Duy-Thuc Nguyen, Min-Jun Baek, Sang Min Lee, Dahan Kim, So-Yeol Yoo, Jae-Young Lee, Dae-Duk Kim
{"title":"Photobleaching-mediated charge-convertible cyclodextrin nanoparticles achieve deep tumour penetration for rectal cancer theranostics","authors":"Duy-Thuc Nguyen, Min-Jun Baek, Sang Min Lee, Dahan Kim, So-Yeol Yoo, Jae-Young Lee, Dae-Duk Kim","doi":"10.1038/s41565-024-01757-4","DOIUrl":"10.1038/s41565-024-01757-4","url":null,"abstract":"Although charge-converting nanoparticles (NPs) potentially penetrate tumours deeply, conventional charge conversion strategies possess limitations, including low selectivity and slow, inconsistent conversion rate within the tumour microenvironment. In this study, we synthesized a zwitterionic near-infrared cyclodextrin derivative of heptamethine cyanine and complexed it with pheophorbide-conjugated ferrocene to produce multifunctional theranostic nanotherapeutics. Our NPs demonstrated enhanced tumour-targeting ability, enabling the highly specific imaging of rectal tumours, with tumour-to-rectum signal ratios reaching up to 7.8. The zwitterionic surface charge of the NPs was rapidly converted to a cationic charge within the tumours on 880 nm near-infrared laser irradiation, promoting the tumoural penetration of NPs via transcytosis. After penetration, photodynamic/chemodynamic therapy was initiated using a 660 nm laser. Our NPs eradicated clinically relevant-sized heterotopic tumours (~250 mm3) and orthotopic rectal tumours, displaying their potential as theranostic nanoplatforms for targeting rectal cancer. The photobleaching property of heptamethine cyanine enables efficient charge conversion of nanoparticles. Here heptamethine-cyanine-based nanoparticles achieve specific tumour imaging, deep tumour penetration and high therapeutic efficacy in rectal cancer animal models.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1723-1734"},"PeriodicalIF":38.1,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142013824","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}
{"title":"Microstrain screening towards defect-less layered transition metal oxide cathodes","authors":"Wenhua Zuo, Jihyeon Gim, Tianyi Li, Dewen Hou, Yibo Gao, Shiyuan Zhou, Chen Zhao, Xin Jia, Zhenzhen Yang, Yuzi Liu, Wenqian Xu, Xianghui Xiao, Gui-Liang Xu, Khalil Amine","doi":"10.1038/s41565-024-01734-x","DOIUrl":"10.1038/s41565-024-01734-x","url":null,"abstract":"Microstrain and the associated surface-to-bulk propagation of structural defects are known to be major roadblocks to developing high-energy and long-life batteries. However, the origin and effects of microstrain during the synthesis of battery materials remain largely unknown. Here we perform microstrain screening during real-time and realistic synthesis of sodium layered oxide cathodes. Evidence gathered from multiscale in situ synchrotron X-ray diffraction and microscopy characterization collectively reveals that the spatial distribution of transition metals within individual precursor particles strongly governs the nanoscale phase transformation, local charge heterogeneity and accumulation of microstrain during synthesis. This unexpected dominance of transition metals results in a counterintuitive outward propagation of defect nucleation and growth. These insights direct a more rational synthesis route to reduce the microstrain and crystallographic defects within the bulk lattice, leading to significantly improved structural stability. The present work on microstrain screening represents a critical step towards synthesis-by-design of defect-less battery materials. In situ synchrotron X-ray tools are used to perform microstrain screening during solid-state synthesis of battery materials, leading to fewer structural defects and improved performance.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1644-1653"},"PeriodicalIF":38.1,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007498","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}
Jehyun Kim, Himanshu Dev, Ravi Kumar, Alexey Ilin, André Haug, Vishal Bhardwaj, Changki Hong, Kenji Watanabe, Takashi Taniguchi, Ady Stern, Yuval Ronen
{"title":"Aharonov–Bohm interference and statistical phase-jump evolution in fractional quantum Hall states in bilayer graphene","authors":"Jehyun Kim, Himanshu Dev, Ravi Kumar, Alexey Ilin, André Haug, Vishal Bhardwaj, Changki Hong, Kenji Watanabe, Takashi Taniguchi, Ady Stern, Yuval Ronen","doi":"10.1038/s41565-024-01751-w","DOIUrl":"10.1038/s41565-024-01751-w","url":null,"abstract":"In the fractional quantum Hall effect, quasiparticles are collective excitations that have a fractional charge and show fractional statistics as they interchange positions. While the fractional charge affects semi-classical characteristics such as shot noise and charging energies, fractional statistics is most notable through quantum interference. Here we study fractional statistics in a bilayer graphene Fabry–Pérot interferometer. We tune the interferometer from the Coulomb-dominated regime to the Aharonov–Bohm regime, both for integer and fractional quantum Hall states. Focusing on the fractional quantum Hall state with a filling factor ν = 1/3, we follow the evolution of the Aharonov–Bohm interference of quasiparticles while varying the magnetic flux through an interference loop and the charge density within the loop independently. When their combined variation is such that the Landau filling remains 1/3, the charge density in the loop varies continuously. We then observe pristine Aharonov–Bohm oscillations with a period of three flux quanta, as expected for quasiparticles of one-third of the electron charge. Yet, when the combined variation leads to discrete events of quasiparticle addition or removal, phase jumps emerge and alter the phase evolution. Notably, across all cases with discrete and continuous charge variation, the average phase consistently increases by 2π with each addition of one electron to the loop, as expected for quasiparticles, obeying fractional statistics. Electrostatically tunable graphene-based electronic interferometers show non-trivial exchange statistics of quasiparticles, revealing their wave-like properties.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1619-1626"},"PeriodicalIF":38.1,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007627","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}
{"title":"Single-molecule sensing inside stereo- and regio-defined hetero-nanopores","authors":"Wei Liu, Qiang Zhu, Chao-Nan Yang, Ying-Huan Fu, Ji-Chang Zhang, Meng-Yin Li, Zhong-Lin Yang, Kai-Li Xin, Jing Ma, Mathias Winterhalter, Yi-Lun Ying, Yi-Tao Long","doi":"10.1038/s41565-024-01721-2","DOIUrl":"10.1038/s41565-024-01721-2","url":null,"abstract":"Heteromeric pore-forming proteins often contain recognition patterns or stereospecific selection filters. However, the construction of heteromeric pore-forming proteins for single-molecule sensing is challenging due to the uncontrollability of producing position isomers and difficulties in purification of regio-defined products. To overcome these preparation obstacles, we present an in situ strategy involving single-molecule chemical modification of a heptameric pore-forming protein to build a stereo- and regio-specific heteromeric nanopore (hetero-nanopore) with a subunit stoichiometric ratio of 3:4. The steric hindrance inherent in the homo-nanopore of K238C aerolysin directs the stereo- and regio-selective modification of maleimide derivatives. Our method utilizes real-time ionic current recording to facilitate controlled voltage manipulation for stoichiometric modification and position-based side-isomer removal. Single-molecule experiments and all-atom molecular dynamics simulations revealed that the hetero-nanopore features an asymmetric stereo- and regio-defined residue structure. The hetero-nanopore produced was characterized by mass spectrometry and single-particle cryogenic electron microscopy. In a proof-of-concept single-molecule sensing experiment, the hetero-nanopore exhibited 95% accuracy for label-free discrimination of four peptide stereoisomers with single-amino-acid structural and chiral differences in the mixtures. The customized hetero-nanopores could advance single-molecule sensing. This Article presents a single-molecule ‘synthesis by sensing’ approach that enables in situ stepwise generation of stereo- and regio-defined heteromeric nanopores to resolve structural and chiral differences of amino-acids in single peptide stereoisomers.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1693-1701"},"PeriodicalIF":38.1,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007611","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}
Xingliang Liu, Shi Chen, Jing Huang, Yibo Du, Zhi Luo, Yue Zhang, Lixin Liu, Yongming Chen
{"title":"Synthetic polypeptides inhibit nucleic acid-induced inflammation in autoimmune diseases by disrupting multivalent TLR9 binding to LL37-DNA bundles","authors":"Xingliang Liu, Shi Chen, Jing Huang, Yibo Du, Zhi Luo, Yue Zhang, Lixin Liu, Yongming Chen","doi":"10.1038/s41565-024-01759-2","DOIUrl":"10.1038/s41565-024-01759-2","url":null,"abstract":"Complexes of extracellular nucleic acids (NAs) with endogenous proteins or peptides, such as LL37, break immune balance and cause autoimmune diseases, whereas NAs with arginine-enriched peptides do not. Inspired by this, we synthesize a polyarginine nanoparticle PEG-TK-NPArg, which effectively inhibits Toll-like receptor-9 (TLR9) activation, in contrast to LL37. To explore the discrepancy effect of PEG-TK-NPArg and LL37, we evaluate the periodic structure of PEG-TK-NPArg-NA and LL37-NA complexes using small-angle X-ray scattering. LL37-NA complexes have a larger inter-NA spacing that accommodates TLR9, while the inter-NA spacing in PEG-TK-NPArg-NA complexes mismatches with the cavity of TLR9, thus inhibiting an interaction with multiple TLR9s, limiting their clustering and damping immune induction. Subsequently, the inhibitory inflammation effect of PEG-TK-NPArg is proved in an animal model of rheumatoid arthritis. This work on how the scavenger-NA complexes inhibit the immune response may facilitate proof-of-concept research translating to clinical application. This study shows how amino acid composition and topology in synthetic polypeptides affect anti-inflammatory effects and how scavenging debris nucleic acids inhibits inflammation and relieves symptoms of autoimmune diseases.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1745-1756"},"PeriodicalIF":38.1,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142002804","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}
{"title":"Nanomedicine pioneers awarded the Kavli Prize","authors":"","doi":"10.1038/s41565-024-01777-0","DOIUrl":"10.1038/s41565-024-01777-0","url":null,"abstract":"The 2024 Kavli Prize in Nanoscience is awarded to three nanomedicine pioneers who laid the foundation of controlled release, biomedical imaging and diagnostics.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 8","pages":"1073-1073"},"PeriodicalIF":38.1,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41565-024-01777-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141992012","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}
Yung-Chien Chou, Chih-Yuan Lin, Alice Castan, Joshua Chen, Rachael Keneipp, Parisa Yasini, Dimitri Monos, Marija Drndić
{"title":"Coupled nanopores for single-molecule detection","authors":"Yung-Chien Chou, Chih-Yuan Lin, Alice Castan, Joshua Chen, Rachael Keneipp, Parisa Yasini, Dimitri Monos, Marija Drndić","doi":"10.1038/s41565-024-01746-7","DOIUrl":"10.1038/s41565-024-01746-7","url":null,"abstract":"Rapid sensing of molecules is increasingly important in many studies and applications, such as DNA sequencing and protein identification. Here, beyond atomically thin 2D nanopores, we conceptualize, simulate and experimentally demonstrate coupled, guiding and reusable bilayer nanopore platforms, enabling advanced ultrafast detection of unmodified molecules. The bottom layer can collimate and decelerate the molecule before it enters the sensing zone, and the top 2D pore (~2 nm) enables position sensing. We varied the number of pores in the bottom layer from one to nine while fixing one 2D pore in the top layer. When the number of pores in the bottom layer is reduced to one, sensing is performed by both layers, and distinct T- and W-shaped translocation signals indicate the precise position of molecules and are sensitive to fragment lengths. This is uniquely enabled by microsecond resolution capabilities and precision nanofabrication. Coupled nanopores represent configurable multifunctional systems with inter- and intralayer structures for improved electromechanical control and prolonged dwell times in a 2D sensing zone. In this study, the authors present the design and fabrication of reusable, atomically thin, coupled bilayer solid-state nanopores that enable the slowing down and positional tracking of molecules for label-free, single-molecule sensing.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1686-1692"},"PeriodicalIF":38.1,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141980964","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}
Tingbiao Guo, Zhi Zhang, Zijian Lin, Jiahan Tian, Yi Jin, Julian Evans, Yinghe Xu, Sailing He
{"title":"Durable and programmable ultrafast nanophotonic matrix of spectral pixels","authors":"Tingbiao Guo, Zhi Zhang, Zijian Lin, Jiahan Tian, Yi Jin, Julian Evans, Yinghe Xu, Sailing He","doi":"10.1038/s41565-024-01756-5","DOIUrl":"10.1038/s41565-024-01756-5","url":null,"abstract":"Locally addressable nanophotonic devices are essential for modern applications such as light detection, optical imaging, beam steering and displays. Despite recent advances, a versatile solution with a high-speed tuning rate, long-life durability and programmability across multiple pixels remains elusive. Here we introduce a programmable nanophotonic matrix consisting of vanadium dioxide (VO2) cavities on pixelated microheaters that meets all these requirements. The indirect Joule heating of these VO2 cavities can result in pronounced spectral modulation with colour changes and ensures exceptional endurance even after a million switching cycles. Precise control over the thermal dissipation power through a SiO2 layer of an optimized thickness on Si facilitates an ultrafast modulation rate exceeding 70 kHz. We demonstrated a video-rate nanophotonic colour display by electrically addressing a matrix of 12 × 12 pixels. Furthermore, inspired by the unique pixel-level programmability with multiple intermediate states of the spectral pixels, a spatiotemporal modulation concept is introduced for spectrum detection. Electrically addressable VO2 elements show large resonance shifts during phase transitions, producing a brilliant colour change at a modulation rate of 70 kHz.","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"19 11","pages":"1635-1643"},"PeriodicalIF":38.1,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41565-024-01756-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141918864","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}