ACS Nano最新文献

{"title":"Decoupling Strategy to Separate Training and Inference with Three-Dimensional Neuromorphic Hardware Composed of Neurons and Hybrid Synapses","authors":"Jung-Woo Lee, See-On Park, Seong-Yun Yun, Yeeun Kim, Hyun Myung, Shinhyun Choi, Yang-Kyu Choi","doi":"10.1021/acsnano.4c18145","DOIUrl":"https://doi.org/10.1021/acsnano.4c18145","url":null,"abstract":"Monolithic 3D integration of neuron and synapse devices is considered a promising solution for energy-efficient and compact neuromorphic hardware. However, achieving optimal performance in both training and inference remains challenging as these processes require different synapse devices with reliable endurance and long retention. Here, we introduce a decoupling strategy to separate training and inference using monolithically integrated neuromorphic hardware with layer-by-layer fabrication. This 3D neuromorphic hardware includes neurons consisting of a single transistor (1T-neuron) in the first layer, long-term operational synapses composed of a single thin-film transistor with a SONOS structure (1TFT-synapses) in the second layer for inference, and durable synapses composed of a memristor (1M-synapses) in the third layer for training. A 1TFT-synapse, utilizing a charge-trap layer, exhibits long retention properties favorable for inference tasks. In contrast, a 1M-synapse, leveraging anion movement at the interface, demonstrates robust endurance for repetitive weight updates during training. With the proposed hybrid synapse architecture, frequent training can be performed using the 1M-synapses with robust endurance, while intermittent inference can be managed using the 1TFT-synapses with long-term retention. This decoupling of synaptic functions is advantageous for achieving a reliable spiking neural network (SNN) in neuromorphic computing.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"35 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713777","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":"2-Nitroimidazole-Functionalized Superparamagnetic Iron Oxide Nanoparticles Detect Hypoxic Regions of Glioblastomas on MRI and Improve Radiotherapy Efficacy","authors":"Yuki Yoshino, Fumi Yoshino, Ichio Aoki, Yasuyuki Mori, Gen Suzuki, Shunichiro Tsuji, Tsukuru Amano, Akihiko Shiino, Tokuhiro Chano, Yoshio Furusho, Takashi Murakami, Hideya Yamazaki, Kei Yamada","doi":"10.1021/acsnano.4c06753","DOIUrl":"https://doi.org/10.1021/acsnano.4c06753","url":null,"abstract":"The presence of hypoxic regions in tumors is associated with malignancy and is an important target for the high-precision diagnosis and treatment of tumors. Radioresistant hypoxic regions can be precisely identified and treated without the use of high doses of radiation if hypoxic region-specific contrast agents have a therapeutic effect. In this study, we synthesized a therapeutic-diagnostic complex agent (SPION-PG-NI) by combining polyglycerol-functionalized superparamagnetic iron oxide nanoparticles (SPION-PG, core diameter of 8.8 ± 1.9 nm) as an MRI contrast agent and 2-nitroimidazole (NI, a pimonidazole derivative) as a hypoxia-targeted ligand to visually evaluate hypoxic regions using MRI and improve radiotherapy efficacy at those sites. SPION-PG-NI showed a concentration-dependent contrast effect and had significantly higher accumulation in subcutaneous glioblastomas than the control agent, SPION-PG, 24 h after administration. Immunohistological evaluations showed that the SPION-PG-NI-accumulated regions corresponded well to hypoxic regions. SPION-PG-NI showed neither migration into the brain parenchyma nor neurotoxicity. Both SPION-PG and SPION-PG-NI decrease reactive oxygen species (ROS); however, they improve radiotherapy efficacy in hypoxic glioblastoma cells due to cytotoxicity. This effect of SPION-PG-NI was significantly higher than that of SPION-PG (<i>p</i> &lt; 0.01). After 12 Gy irradiation, the mean normalized glioblastoma tumor volume on day 38 in the SPION-PG-NI group (288%) was significantly lower than that in the control group (882%) (<i>p</i> &lt; 0.05). Collectively, these findings suggest the potential of SPION-PG-NI as a useful and safe tumor theranostic nanodevice for hypoxic imaging and improving radiotherapy efficacy.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"30 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713780","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":"Layered Metal–Organic Chalcogenides: 2D Optoelectronics in 3D Self-Assembled Semiconductors","authors":"Watcharaphol Paritmongkol, Zhifu Feng, Sivan Refaely-Abramson, William A. Tisdale, Christoph Kastl, Lorenzo Maserati","doi":"10.1021/acsnano.4c18493","DOIUrl":"https://doi.org/10.1021/acsnano.4c18493","url":null,"abstract":"Molecular self-assembly offers an effective and scalable way to design nanostructured materials with tunable optoelectronic properties. In the past 30 years, organic chemistry has delivered a plethora of metal–organic structures based on the combination of organic groups, chalcogens, and a broad range of metals. Among these, several layered metal–organic chalcogenides (MOCs)─including “mithrene” (AgSePh)─recently emerged as interesting platforms to host 2D physics embedded in 3D crystals. Their combination of broad tunability, easy processability, and promising optoelectronic performance is driving a renewed interest in the more general material group of “low-dimensional” hybrids. In addition, the covalent MOC lattice provides higher stability compared with polar materials in operating devices. Here, we provide a perspective on the rise of 2D MOCs in terms of their synthesis approaches, 2D quantum confined exciton physics, and potential future applications in UV and X-ray photodetection, chemical sensors, and electrocatalysis.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"3 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703440","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":"Leveraging Vitamin C to Augment Nanoenabled Photothermal Immunotherapy","authors":"Wuxian Deng, Yiyuan Wang, Junyu Wang, Yitan Su, Mingyang Li, Kun Qu, Yucai Wang, Min Li","doi":"10.1021/acsnano.4c17080","DOIUrl":"https://doi.org/10.1021/acsnano.4c17080","url":null,"abstract":"Photothermal immunotherapy (PTI) is valuable for precise tumor targeting and immune activation. However, its efficacy is hindered by insufficient immune response, elevated antioxidant levels within tumor, and intrinsic tumor resistance mechanisms. This study introduces Vitamin C (VC), a widely available dietary nutrient, as an effective enhancer for PTI. High-dose VC induces oxidative imbalance in tumor cells, making them more susceptible to nanoenabled near-infrared-II photothermal therapy (NIR-II PTT) with the photosensitizer IR1080. The combination of VC and NIR-II PTT significantly amplifies antitumor immunity by upregulating CXCL16 expression and promoting CXCR6⁺ T cell infiltration. Clinical data reveal that higher CXCL16 and CXCR6 levels in human tumors correlate with improved survival and T cell infiltration, underscoring the translational potential of this approach. This study positions VC as a safe, accessible, and cost-effective dietary enhancer for PTI, reshaping the role of dietary nutrients in cancer therapy and offering a strategy for overcoming treatment resistance.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"72 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713761","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":"Unveiling the Assembly Transition of Diphenylalanine and Its Analogs: from Oligomer Equilibrium to Nanocluster Formation","authors":"Chang Liu, Yoav Dan, Ji Yun, Lihi Adler-Abramovich, Jinghui Luo","doi":"10.1021/acsnano.5c00433","DOIUrl":"https://doi.org/10.1021/acsnano.5c00433","url":null,"abstract":"Peptide self-assembly is fundamental to various biological processes and holds significant potential for nanotechnology and biomedical applications. Despite progress in understanding larger-scale assemblies, the early formation of low-molecular-weight oligomers remains poorly understood. In this study, we investigate the aggregation behavior of the self-assembling diphenylalanine (FF) peptide and its analogs. Utilizing single-nanopore analysis, we detected and characterized the low-molecular-oligomer formation of FF, <i>N</i>-<i>tert</i>-butoxycarbonyl-diphenylalanine (BocFF), fluorenylmethyloxycarbonyl-diphenylalanine (FmocFF), and fluorenylmethyloxycarbonyl-pentafluoro-phenylalanine (Fmoc-F₅-Phe) in real time. This approach provided detailed insights into the early stages of peptide self-assembly, revealing the dynamic behavior and formation kinetics of low-molecular-weight oligomeric species. Analysis revealed that the trimer is the key nucleus for FF, while the dimer is the primary nucleus for FmocFF and Fmoc-F₅-Phe aggregation, whereas both the dimer and trimer serve as nuclei for BocFF. Mass photometry was employed to track the evolution of these oligomers, revealing the transition from low- to high-molecular-weight species, thereby elucidating intermediate phases in the aggregation process. Transmission electron microscopy and Fourier transform infrared spectroscopy were further employed to characterize the final assembly states, offering high-resolution imaging of morphological structures and detailed information on secondary structures. Based on these analyses, we constructed a comprehensive graph that correlates the entire aggregation processes of the tested self-assembling peptides across multiple scales. This integrative approach provides a holistic understanding of peptide self-assembly, particularly in the formation of low-molecular-weight oligomers toward mature supramolecular structures. These findings shed light on their assembly pathways and structural properties, advancing our understanding of their assembly pathways for nanotechnology and biomedical applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"16 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703441","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":"Artificial Intelligence-Assisted Multimode Microrobot Swarm Behaviors","authors":"Xuanjie Xia, Miao Ni, Mengchen Wang, Bin Wang, Dong Liu, Yuan Lu","doi":"10.1021/acsnano.4c16347","DOIUrl":"https://doi.org/10.1021/acsnano.4c16347","url":null,"abstract":"Mimicking the swarm behaviors in nature, the microswarm has shown dynamic transformations and flexible assemblies in complex physiological environments, garnering increasing attention for its potential medical applications. However, because of the complexity of swarm behaviors and the corresponding influencing factors, achieving controllability, stability, and diversity of an artificial microswarm remains challenging. Here, a physically assisted artificial intelligence analysis framework was employed to predict the multimode swarm behaviors of a magnetic microswarm. By modulating 12 different parameters of a programmable magnetic field, we obtained various swarm patterns, including liquid, rod, network, ribbon, flocculence, and vortex. A physical model was developed to simulate the programmable 3D magnetic field and the corresponding collective behaviors. Explainable artificial intelligence analysis uncovered the relationship between control parameters and magnetic swarm patterns, achieving a prediction accuracy of 83.87% for pattern classification. Our stability analysis revealed that rod and vortex patterns exhibited higher stability, making them ideal for precise manipulation tasks. Leveraging this framework, we demonstrated environmentally adaptive swarm navigation through complex channels and swarm hunting of specific targets. This study could not only advance the understanding of microswarm control but also provide a strategy for targeted delivery and micromanipulation in potential clinical applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"4 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713776","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":"Phase Changes of Multielemental Alloy Nanoparticles at Elevated Temperatures","authors":"Zhennan Huang, Tangyuan Li, Ying Fang, Jacob Smith, Boyang Li, Alexandra Brozena, Qi Dong, Qian Zhang, Yiheng Du, Scott X. Mao, Guofeng Wang, Miaofang Chi, Liangbing Hu","doi":"10.1021/acsnano.5c02343","DOIUrl":"https://doi.org/10.1021/acsnano.5c02343","url":null,"abstract":"Multielemental alloy (MEA) nanomaterials, such as medium and high entropy alloys, display promising catalytic performance in a range of chemical reactions due to their multicomponent structural configurations. These complex structural and chemical arrangements can be influenced by several factors, such as mechanical stress, irradiation, and high temperatures, which impact the performance of MEAs in various applications. Here, we investigated the effect of high temperatures on MEA nanoparticles composed of noble and transition metals (quaternary PtPdFeCo) at the atomic scale and found the material undergoes a series of phase transitions between solid solution and intermetallic phases at elevated temperatures ranging from room temperature to 1073 K. In contrast, the binary PtFe nanoalloy displays a one-way solid solution to intermetallic transition at these temperatures. Our findings, rationalized by density functional theory (DFT) studies, demonstrate how the varied migration energies of elements govern the solid solution to intermetallic transition and how differences in the bonding energies of elemental pairs influence the Gibbs free energy change (Δ<i>G</i>), which dictates the intermetallic to solid-solution transition. Overall, this work provides better guidance in the design, development, and usage of nano-MEAs for high-temperature-based applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"22 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713779","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":"Correction to “Dual Strategies Based on Golgi Apparatus/Endoplasmic Reticulum Targeting and Anchoring for High-Efficiency siRNA Delivery and Tumor RNAi Therapy”","authors":"Yashi Wang, Sheng Yin, Dan He, Yujia Zhang, Ziyan Dong, Zhipeng Tian, Jiayu Li, Fang Chen, Yang Wang, Man Li, Qin He","doi":"10.1021/acsnano.5c01048","DOIUrl":"https://doi.org/10.1021/acsnano.5c01048","url":null,"abstract":"In the original paper, we identified an error in the Supporting Information. One representative image of the colocalization of endoplasmic reticulum and CPD/FAM-siNC at 4 h was inadvertently used incorrectly during assembly of the images in Figure S6. The authors would like to apologize for this error. The corrected Figure S6 is presented below. The correction does not affect the results or conclusions of this study. Figure S6. Subcellular localization of CPD/FAM-siNC and CPD/FAM-siNC/CS at 4 h. This article has not yet been cited by other publications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"21 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703442","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":"Iron Homeostasis-Regulated Adaptive Metabolism of PEGylated Ultrasmall Iron Oxide Nanoparticles","authors":"Ning Wang, Dandan Zhou, Keyang Xu, Dandan Kou, Can Chen, Cang Li, Jianxian Ge, Lei Chen, Jianfeng Zeng, Mingyuan Gao","doi":"10.1021/acsnano.5c01399","DOIUrl":"https://doi.org/10.1021/acsnano.5c01399","url":null,"abstract":"Iron oxide nanoparticles have become increasingly significant in the biomedical field due to their exceptional magnetic properties and biocompatibility. However, understanding their <i>in vivo</i> metabolism and transformation is crucial due to the potential biological effects they may induce. This study investigates the metabolic pathways of PEGylated ultrasmall iron oxide nanoparticles (PUSIONPs) <i>in vivo</i>, particularly under varying iron statuses and dosages. Employing a comprehensive analytical approach─including magnetic resonance imaging, elemental analysis, histological assessments, hematological analysis, and Western blot analysis─the biodistribution and transformation of PUSIONPs were mapped. The findings reveal significant differences in the metabolic fate of PUSIONPs between iron-sufficient and iron-deficient conditions, underscoring the pivotal role of iron homeostasis in regulating PUSIONPs biodegradation. In iron-deficient states, degradation and transformation were markedly accelerated, with the released iron rapidly incorporated into hemoglobin. Additionally, the liver and spleen exhibited different PUSIONPs metabolism rates due to their distinct physiological roles: the spleen, primarily responsible for iron recycling, facilitated faster degradation, while the liver, serving as an iron storage organ, showed slower degradation. Under iron deficiency, most degradation products were directed toward hemoglobin synthesis, whereas under normal conditions, the liver gradually metabolized the degradation products, and the spleen retained higher iron levels. Moreover, PUSIONPs degradation demonstrated dose dependency, with higher doses slowing degradation and reducing the utilization rate by the iron-deficient body. Comprehensive safety evaluations confirmed that PUSIONPs exhibit excellent biocompatibility across all doses, with no significant safety concerns. Compared to the clinically used intravenous iron supplement iron sucrose, PUSIONPs also demonstrated superior bioavailability and more effective iron supplementation. These findings provide critical insights into the interaction between iron oxide nanoparticles and iron metabolism, offering a foundation for future research and the broader application of PUSIONPs in biomedical contexts.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"88 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703443","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":"Mitigation of Nonradiative Recombination by Reconfiguring Triplet Energy of Additive Toward Efficient Blue Perovskite Light-Emitting Diodes","authors":"Shuang-Qiao Sun, Qi Sun, Yating Cai, Zi-Qi Feng, Qi Zheng, Bochen Liu, Min Zhu, Tingting Shi, Liang-Sheng Liao, Yue-Min Xie, Shuit-Tong Lee, Man-Keung Fung","doi":"10.1021/acsnano.4c18116","DOIUrl":"https://doi.org/10.1021/acsnano.4c18116","url":null,"abstract":"The exceptional optoelectronic properties of metal halide perovskites, including enhanced color saturation and tunable emission wavelengths, render them highly potential candidates for fabricating perovskite light-emitting diodes (PeLEDs). However, blue PeLEDs underperform relative to their red and green counterparts due to substantial nonradiative recombination losses, particularly at the perovskite/electron transporting layer (ETL) interface. Here, we propose an effective energy management strategy aimed at boosting the efficiency of blue PeLEDs by the incorporation of a multifunctional interlayer, specifically 2,8-bis(diphenylphosphoryl)dibenzo[<i>b</i>,<i>d</i>]furan (PPF), at the perovskite/ETL interface. This approach involves the formation of robust P═O/Pb bonds between PPF and perovskite surface defects, thereby effectively mitigating trap-induced nonradiative recombination. Furthermore, the high triplet energy level of PPF inhibits triplet energy transfer from the perovskite to the ETL, leading to further reductions in energy loss. Consequently, the optimized blue PeLEDs exhibit a peak external quantum efficiency (EQE) of 15.1% (peak emission at 472 nm) with a 4-fold increased operational lifetime compared to the control PeLED. Additionally, utilizing blue PeLED units treated with PPF, we achieve a record EQE of 31.1% for hybrid perovskite/organic tandem white LEDs, which exhibit a high color rendering index of 85.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"43 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703438","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}