to individual medical needs.
{"title":"Drug origami: A computation-guided approach for customizable drug release kinetics of oral formulations","authors":"Hao Huang, Haoyu Zhang, Ningjie Du, Yidan Lyu, Jiahang Xu, Haoran Fu, Yixin Guan, Kewang Nan","doi":"10.1016/j.matt.2024.09.022","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.022","url":null,"abstract":"Despite the prolonged therapeutic benefits offered by many existing extended-release oral drug formulations, their inability to conform to circadian rhythms and specific pathological profiles remains a critical limitation. Here, we report drug origami, a computation-guided, origami-inspired approach for modulating the drug release kinetics of oral formulations. By harnessing the precise folding patterns of origami, the drug origami demonstrates characteristics of pulsatile and multiphasic release that can be tailored to match specific medication regimens. By employing computational models guided by control equations, both <em>in vitro</em> and <em>in vivo</em> drug release kinetics can be predicted and modulated with good quantitative agreement. This and other evidence suggest drug origami to be “do-it-yourself” drugs in personalized medicine where patients can create their own formulations according to individual medical needs.","PeriodicalId":388,"journal":{"name":"Matter","volume":"68 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444229","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}
Two-dimensional (2D) transition metal oxides (TMOs) have attracted much interest because of their unusual properties and high-temperature stability. However, due to isotropic bonding in all three dimensions and surface energy constraints, the direct synthesis of 2D TMOs with high crystal quality is challenging. Here, we develop a metal-lattice-heredity (MLH) strategy for synthesizing ultrathin TMO single crystals (e.g., Fe2O3) with tunable properties on SiO2/Si substrates. The MLH starts with chemical vapor deposition-grown 2D transition metal dichalcogenides (TMDs), followed by unique sequential sulfur-to-oxygen substitution reactions to obtain TMOs, where metal atoms retain their original lattice arrangement and symmetry. Such a process results in growing single-crystalline TMOs coinciding with the morphology and thickness of TMD templates, as supported by in situ optical studies and atomic-resolved imaging. The method can be used to grow many 2D TMOs, including Fe2O3, V2O5, Cr2O3, Co3O4, and NiO, with band gaps ranging from the near-infrared to the near-UV.
{"title":"Metal-lattice-heredity synthesis of single-crystalline 2D transition metal oxides","authors":"Junyang Tan, Jingwei Wang, Shengnan Li, Huiyu Nong, Shengfeng Zeng, Xiaolong Zou, Bilu Liu, Hui-Ming Cheng","doi":"10.1016/j.matt.2024.09.017","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.017","url":null,"abstract":"Two-dimensional (2D) transition metal oxides (TMOs) have attracted much interest because of their unusual properties and high-temperature stability. However, due to isotropic bonding in all three dimensions and surface energy constraints, the direct synthesis of 2D TMOs with high crystal quality is challenging. Here, we develop a metal-lattice-heredity (MLH) strategy for synthesizing ultrathin TMO single crystals (e.g., Fe<sub>2</sub>O<sub>3</sub>) with tunable properties on SiO<sub>2</sub>/Si substrates. The MLH starts with chemical vapor deposition-grown 2D transition metal dichalcogenides (TMDs), followed by unique sequential sulfur-to-oxygen substitution reactions to obtain TMOs, where metal atoms retain their original lattice arrangement and symmetry. Such a process results in growing single-crystalline TMOs coinciding with the morphology and thickness of TMD templates, as supported by <em>in situ</em> optical studies and atomic-resolved imaging. The method can be used to grow many 2D TMOs, including Fe<sub>2</sub>O<sub>3</sub>, V<sub>2</sub>O<sub>5</sub>, Cr<sub>2</sub>O<sub>3</sub>, Co<sub>3</sub>O<sub>4</sub>, and NiO, with band gaps ranging from the near-infrared to the near-UV.","PeriodicalId":388,"journal":{"name":"Matter","volume":"58 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439776","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 : 2024-10-16DOI: 10.1016/j.matt.2024.09.023
Ian H. Billinge, Gabriel D. Barbosa, Songsheng Tao, Maxwell W. Terban, C. Heath Turner, Simon J.L. Billinge, Ngai Yin Yip
In this study, we use state-of-the-art X-ray scattering and molecular dynamics to analyze amine-water mixtures that show the unusual lower critical solution temperature (LCST) behavior. The goal is to provide direct experimental evidence for the entropy-lowering molecular cluster formation hypothesized as necessary for LCST behavior. Differential wide-angle X-ray scattering and pair distribution analysis and small-angle X-ray scattering measurements were combined with molecular modeling and liquid-liquid equilibrium measurements, revealing direct experimental evidence for the hypothesis. However, the response of the amine phase to accommodating water is even more subtle than the simple hypothesis suggests, with the formation of robust nanoscale reverse micelles. The techniques developed in this paper can be expected to yield insights in the use of temperature-switchable liquids in solvent extraction and other separations, and the stabilization of organelles in living cells that do not have physical membranes but do require compositional gradients to operate.
在本研究中，我们使用了最先进的 X 射线散射和分子动力学方法来分析表现出不寻常的较低临界溶液温度 (LCST) 行为的胺水混合物。我们的目标是提供直接的实验证据，证明低临界溶液温度（LCST）行为所需的熵降低分子团簇形成的假设。差分广角 X 射线散射和配对分布分析以及小角 X 射线散射测量与分子建模和液液平衡测量相结合，揭示了假设的直接实验证据。然而，胺相在容纳水后的反应比简单假设所显示的更加微妙，形成了稳健的纳米级反向胶束。本文中开发的技术有望在溶剂萃取和其他分离过程中使用温度可切换液体，以及稳定活细胞中没有物理膜但需要成分梯度才能运行的细胞器方面产生深远影响。
{"title":"A structural underpinning of the lower critical solution temperature (LCST) behavior behind temperature-switchable liquids","authors":"Ian H. Billinge, Gabriel D. Barbosa, Songsheng Tao, Maxwell W. Terban, C. Heath Turner, Simon J.L. Billinge, Ngai Yin Yip","doi":"10.1016/j.matt.2024.09.023","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.023","url":null,"abstract":"In this study, we use state-of-the-art X-ray scattering and molecular dynamics to analyze amine-water mixtures that show the unusual lower critical solution temperature (LCST) behavior. The goal is to provide direct experimental evidence for the entropy-lowering molecular cluster formation hypothesized as necessary for LCST behavior. Differential wide-angle X-ray scattering and pair distribution analysis and small-angle X-ray scattering measurements were combined with molecular modeling and liquid-liquid equilibrium measurements, revealing direct experimental evidence for the hypothesis. However, the response of the amine phase to accommodating water is even more subtle than the simple hypothesis suggests, with the formation of robust nanoscale reverse micelles. The techniques developed in this paper can be expected to yield insights in the use of temperature-switchable liquids in solvent extraction and other separations, and the stabilization of organelles in living cells that do not have physical membranes but do require compositional gradients to operate.","PeriodicalId":388,"journal":{"name":"Matter","volume":"43 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439777","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 : 2024-10-16DOI: 10.1016/j.matt.2024.09.021
Qinqi Zhou, Peipei Shao, Renfu Zhang, Siyuan Huang, Yiwen Zhang, Ying Zhu, Menghan Yin, Gunnar A. Niklasson, Rui-Tao Wen
Ion trapping in electrodes upon long-term cycling is found to be one of the main reasons for performance degradation in electrochromic devices. Galvanostatic and potentiostatic post-treatments can rejuvenate degraded electrochromic layers. However, these procedures require high oxidation potentials, which are neither safe for the electrode-electrolyte system nor compatible with the operation of a full device. In the present paper, we report that degraded electrochromic oxides can be rejuvenated by a photo-electrochemical synergistically induced ion detrapping procedure. The UV light-induced photocurrent assists ion detrapping and limits the applied potential to the safe range used for electrochromic switching. This approach has been demonstrated to be effective for several cathodic electrochromic oxides and can be directly implemented in a full device. Our findings provide new vistas for efforts to expand the lifespan of electrochromic devices and other ion intercalation-based devices.
{"title":"Photo-electrochemical synergistically induced ion detrapping for electrochromic device rejuvenation","authors":"Qinqi Zhou, Peipei Shao, Renfu Zhang, Siyuan Huang, Yiwen Zhang, Ying Zhu, Menghan Yin, Gunnar A. Niklasson, Rui-Tao Wen","doi":"10.1016/j.matt.2024.09.021","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.021","url":null,"abstract":"Ion trapping in electrodes upon long-term cycling is found to be one of the main reasons for performance degradation in electrochromic devices. Galvanostatic and potentiostatic post-treatments can rejuvenate degraded electrochromic layers. However, these procedures require high oxidation potentials, which are neither safe for the electrode-electrolyte system nor compatible with the operation of a full device. In the present paper, we report that degraded electrochromic oxides can be rejuvenated by a photo-electrochemical synergistically induced ion detrapping procedure. The UV light-induced photocurrent assists ion detrapping and limits the applied potential to the safe range used for electrochromic switching. This approach has been demonstrated to be effective for several cathodic electrochromic oxides and can be directly implemented in a full device. Our findings provide new vistas for efforts to expand the lifespan of electrochromic devices and other ion intercalation-based devices.","PeriodicalId":388,"journal":{"name":"Matter","volume":"10 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439779","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}
Efforts to combine the advantages of multiple systems to enhance functionalities through solid-solution design present a great challenge due to the constraint imposed by the classical Vegard’s law. Here, we successfully navigate this trade-off by leveraging the synergistic effect of chemical doping and strain engineering in the solid-solution system of (1-x)BiFeO3-xBaTiO3. Unlike bulks, a significant deviation from Vegard’s law accompanied by enhanced multiferroism is observed in strained solid-solution epitaxial films, where we achieve a pronounced tetragonality (∼1.1), enhanced saturated magnetization (∼12 emu/cm3), substantial polarization (∼107 μC/cm2), and high ferroelectric Curie temperature (∼880°C), all while maintaining impressively low leakage current. These characteristics surpass the properties of their parent BiFeO3 and BaTiO3 films. Moreover, the superior ferroelectricity has never been reported in corresponding bulks (e.g., P ∼5 μC/cm2 and TC ∼300°C for bulk, with x = 0.5). These findings underscore the potential of strained (1-x)BiFeO3-xBaTiO3 films as lead-free, room temperature multiferroics.
{"title":"Large enhancement of properties in strained lead-free multiferroic solid solutions with strong deviation from Vegard’s law","authors":"Tao Wang, Min-Jie Zou, Dehe Zhang, Yu-Chieh Ku, Yawen Zheng, Shen Pan, Zhongqi Ren, Zedong Xu, Haoliang Huang, Wei Luo, Yunlong Tang, Lang Chen, Cheng-En Liu, Chun-Fu Chang, Sujit Das, Laurent Bellaiche, Yurong Yang, Xiu-Liang Ma, Chang-Yang Kuo, Xingjun Liu, Zuhuang Chen","doi":"10.1016/j.matt.2024.09.018","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.018","url":null,"abstract":"Efforts to combine the advantages of multiple systems to enhance functionalities through solid-solution design present a great challenge due to the constraint imposed by the classical Vegard’s law. Here, we successfully navigate this trade-off by leveraging the synergistic effect of chemical doping and strain engineering in the solid-solution system of (1-<em>x</em>)BiFeO<sub>3</sub>-<em>x</em>BaTiO<sub>3</sub>. Unlike bulks, a significant deviation from Vegard’s law accompanied by enhanced multiferroism is observed in strained solid-solution epitaxial films, where we achieve a pronounced tetragonality (∼1.1), enhanced saturated magnetization (∼12 emu/cm<sup>3</sup>), substantial polarization (∼107 μC/cm<sup>2</sup>), and high ferroelectric Curie temperature (∼880°C), all while maintaining impressively low leakage current. These characteristics surpass the properties of their parent BiFeO<sub>3</sub> and BaTiO<sub>3</sub> films. Moreover, the superior ferroelectricity has never been reported in corresponding bulks (e.g., <em>P</em> ∼5 μC/cm<sup>2</sup> and <em>T</em><sub>C</sub> ∼300°C for bulk, with <em>x</em> = 0.5). These findings underscore the potential of strained (1-<em>x</em>)BiFeO<sub>3</sub>-<em>x</em>BaTiO<sub>3</sub> films as lead-free, room temperature multiferroics.","PeriodicalId":388,"journal":{"name":"Matter","volume":"43 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436259","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 : 2024-10-15DOI: 10.1016/j.matt.2024.09.019
He Li, Feng Zhao, Maowen Liu, Dasheng Wei, Yan Gao, Chaoli Ma, Ruixiao Zheng, Bin Chen
Single crystals have grain boundary-free structure and possess superior properties; thus, they are in great demand in industry. Conventional melt-based single-crystal growth methods are dominated by strict and complicated processes, usually leading to small and expensive single crystals. Here, we report a solid-based approach, namely “texture-engineered grain growth,” for preparing bulk single crystals in a controllable and cost-efficient manner. Using copper as an example, we show that deformation texturing can effectively induce abnormal grain growth of cold-drawn copper bars during recrystallization, in which {111} grains grow preferably by coalescing neighboring small grains. Moreover, the applied temperature gradient enables the as-formed abnormally large grain to act as a seeding crystal to expand directionally throughout the entire textured copper bar, readily converting the textured polycrystals into a bulk single crystal. The technique is also applicable to the growth of bulk single-crystal nickel. The texture-induced monocrystallization strategy would advance large-scale manufacturing and applications of bulk single crystals.
{"title":"Fabrication of bulk single crystals via texture-engineered grain growth","authors":"He Li, Feng Zhao, Maowen Liu, Dasheng Wei, Yan Gao, Chaoli Ma, Ruixiao Zheng, Bin Chen","doi":"10.1016/j.matt.2024.09.019","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.019","url":null,"abstract":"Single crystals have grain boundary-free structure and possess superior properties; thus, they are in great demand in industry. Conventional melt-based single-crystal growth methods are dominated by strict and complicated processes, usually leading to small and expensive single crystals. Here, we report a solid-based approach, namely “texture-engineered grain growth,” for preparing bulk single crystals in a controllable and cost-efficient manner. Using copper as an example, we show that deformation texturing can effectively induce abnormal grain growth of cold-drawn copper bars during recrystallization, in which {111} grains grow preferably by coalescing neighboring small grains. Moreover, the applied temperature gradient enables the as-formed abnormally large grain to act as a seeding crystal to expand directionally throughout the entire textured copper bar, readily converting the textured polycrystals into a bulk single crystal. The technique is also applicable to the growth of bulk single-crystal nickel. The texture-induced monocrystallization strategy would advance large-scale manufacturing and applications of bulk single crystals.","PeriodicalId":388,"journal":{"name":"Matter","volume":"230 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436290","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}
Layered hybrid perovskites (LHPs) have emerged as promising reduced-dimensional semiconductors for next-generation photonic and energy applications, wherein controlling the size, orientation, and distribution of quantum wells (QWs) is of paramount importance. Here, we reveal that bulky molecular spacers act as crystal-terminating ligands to form colloidal nanoplatelets (NPLs) during early stages of LHP formation. NPLs template the crystallization of LHPs. Using multi-modal diagnostics, we prove that NPLs ripen and grow, playing a decisive role in the time evolution of QW size, population distribution, and orientation. We demonstrate antisolvent drip interrupts NPL ripening and thereby controls QW orientation, population, and energy cascades within LHP films. Using this approach, we achieve low-threshold amplified emission (AE) with remarkable reproducibility. We further introduce synthesized NPLs in the antisolvent step of 3D perovskites to control facet orientation and achieve enhanced efficiency and stability in wide-bandgap solar-cell devices compared to untextured controls.
{"title":"Cationic ligation guides quantum-well formation in layered hybrid perovskites","authors":"Kasra Darabi, Mihirsinh Chauhan, Boyu Guo, Jiantao Wang, Dovletgeldi Seyitliyev, Fazel Bateni, Tonghui Wang, Masoud Ghasemi, Laine Taussig, Nathan Woodward, Xiang-Bin Han, Evgeny O. Danilov, Ruipeng Li, Xiaotong Li, Milad Abolhasani, Kenan Gundogdu, Aram Amassian","doi":"10.1016/j.matt.2024.09.010","DOIUrl":"https://doi.org/10.1016/j.matt.2024.09.010","url":null,"abstract":"Layered hybrid perovskites (LHPs) have emerged as promising reduced-dimensional semiconductors for next-generation photonic and energy applications, wherein controlling the size, orientation, and distribution of quantum wells (QWs) is of paramount importance. Here, we reveal that bulky molecular spacers act as crystal-terminating ligands to form colloidal nanoplatelets (NPLs) during early stages of LHP formation. NPLs template the crystallization of LHPs. Using multi-modal diagnostics, we prove that NPLs ripen and grow, playing a decisive role in the time evolution of QW size, population distribution, and orientation. We demonstrate antisolvent drip interrupts NPL ripening and thereby controls QW orientation, population, and energy cascades within LHP films. Using this approach, we achieve low-threshold amplified emission (AE) with remarkable reproducibility. We further introduce synthesized NPLs in the antisolvent step of 3D perovskites to control facet orientation and achieve enhanced efficiency and stability in wide-bandgap solar-cell devices compared to untextured controls.","PeriodicalId":388,"journal":{"name":"Matter","volume":"26 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142405548","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 : 2024-10-02DOI: 10.1016/j.matt.2024.08.006
Parivash Moradifar , Tao Wang , Nadire Nayir , Tiva Sharifi , Ke Wang , Pulickel Ajayan , Adri C.T. van Duin , Nasim Alem
Layered chalcogenides, including Bi-Sb-Te ternary alloys and heterostructures, are renowned as thermoelectric and topological insulators and have recently been highlighted as plasmonic building blocks beyond noble metals. We conduct joint in situ transmission electron microscopy and density functional theory calculations to investigate the temperature-dependent nanoscale dynamics and interfacial properties, identifying the role of native defects and edge configurations in the anisotropic sublimation of Bi2Te3-Sb2Te3 heterostructures and Sb2-xBixTe3 alloys. We report structural dynamics, including edge evolution, layer-by-layer sublimation, and the formation and coalescence of thermally induced polygonal nanopores. These nanopores are initiated by preferential dissociation of tellurium, reducing thermal stability in heterostructures. Triangular and quasi-hexagonal configurations dominate nanopore structures in heterostructures. Our calculations reveal antisite defects (TeSb and TeBi) as key players in defect-assisted sublimation. These findings enhance our understanding of nanoscale dynamics and assist in designing tunable low-dimensional chalcogenides.
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