Pub Date : 2024-12-05DOI: 10.1038/s41565-024-01821-z
Kangkang Ge, Hui Shao, Zifeng Lin, Pierre-Louis Taberna, Patrice Simon
The advancement of high-performance fast-charging materials has significantly propelled progress in electrochemical capacitors (ECs). Electrochemical capacitors store charges at the nanoscale electrode material–electrolyte interface, where the charge storage and transport mechanisms are mediated by factors such as nanoconfinement, local electrode structure, surface properties and non-electrostatic ion–electrode interactions. This Review offers a comprehensive exploration of probing the confined electrochemical interface using advanced characterization techniques. Unlike classical two-dimensional (2D) planar interfaces, partial desolvation and image charges play crucial roles in effective charge storage under nanoconfinement in porous materials. This Review also highlights the potential of zero charge as a key design principle driving nanoscale ion fluxes and carbon–electrolyte interactions in materials such as 2D and three-dimensional (3D) porous carbons. These considerations are crucial for developing efficient and rapid energy storage solutions for a wide range of applications. This Review clarifies the charge storage and transport mechanisms at confined electrochemical interfaces in electrochemical capacitors, emphasizing their importance in fast-charging energy storage applications.
{"title":"Advanced characterization of confined electrochemical interfaces in electrochemical capacitors","authors":"Kangkang Ge, Hui Shao, Zifeng Lin, Pierre-Louis Taberna, Patrice Simon","doi":"10.1038/s41565-024-01821-z","DOIUrl":"10.1038/s41565-024-01821-z","url":null,"abstract":"The advancement of high-performance fast-charging materials has significantly propelled progress in electrochemical capacitors (ECs). Electrochemical capacitors store charges at the nanoscale electrode material–electrolyte interface, where the charge storage and transport mechanisms are mediated by factors such as nanoconfinement, local electrode structure, surface properties and non-electrostatic ion–electrode interactions. This Review offers a comprehensive exploration of probing the confined electrochemical interface using advanced characterization techniques. Unlike classical two-dimensional (2D) planar interfaces, partial desolvation and image charges play crucial roles in effective charge storage under nanoconfinement in porous materials. This Review also highlights the potential of zero charge as a key design principle driving nanoscale ion fluxes and carbon–electrolyte interactions in materials such as 2D and three-dimensional (3D) porous carbons. These considerations are crucial for developing efficient and rapid energy storage solutions for a wide range of applications. This Review clarifies the charge storage and transport mechanisms at confined electrochemical interfaces in electrochemical capacitors, emphasizing their importance in fast-charging energy storage applications.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"196-208"},"PeriodicalIF":38.1,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777096","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 : 2024-12-05DOI: 10.1038/s41565-024-01825-9
Jun Yi, En-Ming You, Guo-Kun Liu, Zhong-Qun Tian
The 50th anniversary of its discovery underscores surface-enhanced Raman spectroscopy (SERS) as one of the oldest and most dynamic branches of nanoscience and nanotechnology. The time has come for nanostructure-based SERS to integrate artificial intelligence (AI) tools and overcome current commercialization challenges.
{"title":"AI–nano-driven surface-enhanced Raman spectroscopy for marketable technologies","authors":"Jun Yi, En-Ming You, Guo-Kun Liu, Zhong-Qun Tian","doi":"10.1038/s41565-024-01825-9","DOIUrl":"10.1038/s41565-024-01825-9","url":null,"abstract":"The 50th anniversary of its discovery underscores surface-enhanced Raman spectroscopy (SERS) as one of the oldest and most dynamic branches of nanoscience and nanotechnology. The time has come for nanostructure-based SERS to integrate artificial intelligence (AI) tools and overcome current commercialization challenges.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 12","pages":"1758-1762"},"PeriodicalIF":38.1,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777099","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}
Spintronics based on ferromagnets has enabled the development of microwave oscillators and diodes. To achieve even faster operation, antiferromagnets hold great promise despite their challenging manipulation. So far, controlling antiferromagnetic order with microwave currents remains elusive. Here we induce the coherent rotation of antiferromagnetic spins in a Weyl antiferromagnet W/Mn3Sn epitaxial bilayer by DC spin–orbit torque. We show the efficient coupling of this spin rotation with microwave current. The coupled dynamics produce a DC anomalous Hall voltage through rectification, which we coin the antiferromagnetic spin-torque diode effect. Unlike in ferromagnetic systems, the output voltage shows minimal dependence on frequency because of the stabilization of the precession cone angle by exchange interactions. Between 10 GHz and 30 GHz, the output voltage decreases by only 10%. Numerical simulations further reveal that the rectification signals arise from the fast frequency modulation of chiral spin rotation by microwave spin–orbit torque. These results may help the development of high-speed microwave devices for next-generation telecommunication applications. In a Mn3Sn/W epitaxial bilayer, spin–orbit torque induces the coherent rotation of spins, which can couple to microwave currents. Unlike in ferromagnets, the resulting conversion of AC current to DC voltage remains robust at higher frequencies, which may facilitate the development of high-speed electronic devices.
{"title":"Antiferromagnetic spin-torque diode effect in a kagome Weyl semimetal","authors":"Shoya Sakamoto, Takuya Nomoto, Tomoya Higo, Yuki Hibino, Tatsuya Yamamoto, Shingo Tamaru, Yoshinori Kotani, Hidetoshi Kosaki, Masanobu Shiga, Daisuke Nishio-Hamane, Tetsuya Nakamura, Takayuki Nozaki, Kay Yakushiji, Ryotaro Arita, Satoru Nakatsuji, Shinji Miwa","doi":"10.1038/s41565-024-01820-0","DOIUrl":"10.1038/s41565-024-01820-0","url":null,"abstract":"Spintronics based on ferromagnets has enabled the development of microwave oscillators and diodes. To achieve even faster operation, antiferromagnets hold great promise despite their challenging manipulation. So far, controlling antiferromagnetic order with microwave currents remains elusive. Here we induce the coherent rotation of antiferromagnetic spins in a Weyl antiferromagnet W/Mn3Sn epitaxial bilayer by DC spin–orbit torque. We show the efficient coupling of this spin rotation with microwave current. The coupled dynamics produce a DC anomalous Hall voltage through rectification, which we coin the antiferromagnetic spin-torque diode effect. Unlike in ferromagnetic systems, the output voltage shows minimal dependence on frequency because of the stabilization of the precession cone angle by exchange interactions. Between 10 GHz and 30 GHz, the output voltage decreases by only 10%. Numerical simulations further reveal that the rectification signals arise from the fast frequency modulation of chiral spin rotation by microwave spin–orbit torque. These results may help the development of high-speed microwave devices for next-generation telecommunication applications. In a Mn3Sn/W epitaxial bilayer, spin–orbit torque induces the coherent rotation of spins, which can couple to microwave currents. Unlike in ferromagnets, the resulting conversion of AC current to DC voltage remains robust at higher frequencies, which may facilitate the development of high-speed electronic devices.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"216-221"},"PeriodicalIF":38.1,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142760034","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 : 2024-11-26DOI: 10.1038/s41565-024-01816-w
Jung Jae Park, Seung Hwan Ko
Colloidal liquid metals with gradient heterointerfaces offer a scalable and cost-effective solution to the persistent challenges of thermal management in high-performance electronics.
{"title":"Nanoscale gradient interface for efficient heat transfer","authors":"Jung Jae Park, Seung Hwan Ko","doi":"10.1038/s41565-024-01816-w","DOIUrl":"10.1038/s41565-024-01816-w","url":null,"abstract":"Colloidal liquid metals with gradient heterointerfaces offer a scalable and cost-effective solution to the persistent challenges of thermal management in high-performance electronics.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 1","pages":"8-9"},"PeriodicalIF":38.1,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712865","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 : 2024-11-26DOI: 10.1038/s41565-024-01828-6
Patanjali Kambhampati
Lasing from quantum dots has been demonstrated in the previously inaccessible blue spectral region by virtue of carefully engineered Zn-based materials.
通过精心设计的锌基材料，量子点在以前无法进入的蓝色光谱区域实现了激光。
{"title":"Quantum dots are beginning to lase in the blue","authors":"Patanjali Kambhampati","doi":"10.1038/s41565-024-01828-6","DOIUrl":"10.1038/s41565-024-01828-6","url":null,"abstract":"Lasing from quantum dots has been demonstrated in the previously inaccessible blue spectral region by virtue of carefully engineered Zn-based materials.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"189-189"},"PeriodicalIF":38.1,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712867","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 advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm−2) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-Li3N SSE. This vacancy-rich β-Li3N SSE shows a high ionic conductivity of 2.14 × 10−3 S cm−1 at 25 °C and surpasses almost all the reported nitride-based SSEs. A Li- and N-vacancy-mediated fast lithium-ion migration mechanism is unravelled regarding vacancy-triggered reduced activation energy and increased mobile lithium-ion population. All-solid-state lithium symmetric cells using vacancy-rich β-Li3N achieve breakthroughs in high critical current densities up to 45 mA cm−2 and high capacities up to 7.5 mAh cm−2, and ultra-stable lithium stripping and plating processes over 2,000 cycles. The high lithium compatibility mechanism of vacancy-rich β-Li3N is unveiled as intrinsic stability to lithium metal. In addition, β-Li3N possesses excellent air stability through the formation of protection surfaces. All-solid-state lithium metal batteries using the vacancy-rich β-Li3N as SSE interlayers and lithium cobalt oxide (LCO) and Ni-rich LiNi0.83Co0.11Mn0.06O2 (NCM83) cathodes exhibit excellent battery performance. Extremely stable cycling performance is demonstrated with high capacity retentions of 82.05% with 95.2 mAh g−1 over 5,000 cycles at 1.0 C for LCO and 92.5% with 153.6 mAh g−1 over 3,500 cycles at 1.0 C for NCM83. Utilizing the vacancy-rich β-Li3N SSE and NCM83 cathodes, the all-solid-state lithium metal batteries successfully accomplished mild rapid charge and discharge rates up to 5.0 C, retaining 60.47% of the capacity. Notably, these batteries exhibited a high areal capacity, registering approximately 5.0 mAh cm−2 for the compact pellet-type cells and around 2.2 mAh cm−2 for the all-solid-state lithium metal pouch cells. This new β-Li3N solid-state electrolyte demonstrates a vacancy-mediated superionic diffusion mechanism, achieving high ionic conductivity (2.14 × 10−3 S cm−1) and effectively suppressing lithium dendrite growth. Its high compatibility with lithium and air stability promises improved safety and performance in all-solid-state lithium metal batteries, making it ideal for advanced energy storage applications.
全固态锂金属电池的发展需要在固态电解质（SSE）方面取得突破，以抑制锂枝晶在高电流密度和高容量（>3 mAh cm-2）条件下的生长，并在晶体结构、离子导电性和刚性方面对固态电解质进行创新。在此，我们报告了一种超离子导电、高度锂兼容和空气稳定的富空位 β-Li3N SSE。这种富含空位的 β-Li3N SSE 在 25 °C 时的离子电导率高达 2.14 × 10-3 S cm-1，几乎超过了所有已报道的氮化物基 SSE。通过空位引发的活化能降低和移动锂离子群增加，揭示了锂离子和氮空位介导的快速锂离子迁移机制。使用富空位 β-Li3N 的全固态锂对称电池在高临界电流密度（高达 45 mA cm-2）、高容量（高达 7.5 mAh cm-2）以及超过 2,000 次循环的超稳定锂剥离和电镀过程方面取得了突破性进展。富空位 β-Li3N 的高锂兼容性机制被揭示为对锂金属的内在稳定性。此外，β-Li3N 通过形成保护表面而具有出色的空气稳定性。使用富空位的 β-Li3N 作为 SSE 夹层以及锂钴氧化物（LCO）和富镍 LiNi0.83Co0.11Mn0.06O2 (NCM83) 正极的全固态锂金属电池表现出优异的电池性能。LCO 在 1.0 C 下循环 5,000 次后，容量保持率为 82.05%，达到 95.2 mAh g-1；NCM83 在 1.0 C 下循环 3,500 次后，容量保持率为 92.5%，达到 153.6 mAh g-1。利用富含空位的 β-Li3N SSE 和 NCM83 正极，全固态锂金属电池成功实现了高达 5.0 C 的轻度快速充放电，并保留了 60.47% 的容量。值得注意的是，这些电池表现出较高的平均容量，紧凑型颗粒电池的平均容量约为 5.0 mAh cm-2，全固态锂金属袋电池的平均容量约为 2.2 mAh cm-2。
{"title":"Superionic conducting vacancy-rich β-Li3N electrolyte for stable cycling of all-solid-state lithium metal batteries","authors":"Weihan Li, Minsi Li, Shuo Wang, Po-Hsiu Chien, Jing Luo, Jiamin Fu, Xiaoting Lin, Graham King, Renfei Feng, Jian Wang, Jigang Zhou, Ruying Li, Jue Liu, Yifei Mo, Tsun-Kong Sham, Xueliang Sun","doi":"10.1038/s41565-024-01813-z","DOIUrl":"10.1038/s41565-024-01813-z","url":null,"abstract":"The advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm−2) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-Li3N SSE. This vacancy-rich β-Li3N SSE shows a high ionic conductivity of 2.14 × 10−3 S cm−1 at 25 °C and surpasses almost all the reported nitride-based SSEs. A Li- and N-vacancy-mediated fast lithium-ion migration mechanism is unravelled regarding vacancy-triggered reduced activation energy and increased mobile lithium-ion population. All-solid-state lithium symmetric cells using vacancy-rich β-Li3N achieve breakthroughs in high critical current densities up to 45 mA cm−2 and high capacities up to 7.5 mAh cm−2, and ultra-stable lithium stripping and plating processes over 2,000 cycles. The high lithium compatibility mechanism of vacancy-rich β-Li3N is unveiled as intrinsic stability to lithium metal. In addition, β-Li3N possesses excellent air stability through the formation of protection surfaces. All-solid-state lithium metal batteries using the vacancy-rich β-Li3N as SSE interlayers and lithium cobalt oxide (LCO) and Ni-rich LiNi0.83Co0.11Mn0.06O2 (NCM83) cathodes exhibit excellent battery performance. Extremely stable cycling performance is demonstrated with high capacity retentions of 82.05% with 95.2 mAh g−1 over 5,000 cycles at 1.0 C for LCO and 92.5% with 153.6 mAh g−1 over 3,500 cycles at 1.0 C for NCM83. Utilizing the vacancy-rich β-Li3N SSE and NCM83 cathodes, the all-solid-state lithium metal batteries successfully accomplished mild rapid charge and discharge rates up to 5.0 C, retaining 60.47% of the capacity. Notably, these batteries exhibited a high areal capacity, registering approximately 5.0 mAh cm−2 for the compact pellet-type cells and around 2.2 mAh cm−2 for the all-solid-state lithium metal pouch cells. This new β-Li3N solid-state electrolyte demonstrates a vacancy-mediated superionic diffusion mechanism, achieving high ionic conductivity (2.14 × 10−3 S cm−1) and effectively suppressing lithium dendrite growth. Its high compatibility with lithium and air stability promises improved safety and performance in all-solid-state lithium metal batteries, making it ideal for advanced energy storage applications.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"265-275"},"PeriodicalIF":38.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41565-024-01813-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696538","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}
Selective conversion of syngas to value-added higher alcohols (containing two or more carbon atoms), particularly to a specific alcohol, is of great interest but remains challenging. Here we show that atomically intimate assembly of FeOx-Rh-ZrO2 dual interfaces by selectively architecting highly dispersed FeOx on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol. The ethanol selectivity in oxygenates reached ~90% at CO conversion up to 51%, along with a markedly high space-time yield of ethanol of 668.2 mg gcat−1 h−1. In situ spectroscopic characterization and theoretical calculations reveal that Rh-ZrO2 interface promotes dissociative CO activation into CHx through a formate pathway, while the adjacent Rh-FeOx interface accelerates subsequent C–C coupling via nondissociative CO insertion. Consequently, these dual interfaces in atomic-scale proximity with complementary functionalities synergistically boost the exclusive formation of ethanol with exceptional productivity in a tandem manner. Atomically intimate assembly of FeOx-Rh-ZrO2 dual interfaces by selectively architecting highly dispersed FeOx on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol.
{"title":"Atomically intimate assembly of dual metal–oxide interfaces for tandem conversion of syngas to ethanol","authors":"Shang Li, Li Feng, Hengwei Wang, Yue Lin, Zhihu Sun, Lulu Xu, Yuxing Xu, Xinyu Liu, Wei-Xue Li, Shiqiang Wei, Jin-Xun Liu, Junling Lu","doi":"10.1038/s41565-024-01824-w","DOIUrl":"10.1038/s41565-024-01824-w","url":null,"abstract":"Selective conversion of syngas to value-added higher alcohols (containing two or more carbon atoms), particularly to a specific alcohol, is of great interest but remains challenging. Here we show that atomically intimate assembly of FeOx-Rh-ZrO2 dual interfaces by selectively architecting highly dispersed FeOx on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol. The ethanol selectivity in oxygenates reached ~90% at CO conversion up to 51%, along with a markedly high space-time yield of ethanol of 668.2 mg gcat−1 h−1. In situ spectroscopic characterization and theoretical calculations reveal that Rh-ZrO2 interface promotes dissociative CO activation into CHx through a formate pathway, while the adjacent Rh-FeOx interface accelerates subsequent C–C coupling via nondissociative CO insertion. Consequently, these dual interfaces in atomic-scale proximity with complementary functionalities synergistically boost the exclusive formation of ethanol with exceptional productivity in a tandem manner. Atomically intimate assembly of FeOx-Rh-ZrO2 dual interfaces by selectively architecting highly dispersed FeOx on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"255-264"},"PeriodicalIF":38.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696542","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 : 2024-11-15DOI: 10.1038/s41565-024-01809-9
Cheng Xu, Xue Qin, Xin Wei, Jie Yu, Youjia Zhang, Yan Zhang, Dan Ding, Jibin Song, Kanyi Pu
Leveraging X-rays to initiate prolonged luminescence (radio-afterglow) and stimulate radiodynamic 1O2 production from optical agents provides opportunities for diagnosis and therapy at tissue depths inaccessible to light. However, X-ray-responsive organic luminescent materials are rare due to their intrinsic low X-ray conversion efficiency. Here we report a cascade X-ray energy converting approach to develop organic radio-afterglow nanoprobes (RANPs) for cancer theranostics. RANPs comprise a radiowave absorber that down-converts X-ray energy to emit radioluminescence, which is transferred to a radiosensitizer to produce singlet oxygen (1O2). 1O2 then reacts with a radio-afterglow substrate to generate an active intermediate that simultaneously decomposes to emit radio-afterglow. Through finetuning such a cascade, intraparticle radioluminescence energy transfer and the 1O2 transfer process, RANPs possess tunable wavelengths and long half-lives, and generate radio-afterglow and 1O2 at tissue depths of up to 15 cm. Moreover, we developed a biomarker-activatable nanoprobe (tRANP) that produces a tumour-specific radio-afterglow signal, leading to ultrasensitive detection and the possibility of surgical removal of diminutive tumours (1 mm3) under an X-ray dosage 20 times lower than inorganic materials. The efficient radiodynamic 1O2 generation of tRANP permits complete tumour eradication at an X-ray dosage lower than clinical radiotherapy and a drug dosage one to two orders of magnitude lower than most existing inorganic agents, leading to prolonged survival rates with minimized radiation-related adverse effects. Thus, our work reveals a generic approach to address the lack of organic radiotheranostic materials and provides molecular design towards precision cancer radiotherapy. Here, the authors present the design, molecular assembly and mechanistic insights into an organic, biomarker-activatable radiotheranostic nanoprobe for image-guided precision cancer radiotherapy with sensitivity up to a depth of 15 cm in thick tissues.
利用 X 射线启动长时间发光（放射余辉）并刺激光学制剂产生放射动力 1O2 为在光线无法到达的组织深度进行诊断和治疗提供了机会。然而，X 射线响应型有机发光材料因其固有的低 X 射线转换效率而十分罕见。在此，我们报告了一种级联 X 射线能量转换方法，以开发用于癌症治疗的有机放射余辉纳米探针（RANPs）。RANPs 由一个辐射波吸收器组成，该吸收器能向下转换 X 射线能量，从而发出辐射光，辐射光转移到辐射增敏剂上，产生单线态氧（1O2）。然后，1O2 与放射余辉基质反应生成活性中间体，活性中间体同时分解并发出放射余辉。通过对这种级联、粒子内放射发光能量转移和 1O2 转移过程进行微调，RANPs 具有可调波长和长半衰期，可在组织深度达 15 厘米处产生放射余辉和 1O2。此外，我们还开发了一种可激活生物标记物的纳米探针（tRANP），它能产生肿瘤特异性的放射余辉信号，从而实现超灵敏检测，并能在 X 射线剂量比无机材料低 20 倍的情况下，对微小肿瘤（1 立方毫米）进行手术切除。tRANP 的高效放射动力 1O2 生成允许以低于临床放疗的 X 射线剂量和比大多数现有无机制剂低一到两个数量级的药物剂量彻底根除肿瘤，从而延长生存率并最大限度地减少与辐射相关的不良反应。因此，我们的工作揭示了一种解决有机放射治疗材料缺乏问题的通用方法，并为实现精准癌症放射治疗提供了分子设计。
{"title":"A cascade X-ray energy converting approach toward radio-afterglow cancer theranostics","authors":"Cheng Xu, Xue Qin, Xin Wei, Jie Yu, Youjia Zhang, Yan Zhang, Dan Ding, Jibin Song, Kanyi Pu","doi":"10.1038/s41565-024-01809-9","DOIUrl":"10.1038/s41565-024-01809-9","url":null,"abstract":"Leveraging X-rays to initiate prolonged luminescence (radio-afterglow) and stimulate radiodynamic 1O2 production from optical agents provides opportunities for diagnosis and therapy at tissue depths inaccessible to light. However, X-ray-responsive organic luminescent materials are rare due to their intrinsic low X-ray conversion efficiency. Here we report a cascade X-ray energy converting approach to develop organic radio-afterglow nanoprobes (RANPs) for cancer theranostics. RANPs comprise a radiowave absorber that down-converts X-ray energy to emit radioluminescence, which is transferred to a radiosensitizer to produce singlet oxygen (1O2). 1O2 then reacts with a radio-afterglow substrate to generate an active intermediate that simultaneously decomposes to emit radio-afterglow. Through finetuning such a cascade, intraparticle radioluminescence energy transfer and the 1O2 transfer process, RANPs possess tunable wavelengths and long half-lives, and generate radio-afterglow and 1O2 at tissue depths of up to 15 cm. Moreover, we developed a biomarker-activatable nanoprobe (tRANP) that produces a tumour-specific radio-afterglow signal, leading to ultrasensitive detection and the possibility of surgical removal of diminutive tumours (1 mm3) under an X-ray dosage 20 times lower than inorganic materials. The efficient radiodynamic 1O2 generation of tRANP permits complete tumour eradication at an X-ray dosage lower than clinical radiotherapy and a drug dosage one to two orders of magnitude lower than most existing inorganic agents, leading to prolonged survival rates with minimized radiation-related adverse effects. Thus, our work reveals a generic approach to address the lack of organic radiotheranostic materials and provides molecular design towards precision cancer radiotherapy. Here, the authors present the design, molecular assembly and mechanistic insights into an organic, biomarker-activatable radiotheranostic nanoprobe for image-guided precision cancer radiotherapy with sensitivity up to a depth of 15 cm in thick tissues.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"286-295"},"PeriodicalIF":38.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637119","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 : 2024-11-15DOI: 10.1038/s41565-024-01810-2
Leveraging X-rays to induce prolonged luminescence (radio-afterglow) and radiodynamic effects from typically inorganic optical agents enables diagnosis and therapy at light-inaccessible tissue depths. Now, a cascade X-ray energy conversion approach is developed to increase the intrinsically low X-ray conversion efficiency of organic molecules for the construction of radio-afterglow nanoprobes for cancer theranostics.
利用 X 射线诱导典型的无机光学制剂产生长时间发光（放射余辉）和放射动力学效应，可在光线无法到达的组织深度进行诊断和治疗。现在，我们开发了一种级联 X 射线能量转换方法，以提高有机分子固有的低 X 射线转换效率，从而构建用于癌症治疗的放射余辉纳米探针。
{"title":"Organic radio-afterglow nanoprobes for cancer theranostics","authors":"","doi":"10.1038/s41565-024-01810-2","DOIUrl":"10.1038/s41565-024-01810-2","url":null,"abstract":"Leveraging X-rays to induce prolonged luminescence (radio-afterglow) and radiodynamic effects from typically inorganic optical agents enables diagnosis and therapy at light-inaccessible tissue depths. Now, a cascade X-ray energy conversion approach is developed to increase the intrinsically low X-ray conversion efficiency of organic molecules for the construction of radio-afterglow nanoprobes for cancer theranostics.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"194-195"},"PeriodicalIF":38.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637118","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 recent discovery of superconductivity and magnetism in trilayer rhombohedral graphene (RG) establishes an ideal, untwisted platform to study strong correlation electronic phenomena. However, the correlated effects in multilayer RG have received limited attention, and, particularly, the evolution of the correlations with increasing layer number remains an unresolved question. Here we show the observation of layer-dependent electronic structures and correlations—under surprising liquid nitrogen temperature—in RG multilayers from 3 to 9 layers by using scanning tunnelling microscopy and spectroscopy. We explicitly determine layer-enhanced low-energy flat bands and interlayer coupling strengths. The former directly demonstrates the further flattening of low-energy bands in thicker RG, and the latter indicates the presence of varying interlayer interactions in RG multilayers. Moreover, we find significant splittings of the flat bands, ranging from ~50 meV to 80 meV, at 77 K when they are partially filled, indicating the emergence of interaction-induced strongly correlated states. Particularly, the strength of the correlated states is notably enhanced in thicker RG and reaches its maximum in the six-layer, validating directly theoretical predictions and establishing abundant new candidates for strongly correlated systems. Our results provide valuable insights into the layer dependence of the electronic properties in RG and demonstrate it as a suitable system for investigating robust and highly accessible correlated phases. By using scanning tunnelling microscopy and spectroscopy, researchers observe layer-dependent electronic correlations in rhombohedral graphene multilayers at 77 K, revealing the layer-enhanced low-energy flat bands and interlayer interactions.
{"title":"Layer-dependent evolution of electronic structures and correlations in rhombohedral multilayer graphene","authors":"Yang Zhang, Yue-Ying Zhou, Shihao Zhang, Hao Cai, Ling-Hui Tong, Wei-Yu Liao, Ruo-Jue Zou, Si-Min Xue, Yuan Tian, Tongtong Chen, Qiwei Tian, Chen Zhang, Yiliu Wang, Xuming Zou, Xingqiang Liu, Yuanyuan Hu, Ya-Ning Ren, Li Zhang, Lijie Zhang, Wen-Xiao Wang, Lin He, Lei Liao, Zhihui Qin, Long-Jing Yin","doi":"10.1038/s41565-024-01822-y","DOIUrl":"10.1038/s41565-024-01822-y","url":null,"abstract":"The recent discovery of superconductivity and magnetism in trilayer rhombohedral graphene (RG) establishes an ideal, untwisted platform to study strong correlation electronic phenomena. However, the correlated effects in multilayer RG have received limited attention, and, particularly, the evolution of the correlations with increasing layer number remains an unresolved question. Here we show the observation of layer-dependent electronic structures and correlations—under surprising liquid nitrogen temperature—in RG multilayers from 3 to 9 layers by using scanning tunnelling microscopy and spectroscopy. We explicitly determine layer-enhanced low-energy flat bands and interlayer coupling strengths. The former directly demonstrates the further flattening of low-energy bands in thicker RG, and the latter indicates the presence of varying interlayer interactions in RG multilayers. Moreover, we find significant splittings of the flat bands, ranging from ~50 meV to 80 meV, at 77 K when they are partially filled, indicating the emergence of interaction-induced strongly correlated states. Particularly, the strength of the correlated states is notably enhanced in thicker RG and reaches its maximum in the six-layer, validating directly theoretical predictions and establishing abundant new candidates for strongly correlated systems. Our results provide valuable insights into the layer dependence of the electronic properties in RG and demonstrate it as a suitable system for investigating robust and highly accessible correlated phases. By using scanning tunnelling microscopy and spectroscopy, researchers observe layer-dependent electronic correlations in rhombohedral graphene multilayers at 77 K, revealing the layer-enhanced low-energy flat bands and interlayer interactions.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"20 2","pages":"222-228"},"PeriodicalIF":38.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601594","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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