Kaijian Xing, Daniel McEwen, Yuefeng Yin, Weiyao Zhao, Abdulhakim Bake, David Cortie, Jingying Liu, Thi-Hai-Yen Vu, Yi-Hsun Chen, James Hone, Alastair Stacey, Mark T. Edmonds, Nikhil V. Medhekar, Kenji Watanabe, Takashi Taniguchi, Qingdong Ou, Dong-Chen Qi, Michael S. Fuhrer
Van der Waals electrode integration is a promising strategy to create nearly perfect interfaces between metals and 2D materials, with advantages such as eliminating Fermi-level pinning and reducing contact resistance. However, the lack of a simple, generalizable pick-and-place transfer technology has greatly hampered the wide use of this technique. We demonstrate the pick-and-place transfer of prefabricated electrodes from reusable polished hydrogenated diamond substrates without the use of any sacrificial layers due to the inherent low-energy and dangling-bond-free nature of the hydrogenated diamond surface. The technique enables transfer of arbitrary-metal electrodes and an electrode array, as demonstrated by successful transfer of eight different elemental metals with work functions ranging from 4.22 to 5.65 eV. We also demonstrate the electrode array transfer for large-scale device fabrication. The mechanical transfer of metal electrodes from diamond to van der Waals materials creates atomically smooth interfaces with no interstitial impurities or disorder, as observed with cross-section high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy. As a demonstration of its device application, we use the diamond transfer technique to create metal contacts to monolayer transition metal dichalcogenide semiconductors with high-work-function Pd, low-work-function Ti, and semimetal Bi to create n- and p-type field-effect transistors with low Schottky barrier heights. We also extend this technology to air-sensitive materials (trilayer 1T’ WTe2) and other applications such as ambipolar transistors, Schottky diodes, and optoelectronics. This highly reliable and reproducible technology paves the way for new device architectures and high-performance devices.
{"title":"Pick-and-Place Transfer of Arbitrary-Metal Electrodes for van der Waals Device Fabrication","authors":"Kaijian Xing, Daniel McEwen, Yuefeng Yin, Weiyao Zhao, Abdulhakim Bake, David Cortie, Jingying Liu, Thi-Hai-Yen Vu, Yi-Hsun Chen, James Hone, Alastair Stacey, Mark T. Edmonds, Nikhil V. Medhekar, Kenji Watanabe, Takashi Taniguchi, Qingdong Ou, Dong-Chen Qi, Michael S. Fuhrer","doi":"10.1021/acsnano.4c13592","DOIUrl":"https://doi.org/10.1021/acsnano.4c13592","url":null,"abstract":"Van der Waals electrode integration is a promising strategy to create nearly perfect interfaces between metals and 2D materials, with advantages such as eliminating Fermi-level pinning and reducing contact resistance. However, the lack of a simple, generalizable pick-and-place transfer technology has greatly hampered the wide use of this technique. We demonstrate the pick-and-place transfer of prefabricated electrodes from reusable polished hydrogenated diamond substrates without the use of any sacrificial layers due to the inherent low-energy and dangling-bond-free nature of the hydrogenated diamond surface. The technique enables transfer of arbitrary-metal electrodes and an electrode array, as demonstrated by successful transfer of eight different elemental metals with work functions ranging from 4.22 to 5.65 eV. We also demonstrate the electrode array transfer for large-scale device fabrication. The mechanical transfer of metal electrodes from diamond to van der Waals materials creates atomically smooth interfaces with no interstitial impurities or disorder, as observed with cross-section high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy. As a demonstration of its device application, we use the diamond transfer technique to create metal contacts to monolayer transition metal dichalcogenide semiconductors with high-work-function Pd, low-work-function Ti, and semimetal Bi to create <i>n</i>- and <i>p</i>-type field-effect transistors with low Schottky barrier heights. We also extend this technology to air-sensitive materials (trilayer 1T’ WTe<sub>2</sub>) and other applications such as ambipolar transistors, Schottky diodes, and optoelectronics. This highly reliable and reproducible technology paves the way for new device architectures and high-performance devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"36 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975221","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}
The emerging combination of chemotherapy and radionuclide therapy has been actively investigated to overcome the limitations of monotherapy and augment therapeutic efficacy. However, it remains a challenge to design a single delivery vehicle that can incorporate chemotherapeutics and radionuclides into a compact structure. Here, a chelator DOTA- or NOTA-modified Evans blue conjugated camptothecin molecule (EB-CPT) nanoprodrug was synthesized, which could self-assemble into nanoparticles due to its inherent amphiphilicity. The nanoparticles could then be effectively labeled with therapeutic radionuclide lutetium-177 (177Lu) or diagnostic radionuclides gallium-68 (68Ga)/copper-64 (64Cu) with high radiolabeling efficiency and radiochemical stability. Impressively, a single-dose chemoradiation therapy of [177Lu]Lu-DOTA-EB-CPT plus EB-CPT effectively inhibited tumor growth in HCT116 tumor-bearing mice compared to the respective individual therapeutic approach. The [64Cu]Cu-NOTA-EB-CPT nanoparticles also exhibited excellent in vivo characteristics including favorable blood circulation properties and prolonged tumor retention in tumor-bearing mice. The safety, feasibility, tolerability, and biodistribution of [68Ga]Ga-NOTA-EB-ss-CPT were also preliminarily characterized in a first-in-human study. This study presents a simple but robust EB-CPT radiopharmaceutical that leverages EB as an albumin binder to strike a delicate balance between enhanced tumor accumulation, safety, and diagnostic efficacy, facilitating an integrated theranostic strategy within a single molecular structure. This radionuclide-labeled EB-CPT nanomedicine presents a step toward clinical translation of the combination of chemotherapy and radiotheranostics.
{"title":"Preclinical and First-in-Human Study of a Compact Radionuclide Labeled Self-Assembly Nanomedicine for Chemo-Radio-Theranostics of Cancer","authors":"Hehe Xiong, Rongxi Wang, Heng Zhang, Qianyu Zhang, Yatong Qin, Chao Du, Xinyi Zhang, Jinmin Ye, Changrong Shi, Huaxiang Shen, Zhaohui Zhu, Zijian Zhou, Xiaoyuan Chen, Jingjing Zhang","doi":"10.1021/acsnano.4c18489","DOIUrl":"https://doi.org/10.1021/acsnano.4c18489","url":null,"abstract":"The emerging combination of chemotherapy and radionuclide therapy has been actively investigated to overcome the limitations of monotherapy and augment therapeutic efficacy. However, it remains a challenge to design a single delivery vehicle that can incorporate chemotherapeutics and radionuclides into a compact structure. Here, a chelator DOTA- or NOTA-modified Evans blue conjugated camptothecin molecule (EB-CPT) nanoprodrug was synthesized, which could self-assemble into nanoparticles due to its inherent amphiphilicity. The nanoparticles could then be effectively labeled with therapeutic radionuclide lutetium-177 (<sup>177</sup>Lu) or diagnostic radionuclides gallium-68 (<sup>68</sup>Ga)/copper-64 (<sup>64</sup>Cu) with high radiolabeling efficiency and radiochemical stability. Impressively, a single-dose chemoradiation therapy of [<sup>177</sup>Lu]Lu-DOTA-EB-CPT plus EB-CPT effectively inhibited tumor growth in HCT116 tumor-bearing mice compared to the respective individual therapeutic approach. The [<sup>64</sup>Cu]Cu-NOTA-EB-CPT nanoparticles also exhibited excellent in vivo characteristics including favorable blood circulation properties and prolonged tumor retention in tumor-bearing mice. The safety, feasibility, tolerability, and biodistribution of [<sup>68</sup>Ga]Ga-NOTA-EB-ss-CPT were also preliminarily characterized in a first-in-human study. This study presents a simple but robust EB-CPT radiopharmaceutical that leverages EB as an albumin binder to strike a delicate balance between enhanced tumor accumulation, safety, and diagnostic efficacy, facilitating an integrated theranostic strategy within a single molecular structure. This radionuclide-labeled EB-CPT nanomedicine presents a step toward clinical translation of the combination of chemotherapy and radiotheranostics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"21 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975223","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}
Optical metasurfaces, arrays of nanostructures engineered to manipulate light, have emerged as a transformative technology in both research and industry due to their compact design and exceptional light control capabilities. Their strong light–matter interactions enable precise wavefront modulation, polarization control, and significant near-field enhancements. These unique properties have recently driven their application in biomedical fields. In particular, metasurfaces have led to breakthroughs in biomedical imaging technologies, such as achromatic imaging, phase imaging, and extended depth-of-focus imaging. They have also advanced cutting-edge biosensing technologies, featuring high-quality factor resonators and near-field enhancements. As the demand for device miniaturization and system integration increases, metasurfaces are expected to play a pivotal role in the development of next-generation biomedical devices. In this review, we explore the latest advancements in the use of metasurfaces for biomedical applications, with a particular focus on imaging and sensing. Additionally, we discuss future directions aimed at transforming the biomedical field by leveraging the full potential of metasurfaces to provide compact, high-performance solutions for a wide range of applications.
{"title":"Optical Metasurfaces for Biomedical Imaging and Sensing","authors":"Hongyoon Kim, Heechang Yun, Sebin Jeong, Seokho Lee, Eunseo Cho, Junsuk Rho","doi":"10.1021/acsnano.4c14751","DOIUrl":"https://doi.org/10.1021/acsnano.4c14751","url":null,"abstract":"Optical metasurfaces, arrays of nanostructures engineered to manipulate light, have emerged as a transformative technology in both research and industry due to their compact design and exceptional light control capabilities. Their strong light–matter interactions enable precise wavefront modulation, polarization control, and significant near-field enhancements. These unique properties have recently driven their application in biomedical fields. In particular, metasurfaces have led to breakthroughs in biomedical imaging technologies, such as achromatic imaging, phase imaging, and extended depth-of-focus imaging. They have also advanced cutting-edge biosensing technologies, featuring high-quality factor resonators and near-field enhancements. As the demand for device miniaturization and system integration increases, metasurfaces are expected to play a pivotal role in the development of next-generation biomedical devices. In this review, we explore the latest advancements in the use of metasurfaces for biomedical applications, with a particular focus on imaging and sensing. Additionally, we discuss future directions aimed at transforming the biomedical field by leveraging the full potential of metasurfaces to provide compact, high-performance solutions for a wide range of applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"28 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975219","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}
Etsuki Kobiyama, Darius Urbonas, Benjamin Aymoz, Maryna I. Bodnarchuk, Gabriele Rainò, Antonis Olziersky, Daniele Caimi, Marilyne Sousa, Rainer F. Mahrt, Maksym V. Kovalenko, Thilo Stöferle
Highly ordered nanocrystal (NC) assemblies, namely, superlattices (SLs), have been investigated as materials for optical and optoelectronic devices due to their unique properties based on interactions among neighboring NCs. In particular, lead halide perovskite NC SLs have attracted significant attention owing to their extraordinary optical characteristics of individual NCs and collective emission processes like superfluorescence (SF). So far, the primary method for preparing perovskite NC SLs has been the drying-mediated self-assembly method, in which the colloidal NCs spontaneously assemble into SLs during solvent evaporation. However, this method lacks controllability because NCs form random-sized SLs at random positions on the substrate, rendering NC assemblies in conjunction with device structures, such as photonic waveguides or microcavities, challenging. Here, we demonstrate template-assisted self-assembly to deterministically place perovskite NC SLs and control their geometrical properties. A solution of CsPbBr3 NCs is drop-casted on a substrate with lithographically defined hollow structures. After solvent evaporation and removal of excess NCs from the substrate surface, NCs remain only in the templates, thereby defining the position and size of these NC assemblies. We performed photoluminescence (PL) measurements on these NC assemblies and observed signatures of SF, similar to those in spontaneously assembled SLs. Our findings are crucial for optical devices that harness embedded perovskite NC assemblies and enable fundamental studies on how these collective effects can be tailored through the SL geometry.
{"title":"Perovskite Nanocrystal Self-Assemblies in 3D Hollow Templates","authors":"Etsuki Kobiyama, Darius Urbonas, Benjamin Aymoz, Maryna I. Bodnarchuk, Gabriele Rainò, Antonis Olziersky, Daniele Caimi, Marilyne Sousa, Rainer F. Mahrt, Maksym V. Kovalenko, Thilo Stöferle","doi":"10.1021/acsnano.4c07819","DOIUrl":"https://doi.org/10.1021/acsnano.4c07819","url":null,"abstract":"Highly ordered nanocrystal (NC) assemblies, namely, superlattices (SLs), have been investigated as materials for optical and optoelectronic devices due to their unique properties based on interactions among neighboring NCs. In particular, lead halide perovskite NC SLs have attracted significant attention owing to their extraordinary optical characteristics of individual NCs and collective emission processes like superfluorescence (SF). So far, the primary method for preparing perovskite NC SLs has been the drying-mediated self-assembly method, in which the colloidal NCs spontaneously assemble into SLs during solvent evaporation. However, this method lacks controllability because NCs form random-sized SLs at random positions on the substrate, rendering NC assemblies in conjunction with device structures, such as photonic waveguides or microcavities, challenging. Here, we demonstrate template-assisted self-assembly to deterministically place perovskite NC SLs and control their geometrical properties. A solution of CsPbBr<sub>3</sub> NCs is drop-casted on a substrate with lithographically defined hollow structures. After solvent evaporation and removal of excess NCs from the substrate surface, NCs remain only in the templates, thereby defining the position and size of these NC assemblies. We performed photoluminescence (PL) measurements on these NC assemblies and observed signatures of SF, similar to those in spontaneously assembled SLs. Our findings are crucial for optical devices that harness embedded perovskite NC assemblies and enable fundamental studies on how these collective effects can be tailored through the SL geometry.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"52 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975418","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}
Immunogenic cell death (ICD) of tumor cells, which is characterized by releasing immunostimulatory “find me” and “eat me” signals, expressing proinflammatory cytokines and providing personalized and broad-spectrum tumor antigens draws increasing attention in developing a tumor vaccine. In this study, we aimed to investigate whether the influenza virus (IAV) is efficient enough to induce ICD in tumor cells and an extra modification of IAV components such as hemeagglutinin (HA) will be helpful for the ICD-induced cells to elicit robust antitumor effects; in addition, to evaluate whether the membrane-engineering polylactic coglycolic acid nanoparticles (PLGA NPs) simulating ICD immune stimulation mechanisms hold the potential to be a promising vaccine candidate, a mouse melanoma cell line (B16–F10 cell) was infected with IAV rescued by the reverse genetic system, and the prepared cells and membrane-modified PLGA NPs were used separately to immunize the melanoma-bearing mice. IAV-infected tumor cells exhibit dying status, releasing high mobility group box-1 (HMGB1) and adenosine triphosphate (ATP), and exposing calreticulin (CRT), IAV hemeagglutinin (HA), and tumor antigens like tyrosinase-related protein 2 (TRP2). IAV-induced ICD cells enhance biomass-derived carbon (BMDCs) migration, antigen uptake, cross-presentation, and maturation in vitro. Furthermore, immunization with IAV-induced ICD cells effectively suppressed tumor growth in melanoma-bearing mice. The isolated cell membrane inherited the immunological characteristics from the ICD cells and elicited robust antitumor immune responses through decorating PLGA NPs loading with a tumor-specific helper T-cell peptide and supplemented with ATP in a hydrogel system. This study indicated a promising strategy for developing cell-based and personalized tumor vaccines through fully taking advantage of the immune stimulation mechanisms of ICD occurrence in tumor cells, IAV modification, and nanoscale delivery.
{"title":"Tumor Vaccine Exploiting Membranes with Influenza Virus-Induced Immunogenic Cell Death to Decorate Polylactic Coglycolic Acid Nanoparticles","authors":"Ying Yang, Yongmao Hu, Ying Yang, Qingwen Liu, Peng Zheng, Zhongqian Yang, Biao Duan, Jinrong He, Weiran Li, Duo Li, Xiao Zheng, Mengzhen Wang, Yuting Fu, Qiong Long, Yanbing Ma","doi":"10.1021/acsnano.4c00654","DOIUrl":"https://doi.org/10.1021/acsnano.4c00654","url":null,"abstract":"Immunogenic cell death (ICD) of tumor cells, which is characterized by releasing immunostimulatory “find me” and “eat me” signals, expressing proinflammatory cytokines and providing personalized and broad-spectrum tumor antigens draws increasing attention in developing a tumor vaccine. In this study, we aimed to investigate whether the influenza virus (IAV) is efficient enough to induce ICD in tumor cells and an extra modification of IAV components such as hemeagglutinin (HA) will be helpful for the ICD-induced cells to elicit robust antitumor effects; in addition, to evaluate whether the membrane-engineering polylactic coglycolic acid nanoparticles (PLGA NPs) simulating ICD immune stimulation mechanisms hold the potential to be a promising vaccine candidate, a mouse melanoma cell line (B16–F10 cell) was infected with IAV rescued by the reverse genetic system, and the prepared cells and membrane-modified PLGA NPs were used separately to immunize the melanoma-bearing mice. IAV-infected tumor cells exhibit dying status, releasing high mobility group box-1 (HMGB1) and adenosine triphosphate (ATP), and exposing calreticulin (CRT), IAV hemeagglutinin (HA), and tumor antigens like tyrosinase-related protein 2 (TRP2). IAV-induced ICD cells enhance biomass-derived carbon (BMDCs) migration, antigen uptake, cross-presentation, and maturation in vitro. Furthermore, immunization with IAV-induced ICD cells effectively suppressed tumor growth in melanoma-bearing mice. The isolated cell membrane inherited the immunological characteristics from the ICD cells and elicited robust antitumor immune responses through decorating PLGA NPs loading with a tumor-specific helper T-cell peptide and supplemented with ATP in a hydrogel system. This study indicated a promising strategy for developing cell-based and personalized tumor vaccines through fully taking advantage of the immune stimulation mechanisms of ICD occurrence in tumor cells, IAV modification, and nanoscale delivery.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975416","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}
Gefei Niu, Jianchen Lu, Lei Gao, Jianqun Geng, Wei Xiong, Yong Zhang, Hui Zhang, Shicheng Li, Yuhang Yang, Boyu Fu, Yi Zhang, Jinming Cai
Artificial dimension control has been playing a vital role in electronic structure manipulation and properties generation. However, systematic investigations into the dimensional regulation, such as transformation from two-dimensional (2D) materials to well-controlled one-dimensional (1D) ribbons, remain insufficient via molecular beam epitaxy. Here, high-quality ultranarrow zigzag CuTe nanoribbons are atomically precisely prepared via the dimensional regulation induced by adjusting the Te chemical potential, utilizing CuSe monolayer as the starting 2D template. Introducing Te atoms into the CuSe monolayer and subsequent annealing, Te atoms replace Se atoms within CuSe lattice. As the Te substitution ratio increases, strain accumulates and elongated nanopores emerge, which expand and interconnect to form 1D CuSe1–xTex (0 ≤ x ≤ 1) nanoribbons and ultimately coalesce into a 1D ultranarrow zigzag CuTe nanoribbons with a honeycomb lattice. The entire structural transformation is verified through scanning tunneling microscopy (STM) and density functional theory (DFT). Contrary to the 2D semiconducting nature of CuSe and CuSe1–xTex monolayers, newly formed 1D CuTe nanoribbons exhibit metallic properties. Intriguingly, DFT calculations further reveal spin-polarized states at the zigzag edges of CuTe nanoribbons. Our proposed dimensional regulation strategy from 2D materials to well-controlled 1D nanoribbons presents avenues for refining and enhancing the synthesis process.
人工尺寸控制在电子结构操作和特性生成方面一直发挥着重要作用。然而，通过分子束外延技术对尺寸调控（如从二维（2D）材料转变为控制良好的一维（1D）带）的系统研究仍然不足。在这里，利用 CuSe 单层作为起始二维模板，通过调节 Te 化学势诱导的尺寸调节，在原子上精确制备出了高质量的超细人字形 CuTe 纳米带。在 CuSe 单层中引入 Te 原子并随后进行退火，Te 原子取代了 CuSe 晶格中的 Se 原子。随着 Te 替代率的增加，应变不断积累并出现细长的纳米孔，这些纳米孔不断扩大并相互连接，形成一维 CuSe1-xTex （0 ≤ x ≤ 1）纳米带，并最终凝聚成具有蜂巢晶格的一维纵向人字形 CuTe 纳米带。扫描隧道显微镜（STM）和密度泛函理论（DFT）验证了整个结构转变过程。与 CuSe 和 CuSe1-xTex 单层的二维半导体性质相反，新形成的一维 CuTe 纳米带具有金属特性。有趣的是，DFT 计算进一步揭示了 CuTe 纳米带之字形边缘的自旋极化态。我们提出的从二维材料到控制良好的一维纳米带的尺寸调节策略为改进和提高合成工艺提供了途径。
{"title":"Atomically Precise Fabrication of Ultranarrow Zigzag CuTe Nanoribbons via Dimensional Regulation","authors":"Gefei Niu, Jianchen Lu, Lei Gao, Jianqun Geng, Wei Xiong, Yong Zhang, Hui Zhang, Shicheng Li, Yuhang Yang, Boyu Fu, Yi Zhang, Jinming Cai","doi":"10.1021/acsnano.4c14204","DOIUrl":"https://doi.org/10.1021/acsnano.4c14204","url":null,"abstract":"Artificial dimension control has been playing a vital role in electronic structure manipulation and properties generation. However, systematic investigations into the dimensional regulation, such as transformation from two-dimensional (2D) materials to well-controlled one-dimensional (1D) ribbons, remain insufficient via molecular beam epitaxy. Here, high-quality ultranarrow zigzag CuTe nanoribbons are atomically precisely prepared via the dimensional regulation induced by adjusting the Te chemical potential, utilizing CuSe monolayer as the starting 2D template. Introducing Te atoms into the CuSe monolayer and subsequent annealing, Te atoms replace Se atoms within CuSe lattice. As the Te substitution ratio increases, strain accumulates and elongated nanopores emerge, which expand and interconnect to form 1D CuSe<sub>1–<i>x</i></sub>Te<sub><i>x</i></sub> (0 ≤ <i>x</i> ≤ 1) nanoribbons and ultimately coalesce into a 1D ultranarrow zigzag CuTe nanoribbons with a honeycomb lattice. The entire structural transformation is verified through scanning tunneling microscopy (STM) and density functional theory (DFT). Contrary to the 2D semiconducting nature of CuSe and CuSe<sub>1–<i>x</i></sub>Te<sub><i>x</i></sub> monolayers, newly formed 1D CuTe nanoribbons exhibit metallic properties. Intriguingly, DFT calculations further reveal spin-polarized states at the zigzag edges of CuTe nanoribbons. Our proposed dimensional regulation strategy from 2D materials to well-controlled 1D nanoribbons presents avenues for refining and enhancing the synthesis process.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"9 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968329","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}
Gerrit Behner, Abdur Rehman Jalil, Alina Rupp, Hans Lüth, Detlev Grützmacher, Thomas Schäpers
The combination of an ordinary s-type superconductor with three-dimensional topological insulators creates a promising platform for fault-tolerant topological quantum computing circuits based on Majorana braiding. The backbone of the braiding mechanism are three-terminal Josephson junctions. It is crucial to understand the transport in these devices for further use in quantum computing applications. We present low-temperature measurements of topological insulator-based three-terminal Josephson junctions fabricated by a combination of selective-area growth of Bi0.8Sb1.2Te3 and shadow mask evaporation of Nb. This approach allows for the in situ fabrication of Josephson junctions with an exceptional interface quality, important for the study of the proximity-effect. We map out the transport properties of the device as a function of bias currents and prove the coupling of the junctions by the observation of a multiterminal geometry-induced diode effect. We find good agreement of our findings with a resistively and capacitively shunted junction network model.
{"title":"Superconductive Coupling Effects in Selectively Grown Topological Insulator-Based Three-Terminal Junctions","authors":"Gerrit Behner, Abdur Rehman Jalil, Alina Rupp, Hans Lüth, Detlev Grützmacher, Thomas Schäpers","doi":"10.1021/acsnano.4c15893","DOIUrl":"https://doi.org/10.1021/acsnano.4c15893","url":null,"abstract":"The combination of an ordinary s-type superconductor with three-dimensional topological insulators creates a promising platform for fault-tolerant topological quantum computing circuits based on Majorana braiding. The backbone of the braiding mechanism are three-terminal Josephson junctions. It is crucial to understand the transport in these devices for further use in quantum computing applications. We present low-temperature measurements of topological insulator-based three-terminal Josephson junctions fabricated by a combination of selective-area growth of Bi<sub>0.8</sub>Sb<sub>1.2</sub>Te<sub>3</sub> and shadow mask evaporation of Nb. This approach allows for the in situ fabrication of Josephson junctions with an exceptional interface quality, important for the study of the proximity-effect. We map out the transport properties of the device as a function of bias currents and prove the coupling of the junctions by the observation of a multiterminal geometry-induced diode effect. We find good agreement of our findings with a resistively and capacitively shunted junction network model.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"26 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975222","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}
Tongpeng Zhao, Ruiqin He, Tanghao Liu, Yanhao Li, De Yu, Yuxin Gao, Geyang Qu, Ning Li, Chunmei Wang, Huang Huang, Jiong Zhou, Sai Bai, Shumin Xiao, Zhaolai Chen, Yimu Chen, Qinghai Song
The power conversion efficiencies (PCEs) of polycrystalline perovskite solar cells (PC–PSCs) have now reached a plateau after a decade of rapid development, leaving a distinct gap from their Shockley-Queisser limit. To continuously mitigate the PCE deficit, nonradiative carrier losses resulting from defects should be further optimized. Single-crystal perovskites are considered an ideal platform to study the efficiency limit of perovskite solar cells due to their intrinsically low defect density, as demonstrated in bulk single crystals. However, current single-crystal perovskite solar cells (SC-PSCs) based on single-crystal thin film (SCTF) suffer from severe nonradiative carrier losses at the interface and in the bulk simultaneously due to the immature SCTF growth techniques. In this study, we show that the SC-PSCs can outperform state-of-the-art PC–PSCs, with MAPbI3 as an example, by suppressing carrier losses at the interface and in the bulk in device-compatible SCTFs through precisely controlling their growth.
{"title":"Mitigating the Efficiency Deficit in Single-Crystal Perovskite Solar Cells by Precise Control of the Growth Processes","authors":"Tongpeng Zhao, Ruiqin He, Tanghao Liu, Yanhao Li, De Yu, Yuxin Gao, Geyang Qu, Ning Li, Chunmei Wang, Huang Huang, Jiong Zhou, Sai Bai, Shumin Xiao, Zhaolai Chen, Yimu Chen, Qinghai Song","doi":"10.1021/acsnano.4c11691","DOIUrl":"https://doi.org/10.1021/acsnano.4c11691","url":null,"abstract":"The power conversion efficiencies (PCEs) of polycrystalline perovskite solar cells (PC–PSCs) have now reached a plateau after a decade of rapid development, leaving a distinct gap from their Shockley-Queisser limit. To continuously mitigate the PCE deficit, nonradiative carrier losses resulting from defects should be further optimized. Single-crystal perovskites are considered an ideal platform to study the efficiency limit of perovskite solar cells due to their intrinsically low defect density, as demonstrated in bulk single crystals. However, current single-crystal perovskite solar cells (SC-PSCs) based on single-crystal thin film (SCTF) suffer from severe nonradiative carrier losses at the interface and in the bulk simultaneously due to the immature SCTF growth techniques. In this study, we show that the SC-PSCs can outperform state-of-the-art PC–PSCs, with MAPbI<sub>3</sub> as an example, by suppressing carrier losses at the interface and in the bulk in device-compatible SCTFs through precisely controlling their growth.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"16 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968328","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}
The synthesis of covalent organic frameworks (COFs) with excellent luminescent properties and their effective application in the field of bionic sensing remain a formidable challenge. Herein, a series of COFs with different numbers of hydroxyl groups are successfully synthesized, and the number of hydroxyl groups on the benzene-1,3,5-tricarbaldehyde (BTA) linker influences the properties of the final COFs. The COF (HHBTA-OH) prepared with hydrazine hydrate (HH) and BTA containing one hydroxyl group as the ligands exhibits the best fluorescent performance. MA@HHBTA-OH is formed by the reaction of HHBTA-OH with meldrum’s acid (MA) and has its extremely high hydrophilicity, dispersibility, and strong red fluorescence, which can imitate the human gustatory system to detect bitter substances. MA@HHBTA-OH was combined with agarose (AG) to construct a MA@HHBTA-OH@AG film for assessing food freshness. In addition, an acoustic MA@HHBTA-OH@MF sensor is fabricated by integrating luminescent MA@HHBTA-OH with melamine foam (MF) through a strong hydrogen bond. MA@HHBTA-OH@MF functions like an eardrum and recognizes sound through pressure waves with excellent mechanical sensing performance. In summary, biomimetic luminescent sensors based on MA@HHBTA-OH were successfully constructed, which can monitor auditory, gustatory, and olfactory information to achieve the multimode perception of sound, bitter substances, and food freshness.
{"title":"Bionic Luminescent Sensors Based on Covalent Organic Frameworks: Auditory, Gustatory, and Olfactory Information Monitoring for Multimode Perception","authors":"Xueping Quan, Kai Zhu, Yinsheng Liu, Bing Yan","doi":"10.1021/acsnano.4c15289","DOIUrl":"https://doi.org/10.1021/acsnano.4c15289","url":null,"abstract":"The synthesis of covalent organic frameworks (COFs) with excellent luminescent properties and their effective application in the field of bionic sensing remain a formidable challenge. Herein, a series of COFs with different numbers of hydroxyl groups are successfully synthesized, and the number of hydroxyl groups on the benzene-1,3,5-tricarbaldehyde (BTA) linker influences the properties of the final COFs. The COF (HHBTA-OH) prepared with hydrazine hydrate (HH) and BTA containing one hydroxyl group as the ligands exhibits the best fluorescent performance. MA@HHBTA-OH is formed by the reaction of HHBTA-OH with meldrum’s acid (MA) and has its extremely high hydrophilicity, dispersibility, and strong red fluorescence, which can imitate the human gustatory system to detect bitter substances. MA@HHBTA-OH was combined with agarose (AG) to construct a MA@HHBTA-OH@AG film for assessing food freshness. In addition, an acoustic MA@HHBTA-OH@MF sensor is fabricated by integrating luminescent MA@HHBTA-OH with melamine foam (MF) through a strong hydrogen bond. MA@HHBTA-OH@MF functions like an eardrum and recognizes sound through pressure waves with excellent mechanical sensing performance. In summary, biomimetic luminescent sensors based on MA@HHBTA-OH were successfully constructed, which can monitor auditory, gustatory, and olfactory information to achieve the multimode perception of sound, bitter substances, and food freshness.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"51 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968330","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}
Robert L. Stamps, Rehana Begum Popy, Johan van Lierop
Theory and simulations are used to demonstrate implementation of a variational Bayes algorithm called “active inference” in interacting arrays of nanomagnetic elements. The algorithm requires stochastic elements, and a simplified model based on a magnetic artificial spin ice geometry is used to illustrate how nanomagnets can generate the required random dynamics. Examples of tracking and PID control are demonstrated and shown to be consistent with the original stochastic differential equation formulation of active inference. Interestingly, nonlinear response in the form of spikes and spike trains not predicted by the original theory can appear in the nanomagnet system for certain temperature regimes. A theoretical approach using a mean-field approximation for spin systems is proposed, which describes the transition to nonlinear response. Finally, the possibility to create simple magnetic arrays using realistic models is shown with micromagnetic simulations of a simple 17 element array of nanomagnets that include magnetic anisotropies, and exchange and dipolar interactions. Possible applications are simulated to illustrate how nanomagnetic arrays can be used as the stochastic element for feedback control of processes, investigation and control of magnetic state evolution, and as a method to optimize pulsed field magnetic switching protocols.
{"title":"Active Inference and Artificial Spin Ice: Control Processes and State Selection","authors":"Robert L. Stamps, Rehana Begum Popy, Johan van Lierop","doi":"10.1021/acsnano.4c13673","DOIUrl":"https://doi.org/10.1021/acsnano.4c13673","url":null,"abstract":"Theory and simulations are used to demonstrate implementation of a variational Bayes algorithm called “active inference” in interacting arrays of nanomagnetic elements. The algorithm requires stochastic elements, and a simplified model based on a magnetic artificial spin ice geometry is used to illustrate how nanomagnets can generate the required random dynamics. Examples of tracking and PID control are demonstrated and shown to be consistent with the original stochastic differential equation formulation of active inference. Interestingly, nonlinear response in the form of spikes and spike trains not predicted by the original theory can appear in the nanomagnet system for certain temperature regimes. A theoretical approach using a mean-field approximation for spin systems is proposed, which describes the transition to nonlinear response. Finally, the possibility to create simple magnetic arrays using realistic models is shown with micromagnetic simulations of a simple 17 element array of nanomagnets that include magnetic anisotropies, and exchange and dipolar interactions. Possible applications are simulated to illustrate how nanomagnetic arrays can be used as the stochastic element for feedback control of processes, investigation and control of magnetic state evolution, and as a method to optimize pulsed field magnetic switching protocols.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"74 6 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975421","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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