Nano LettersPub Date : 2025-03-26DOI: 10.1021/acs.nanolett.5c00458
Yang Li, Quanlin Chen, Yawei Lv, Yufan Wang, Saif M. H. Qaid, Ying Jiang, Fuxiang Li, Xiujuan Zhuang, Mingjian Yuan
{"title":"Order–Disorder Transition Induced Dynamic Rashba Effect in 2D Halide Perovskites","authors":"Yang Li, Quanlin Chen, Yawei Lv, Yufan Wang, Saif M. H. Qaid, Ying Jiang, Fuxiang Li, Xiujuan Zhuang, Mingjian Yuan","doi":"10.1021/acs.nanolett.5c00458","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00458","url":null,"abstract":"Two-dimensional (2D) hybrid organic–inorganic perovskites exhibit pronounced Rashba splitting, positioning them as promising candidates for spintronic applications. However, the underlying mechanism of inversion symmetry breaking and its impact on excitonic optical properties remains elusive. In this study, we investigate a series of 2D Ruddlesden–Popper perovskites and reveal that the order–disorder transition induced by phenyl-based cations triggers a dynamic Rashba effect. At the critical temperature, we observe a reduction in exciton recombination lifetime, an increase in circularly polarized photoluminescence, and a 3-fold enhancement in polarization by constructing a van der Waals heterostructure. Theoretical calculations indicate that local inversion symmetry breaking, driven by the slight displacement of Pb atoms, is the key mechanism underlying the dynamic Rashba effect. These findings establish the dynamic Rashba effect as a critical mechanism governing exciton dynamics, offering valuable insights into advancing spintronic and optoelectronic technologies based on 2D perovskites.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"183 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703676","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":"Rotation-Symmetry Grating Contact Photodetector for Visible Full Linear Polarimetry Detection","authors":"Chunhua Wang, Chenglin He, Liang Liu, Zilan Tang, Yufan Wang, Honglin Wang, Wenqi Liu, Xiao Wang, Xiaoxia Wang, Anlian Pan","doi":"10.1021/acs.nanolett.5c00461","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00461","url":null,"abstract":"Integrated linearly polarized (LP) light detectors hold importance for next-generation optoelectronic systems. However, current compact LP photodetectors relying on the scalar anisotropic absorption of natural materials or the bipolar polarization photoresponse of artificial structures are usually unable to achieve full polarization angle detection or are restricted to the long-infrared waveband. Here, we report a photodetector by integrating InSe flakes with three-fold rotation-symmetry grating contacts for zero-bias full linear polarimetry detection. The photodetector creates an asymmetric junction interface driven by the polarization-dependent propagating surface plasmon polariton wave, generating a zero-bias bipolar polarization photoresponse. By direct measurement of the photocurrents, linear polarization angle and incident power intensity detection can be achieved in a single device at 633 nm. Moreover, we demonstrate the decoding of polarization-angle-encrypted information, showing the great potential of the proposed devices in polarization information processing. Our work offers a promising strategy for developing compact full linear polarimetry photodetectors.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"215 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703649","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}
Nano LettersPub Date : 2025-03-25DOI: 10.1021/acs.nanolett.5c00967
Chaobiao Zhou, Mimi Zhou, Zhenchu Fu, Haoxuan He, Zi-Lan Deng, Hong Xiang, Xiaoshuang Chen, Wei Lu, Guanhai Li, Dezhuan Han
{"title":"Ultrahigh-Q Quasi-BICs via Precision-Controlled Asymmetry in Dielectric Metasurfaces","authors":"Chaobiao Zhou, Mimi Zhou, Zhenchu Fu, Haoxuan He, Zi-Lan Deng, Hong Xiang, Xiaoshuang Chen, Wei Lu, Guanhai Li, Dezhuan Han","doi":"10.1021/acs.nanolett.5c00967","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00967","url":null,"abstract":"Achieving ultrahigh quality factor optical resonances is crucial for advancing low-threshold lasers, high-sensitivity sensors, and nonlinear photonics. While dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) show great potential, their experimental realization has been challenging due to the difficulty of precisely controlling symmetry-breaking at the nanoscale. Here, we introduce a precision-controlled symmetry-protected qBIC method using angular perturbations to precisely tune asymmetry, ensuring both high precision and reproducibility of Q-factors. In contrast to traditional SP-qBIC excitation, which relies on uncontrolled asymmetry, our method offers more accurate and consistent control by precisely tuning angular perturbations instead of structural variations. Additionally, our approach defines the lower limit of achievable Q-factors, providing a reliable lower bound. The experimental demonstration of SP-qBICs in composite nanoslit metasurfaces achieves a record-breaking Q-factor of 1.1 × 10<sup>5</sup>-the highest reported for SP-qBICs to date. These findings offer a promising platform for designing ultrahigh-Q resonators for next-generation photonic-applications.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"10 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703655","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}
Nano LettersPub Date : 2025-03-25DOI: 10.1021/acs.nanolett.4c04995
Jessica Kline, Shaun Gallagher, Benjamin F. Hammel, Reshma Mathew, Dylan M. Ladd, Robert J. E. Westbrook, Jalen N. Pryor, Michael F. Toney, Matthew Pelton, Sadegh Yazdi, Gordana Dukovic, David S. Ginger
{"title":"Emissive Traps Lead to Asymmetric Photoluminescence Line Shape in Spheroidal CsPbBr3 Quantum Dots","authors":"Jessica Kline, Shaun Gallagher, Benjamin F. Hammel, Reshma Mathew, Dylan M. Ladd, Robert J. E. Westbrook, Jalen N. Pryor, Michael F. Toney, Matthew Pelton, Sadegh Yazdi, Gordana Dukovic, David S. Ginger","doi":"10.1021/acs.nanolett.4c04995","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04995","url":null,"abstract":"The morphology of quantum dots plays an important role in governing their photophysics. Here, we explore the photoluminescence of spheroidal CsPbBr<sub>3</sub> quantum dots synthesized via the room-temperature trioctylphosphine oxide/PbBr<sub>2</sub> method. Despite photoluminescence quantum yields nearing 100%, these spheroidal quantum dots exhibit an elongated red photoluminescence tail not observed in typical cubic quantum dots synthesized via hot injection. We explore the origins of this elongated red tail through structural and optical characterization including small-angle X-ray scattering, transmission electron microscopy and time-resolved, steady-state, and single quantum dot photoluminescence. From these measurements we conclude that the red tail originates from emissive traps. We show that treating spheroidal quantum dots with phenethylammonium bromide decreases the line shape asymmetry and increases passivation–consistent with emissive traps due to polar facets.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"29 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695548","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}
Nano LettersPub Date : 2025-03-25DOI: 10.1021/acs.nanolett.5c00031
Mei-Tong Wei, Lu Wu, Zhi-Yi Hu, Kun-Xiao Wu, Jing-Yi Sun, Zhi-Wen Yin, Zhi-Rong Li, Xiao-Yu Yang, Yu Li, Gustaaf Van Tendeloo, Bao-Lian Su
{"title":"La Doping LiNiO2 Cathode to Immobilize the Lattice Oxygen for Highly Stable Lithium-Ion Batteries","authors":"Mei-Tong Wei, Lu Wu, Zhi-Yi Hu, Kun-Xiao Wu, Jing-Yi Sun, Zhi-Wen Yin, Zhi-Rong Li, Xiao-Yu Yang, Yu Li, Gustaaf Van Tendeloo, Bao-Lian Su","doi":"10.1021/acs.nanolett.5c00031","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00031","url":null,"abstract":"LiNiO<sub>2</sub> (LNO) with a high theoretical capacity and entirely free of cobalt has aroused much attention as a promising cathode material for lithium-ion batteries (LIBs). The rapid capacity decay, however, obstructs its commercialization. We first propose a strategy of La lattice-doping in the LNO (La-LNO) as a high-stability cathode for LIBs. Density-functional theory calculations suggest that the La dopant occupies the Ni-sites to stabilize the lattice oxygen due to a strengthening of the transition metal–oxygen bonds and mitigation of the charge compensation. La lattice-doped LNO cathode materials were fabricated successfully and had a specific capacity of 159.6 mAh g<sup>–1</sup> after 100 cycles at 1 C with a capacity retention of 94.2% and a voltage retention of 99.9%. Atomic characterization reveals that La-LNO effectively inhibits the oxygen release and phase transformation during the cycling process. Our strategy provides leading guidance for designing practical high-performance LNO cathode materials for advanced LIBs.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"16 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695549","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":"Stable Semitransparent All-Polymer Solar Cells with Color-Tunable Reflection and Neutral Transmission","authors":"Shilin Li, Linge Xiao, Hong Zhang, Yingyu Zhang, Weichao Zhang, Huiqiong Zhou, Yuan Zhang","doi":"10.1021/acs.nanolett.5c00246","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00246","url":null,"abstract":"Enhancing the stability and optical tailorability of semitransparent organic solar cells (ST-OSCs) is crucial for building-integrated photovoltaics. In this work, we propose a smart design for realizing stable and color-tunable all-polymer ST-OSCs through integrating a self-assembled MeO-2PACZ layer capped in conjunction with an optically engineered coupling structure (dielectric layer/metal/dielectric layer). Owing to the effective blocking of interfacial diffusion of metal ions, the devices with MeO-2PACZ receive considerable gains of stability, as manifested by the retention of 90% of the initial efficiency after 4000 h under storage and a retention of 82% after 600 h at maximum power point tracking. The optical coupling layer enables independent modulation of reflective properties while maintaining a high transmittance neutrality. This results in colorful ST-OSCs with a wide reflective chrominance range and a peak light utilization efficiency of 3.62%, among the best for all-polymer ST-OSCs. This strategy advances next-generation, sustainable photovoltaic windows.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"215 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695550","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}
Nano LettersPub Date : 2025-03-25DOI: 10.1021/acs.nanolett.5c00500
Nader Sawtarie, Jonathon R. Schrecengost, Krishnan Mekkanamkulam Ananthanarayanan, Nithil Harris Manimaran, Shubham Sukumar Awate, Chengye Dong, Ke Xu, Yuanxi Wang, Joshua A. Robinson, Noel C. Giebink, Susan K. Fullerton-Shirey
{"title":"Permanent Dipole Moment in a Quantum-Confined Two-Dimensional Metal Revealed by Electric Double Layer Gating","authors":"Nader Sawtarie, Jonathon R. Schrecengost, Krishnan Mekkanamkulam Ananthanarayanan, Nithil Harris Manimaran, Shubham Sukumar Awate, Chengye Dong, Ke Xu, Yuanxi Wang, Joshua A. Robinson, Noel C. Giebink, Susan K. Fullerton-Shirey","doi":"10.1021/acs.nanolett.5c00500","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00500","url":null,"abstract":"The tunable optical properties of metals through size-dependent quantum effects have attracted attention due to synthesis of chemically stable, ultrathin, and two-dimensional metals. Gate tunability, from the reduced screening of low-dimensional metals, adds an additional route for control over optical properties. Here, two-dimensional (2D) Ga is synthesized via confinement heteroepitaxy and patterned into electric-double-layer (EDL) gated transistors. 2D Ga is predicted to have an out-of-plane permanent dipole moment resulting from a non-centrosymmetric interface. Alternating current EDL gating induces a measurable change in 2D Ga reflectivity of Δ<i>R</i>/<i>R</i> ∼ 8 × 10<sup>–4</sup>. The optical response is dominated by a linear Stark shift of 1.8 meV, corresponding to a 0.4 D change in the permanent dipole moment between the ground and excited states of 2D Ga. These results are the first demonstration of 2D metal gating and the first direct evidence of a permanent dipole moment in a 2D metal.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"57 19 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695551","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}
Nano LettersPub Date : 2025-03-25DOI: 10.1021/acs.nanolett.5c00702
Marta Perxés Perich, Jan-Willem Lankman, Claudia J. Keijzer, Jessi E. S. van der Hoeven
{"title":"In Situ Gas-Phase 4D-STEM for Strain Mapping during Hydride Formation in Palladium Nanocubes","authors":"Marta Perxés Perich, Jan-Willem Lankman, Claudia J. Keijzer, Jessi E. S. van der Hoeven","doi":"10.1021/acs.nanolett.5c00702","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00702","url":null,"abstract":"The uptake and release of hydrogen are key parameters for hydrogen storage materials. Lattice strain offers a powerful way to tune hydride formation in metal nanoparticles. However, the role of strain on hydride formation is difficult to assess on a single nanoparticle level due to the lack of <i>in situ</i> characterization tools to quantify strain in the presence of a gas. Here, we achieve a dynamic, <i>in situ</i> study on the reversible hydride formation in individual palladium nanocubes by applying 4D scanning transmission electron microscopy (4D-STEM) in the presence of 1 bar H<sub>2</sub> and quantitatively assess the lattice strain with subnanometer resolution. Upon hydride formation at 125 °C, the Pd lattice expands by ∼3.1% and relaxes back upon hydrogen desorption at 200 °C. Our <i>in situ</i> 4D-STEM approach is relevant to a wide range of nanoparticle systems and applications, including catalyst- and gas-sensing materials.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"35 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695552","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}
Nano LettersPub Date : 2025-03-25DOI: 10.1021/acs.nanolett.5c00946
Nannan Zheng, Dan Li, Xin Hu, Li Yan, Ling-yun Ding, Juan Feng, Tao Ji, Shuqing He, Yudai Huang, Junqing Hu
{"title":"Enhanced Sonodynamic Cancer Therapy through Boosting Reactive Oxygen Species and Depleting Glutathione","authors":"Nannan Zheng, Dan Li, Xin Hu, Li Yan, Ling-yun Ding, Juan Feng, Tao Ji, Shuqing He, Yudai Huang, Junqing Hu","doi":"10.1021/acs.nanolett.5c00946","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00946","url":null,"abstract":"The complex tumor microenvironment (TME) affects reactive oxygen species (ROS)-based therapies; breaking the limitations of the TME to enhance the effectiveness of sonodynamic therapy (SDT) is full of great challenges. Herein, iron atomically dispersed nanoparticles (Fe–N–C) were first reported as sonosensitizers with highly efficient ROS generation by overcoming TME limitations. Its peroxidase and catalase-like activities catalyze H<sub>2</sub>O<sub>2</sub> to produce highly toxic ·OH and <i>in situ</i> O<sub>2</sub>, respectively, and then O<sub>2</sub> molecules adsorbed at Fe active sites obviously lower the energy barrier for ·OH formation. Meanwhile, its glutathione-oxidase-like activity can rapidly consume glutathione (GSH) in the TME to induce tumor cell apoptosis and ferroptosis. Density functional theory calculation results elucidate the possible mechanism of ROS generation: O<sub>2</sub> molecules are activated by receiving sonoelectrons to generate ·O<sub>2</sub><sup>–</sup>, which further reacts with H<sub>2</sub>O to produce OH<sup>–</sup>. Then OH<sup>–</sup> is oxidized by sonoholes to form ·OH. Fe–N–C displays a superior tumor specificity SDT.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"71 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695660","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":"Reconfigurable Neuromorphic Computing Using Methyl-Engineered One-Dimensional Covalent Organic Framework Memristors","authors":"Pan-Ke Zhou, Ziyue Yu, Tao Zeng, Cong Zhang, Yuxing Huang, Qian Chen, Chao Lin, Liming Zhao, Xiong Chen","doi":"10.1021/acs.nanolett.5c00890","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00890","url":null,"abstract":"The rapid evolution of neuromorphic devices seeks to bridge biological neural networks and artificial systems, enabling energy-efficient and scalable computing for next-generation artificial intelligence. Herein, we introduce methyl-engineered one-dimensional covalent organic framework (1D COF)-based memristors as a transformative platform for reconfigurable neuromorphic computing. The incorporation of methyl groups enhances localized polarization effects within the COF framework, effectively mitigating random Ag<sup>+</sup> migration/diffusion and stabilizing conductive filament morphology. This strategic modification yields devices with exceptional multilevel storage capabilities, exhibiting superior stability, linearity, and reproducibility. Moreover, the highly ordered architecture and customizable chemical environment of the methyl-functionalized 1D COF allows for precise control over resistive switching behaviors, facilitating the emulation of synaptic functions and the development of artificial neural network architectures. Demonstrating exceptional performance in neuromorphic tasks such as high-accuracy image recognition, these devices showcase significant promise as the foundation for energy-efficient, next-generation neuromorphic computing systems.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"49 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703653","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}