ACS NanoPub Date : 2024-12-10DOI: 10.1021/acsnano.4c13880
Neng Yan, Yan Wang, Tin Yan Wong, Zhiwei Wu, Xiuxiu Wang, Minwei Xie, Alessandro Parodi, Wen-Xiong Wang, Jianbo Shi
{"title":"Spatiotemporal Mapping of the Evolution of Silver Nanoparticles in Living Cells","authors":"Neng Yan, Yan Wang, Tin Yan Wong, Zhiwei Wu, Xiuxiu Wang, Minwei Xie, Alessandro Parodi, Wen-Xiong Wang, Jianbo Shi","doi":"10.1021/acsnano.4c13880","DOIUrl":"https://doi.org/10.1021/acsnano.4c13880","url":null,"abstract":"Bioaccumulated silver nanoparticles (AgNPs) can undergo transformation and release toxic Ag<sup>+</sup>, which can be further reduced and form secondary AgNPs (Ag<sup>0</sup>NPs). However, the intricate interconversions among AgNPs, Ag<sup>+</sup>, and Ag<sup>0</sup>NPs remain speculative. Herein, we developed a bioimaging method by coupling the aggregation-induced emission method with the label-free confocal scattering and hyperspectral imaging techniques to quantitatively visualize the biodistribution and biotransformation of AgNPs, Ag<sup>0</sup>NPs, and Ag<sup>+</sup> in living cells. We demonstrated that AgNPs were first dissolved in the medium, and the released Ag<sup>+</sup> was converted into Ag<sup>0</sup>NPs with the presence of algal extracellular polymeric substances and light. Under these conditions, AgNPs alone accounted for 12.4% of the total AgNP toxicity, a percentage comparable to that of Ag<sup>0</sup>NPs (15.6%). However, Ag<sup>+</sup> remained the primary contributor to overall AgNP toxicity. Additionally, we found that about 9.00% of the accumulated AgNPs within the algal cells were transformed after 24 h exposure. Of these transformed AgNPs, 4.70% remained as Ag<sup>+</sup> forms (located in the apical region, nucleus, and pyrenoid), while 4.30% persisted as Ag<sup>0</sup>NP forms (located in the cytosol) that were only detectable after a 4 h exposure. We further showed that AgNP exposure upregulated algal glutathione production with a 38.3-fold increase in glutathione reductase activity, which potentially resulted in Ag<sup>0</sup>NP formation at the active site. Overall, this study differentiated the toxicity of AgNPs, Ag<sup>+</sup>, and Ag<sup>0</sup>NPs and directly visualized the ongoing transformation and translocation of AgNPs, Ag<sup>+</sup>, and Ag<sup>0</sup>NPs within living cells, which are critical in unveiling the toxicity mechanisms of AgNPs.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"237 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797616","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}
ACS NanoPub Date : 2024-12-10Epub Date: 2024-11-01DOI: 10.1021/acsnano.4c12166
Zhilong Wang, Sixian Liu, Kehao Tao, An Chen, Hongxiao Duan, Yanqiang Han, Fengqi You, Gang Liu, Jinjin Li
{"title":"Interpretable Surrogate Learning for Electronic Material Generation.","authors":"Zhilong Wang, Sixian Liu, Kehao Tao, An Chen, Hongxiao Duan, Yanqiang Han, Fengqi You, Gang Liu, Jinjin Li","doi":"10.1021/acsnano.4c12166","DOIUrl":"10.1021/acsnano.4c12166","url":null,"abstract":"<p><p>Despite many accessible AI models that have been developed, it is an open challenge to fully exploit interpretable insights to enable effective materials design and develop materials with desired properties for target applications. Here, we introduce an interpretable surrogate learning framework that can actively design and generate electronic materials (EMGen), akin to producing updated materials with requirements by screening all possible elements and fractions. Taking the materials system with required band gaps as a case study, EMGen exhibits a benchmarking predictive error and a running time of 1.7 min for designing and producing a structure with a desired band gap. Using EMGen, we establish a large hybrid functional band gap database, and more uplifting is that the proposed EMGen effectively designs Ga<sub><i>x</i></sub>O<sub><i>y</i></sub> with a wide band gap (>5.0 eV) for deep ultraviolet (DUV) optoelectronic devices, enabling a breakthrough extension of the applicability of Ga<sub><i>x</i></sub>O<sub><i>y</i></sub> films in photodetectors to DUV light below 240 nm. The augmented band gap also helps improve the breakdown voltage and the heat resilience performance of the amorphous Ga<sub><i>x</i></sub>O<sub><i>y</i></sub> film, thereby achieving considerable potential within the realm of power electronics applications. The proposed EMGen, as a specialized, interpretable AI model for the generation of electronic materials, is demonstrated to be an essential tool for on-demand semiconductor materials design.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":"33587-33601"},"PeriodicalIF":15.8,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556570","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}
ACS NanoPub Date : 2024-12-10DOI: 10.1021/acsnano.4c06030
Tiffany W. Leong, Zhenghong Gao, Eric T. David, Xiaoqing Li, Qi Cai, Juliet M. Mwirigi, Tingting Zhang, Monica Giannotta, Elisabetta Dejana, John Wiggins, Sharada Krishnagiri, Robert M. Bachoo, Xiaoqian Ge, Theodore J. Price, Zhenpeng Qin
{"title":"Spatially Precise and Minimally Invasive Delivery of Peptides to the Spinal Cord for Behavior Modulation","authors":"Tiffany W. Leong, Zhenghong Gao, Eric T. David, Xiaoqing Li, Qi Cai, Juliet M. Mwirigi, Tingting Zhang, Monica Giannotta, Elisabetta Dejana, John Wiggins, Sharada Krishnagiri, Robert M. Bachoo, Xiaoqian Ge, Theodore J. Price, Zhenpeng Qin","doi":"10.1021/acsnano.4c06030","DOIUrl":"https://doi.org/10.1021/acsnano.4c06030","url":null,"abstract":"The blood–spinal cord barrier (BSCB) tightly regulates the transport of molecules from the blood to the spinal cord. Herein, we present an approach for transient modulation of BSCB permeability and localized delivery of peptides into the spinal cord for behavior modulation with high spatial resolution. This approach utilizes optical stimulation of vasculature-targeted nanoparticles and allows delivery of BSCB-impermeable molecules into the spinal cord without significant glial activation or impact on animal locomotor behavior. We demonstrate minimally invasive light delivery into the spinal cord using an optical fiber and BSCB permeability modulation in the lumbar region. Our method of BSCB modulation allows the delivery of bombesin, a centrally acting and itch-inducing peptide, into the spinal cord and induces a rapid and transient increase in itching behaviors in mice. This minimally invasive approach enables behavior modulation without genetic modifications and is promising for delivering a wide range of biologics into the spinal cord for potential therapy with high spatiotemporal resolution.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"21 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797613","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":"Large-Area Aligned Growth of Low-Symmetry 2D ReS2 on a High-Symmetry Surface","authors":"Honglin Chen, Shan Jiang, Lingli Huang, Ping Man, Qingming Deng, Jiong Zhao, Thuc Hue Ly","doi":"10.1021/acsnano.4c14162","DOIUrl":"https://doi.org/10.1021/acsnano.4c14162","url":null,"abstract":"The large-scale preparation of two-dimensional (2D) materials is pivotal in unlocking their extensive potential for next-generation semiconductor device applications. Wafer-scale single crystals of a high-symmetry 2D material (e.g., graphene and molybdenum disulfide) can be achieved by seamlessly stitching the aligned domains. However, achieving the alignment of low-symmetry 2D materials remains a great challenge and is rarely reported. Rhenium disulfide (ReS<sub>2</sub>), one of the low-symmetry 2D materials, shows considerable promise for optoelectronics, especially polarization-sensitive applications. Here, we report large-area chemical vapor deposition synthesis of highly oriented, low-symmetry monolayer ReS<sub>2</sub> flakes on a high-symmetry Au(111) surface, followed by seamless stitching into a centimeter-scale continuous 2D film. Cross-sectional scanning transmission electron microscopy reveals that the aligned monolayer ReS<sub>2</sub> flakes are guided by step edges on Au(111) surfaces along the [011̅] direction. Additionally, 2D ReS<sub>2</sub> can flatten Au surfaces during its growth through surface step bunching. The growth of the ReS<sub>2</sub> monolayer demonstrates its ability to extend across Au surface steps and facets. Thus, we have established a reliable and robust synthesis route that accommodates different surface roughness conditions. The aligned and scalable film growth of low-symmetry 2D ReS<sub>2</sub> significantly contributes to the in-depth understanding of epitaxial growth mechanisms for low-symmetry 2D materials, holding promise for advancing their future applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"77 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805194","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}
ACS NanoPub Date : 2024-12-10DOI: 10.1021/acsnano.4c10274
Jingfeng Wang, Xiaoming Zhang, Ruichen Shen, Quan Yuan, Yanbing Yang
{"title":"Staggered-Stacking Two-Dimensional Covalent Organic Framework Membranes for Molecular and Ionic Sieving","authors":"Jingfeng Wang, Xiaoming Zhang, Ruichen Shen, Quan Yuan, Yanbing Yang","doi":"10.1021/acsnano.4c10274","DOIUrl":"https://doi.org/10.1021/acsnano.4c10274","url":null,"abstract":"Two-dimensional covalent organic frameworks (2D COFs), a family of crystalline materials with abundant porous structures offering nanochannels for molecular transport, have enormous potential in the applications of separation, energy storage, and catalysis. However, 2D COFs remain limited by relatively large pore sizes (>1 nm) and weak interlayer interactions between 2D nanosheets, making it difficult to achieve efficient membranes to meet the selective sieving requirements for water molecules (0.3 nm) and hydrated salt ions (>0.7 nm). Here, we report a high-performance 2D COF membrane with narrowed channels (0.7 × 0.4 nm<sup>2</sup>) and excellent mechanical performance constructed by the staggered stacking of cationic and anionic 2D COF nanosheets for selectively sieving of water molecules and hydrated salt ions. The mechanical performance has been improved by two times than that of single-phase 2D COF membranes due to the enhanced interlayer interactions between nanosheets. The stacked 2D COF membranes exhibit significantly improved monovalent salt ions rejection ratio (up to 77.9%) compared with single-phase COF membranes (∼49.2%), while maintaining comparable water permeability. The design of stacked 2D COF membranes provides a potential strategy for constructing high-performance nanoporous membranes to achieve precise molecular and ionic sieving.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805123","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}
ACS NanoPub Date : 2024-12-09DOI: 10.1021/acsnano.4c11724
Nivetha Gunaseelan, Pranay Saha, Nada Maher, Dipanjan Pan
{"title":"Nanoparticles with “K-edge” Metals Bring “Color” in Multiscale Spectral Photon Counting X-ray Imaging","authors":"Nivetha Gunaseelan, Pranay Saha, Nada Maher, Dipanjan Pan","doi":"10.1021/acsnano.4c11724","DOIUrl":"https://doi.org/10.1021/acsnano.4c11724","url":null,"abstract":"Preclinical and clinical diagnostics depend greatly on medical imaging, which enables the identification of physiological and pathological processes in living subjects. It is often necessary to use contrast agents to complement anatomical data with functional information or to describe the disease phenotypically. Nanomaterials are used as contrast agents in many advanced bioimaging techniques and applications because of their high payload, physicochemical properties, improved sensitivity, and multimodality. Metals with k-edge energy within the X-ray bandwidth respond to photon counting and spectral X-ray imaging. This Perspective examines the progress made in the emerging area of nanoparticle-based k-edge contrast agents. These nano <i>“k-edge”</i> particles have been explored with spectral photon counting CT (SPCCT) for multiplexed molecular imaging, pushing the boundaries of resolution and capabilities of CT imaging. Design considerations, contrast properties, and biological behavior are discussed in detail. The key applications are highlighted by categorizing these nanomaterials based on their X-ray, k-edge energy, and biological properties, as well as their synthesis, functionalization, and characterization processes. The article delves into the transformative impact of nano “<i>k-edge</i>” particles on early disease detection and other biomedical applications. The review provides further insights into how the “k-edge signatures” of these nanoparticles combined with photon counting technique can be leveraged for quantitative, multicontrast imaging of diseases. We also discuss the status quo of clinically approved nanoparticles for imaging and highlight the challenges such as toxicity and clearance as well as promising clinical perspectives, providing a balanced view of the potential and limitations of these nanomaterials. Furthermore, we discuss the necessary future research efforts required to clinically translate nano “<i>k-edge</i>” particles as SPCCT contrast agents for early disease diagnosis and tracking.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"28 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797673","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}
ACS NanoPub Date : 2024-12-09DOI: 10.1021/acsnano.4c12502
Suo Tu, Ting Tian, Jinsheng Zhang, Suzhe Liang, Guangjiu Pan, Xiaoxin Ma, Liangzhen Liu, Roland A. Fischer, Peter Müller-Buschbaum
{"title":"Electrostatic Tailoring of Freestanding Polymeric Films for Multifunctional Thermoelectrics, Hydrogels, and Actuators","authors":"Suo Tu, Ting Tian, Jinsheng Zhang, Suzhe Liang, Guangjiu Pan, Xiaoxin Ma, Liangzhen Liu, Roland A. Fischer, Peter Müller-Buschbaum","doi":"10.1021/acsnano.4c12502","DOIUrl":"https://doi.org/10.1021/acsnano.4c12502","url":null,"abstract":"Organic conducting polymer poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) has garnered enormous attention in organic electronics due to its low-cost solution processability, highly tunable conductivity, superior mechanical flexibility, and good biocompatibility together with excellent atmospheric stability. Nevertheless, limited electrical properties and unfavorable water instability of pristine PEDOT:PSS film impede its further implementation in a broad spectrum of practical applications. In this work, the successful tailoring of the intrinsic electrostatic interaction within PEDOT:PSS and consequent optimized electrical properties are enabled by a simple yet effective ionic salt post-treatment strategy. The choice of zinc di[bis(trifluoromethylsulfonyl)imide] (Zn(TFSI)<sub>2</sub>) not only endows the post-treated PEDOT:PSS film with high electrical properties but also other compelling characteristics, including superior water stability, excellent mechanical flexibility, and fast humidity responsiveness. Multidimensional characterizations are conducted to gain in-depth insights into the mechanisms underlying such improved performance, ranging from intermolecular interactions, polymer conformations, and doping levels to microstructural characteristics. Benefiting from these versatile properties, the as-prepared freestanding Zn(TFSI)<sub>2</sub>-post-treated PEDOT:PSS films can serve as promising candidates for high-performance polymeric materials integrated into multifunctional flexible electronics, including thermoelectric power generators, conductive hydrogels, and humidity-responsive actuators. This study demonstrates a facile methodology for the exploration of multifunctional conducting polymers, whose implications can extend across a wide range of next-generation wearable devices, bioelectronics, and soft robotics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"96 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797674","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}
ACS NanoPub Date : 2024-12-09DOI: 10.1021/acsnano.4c12814
Jiafan Qu, Yadong Wei, Liang Zhao, Ruoxi Tan, Weiqi Li, Hongyan Shi, Yueling Zhang, Jianqun Yang, Bo Gao, Xingji Li
{"title":"Defect-Mediated Exciton Localization and Relaxation in Monolayer MoS2","authors":"Jiafan Qu, Yadong Wei, Liang Zhao, Ruoxi Tan, Weiqi Li, Hongyan Shi, Yueling Zhang, Jianqun Yang, Bo Gao, Xingji Li","doi":"10.1021/acsnano.4c12814","DOIUrl":"https://doi.org/10.1021/acsnano.4c12814","url":null,"abstract":"Defects in chemical vapor deposition (CVD)-grown monolayer MoS<sub>2</sub> are unavoidable and provide a powerful approach to creating single-photon emitters and quantum information systems through localizing excitons. However, insight into the A<sup>–</sup> trion and B/C exciton localization in monolayer MoS<sub>2</sub> remains elusive. Here, we investigate defect-mediated A<sup>–</sup> trion and B/C exciton localization and relaxation in CVD-grown monolayer MoS<sub>2</sub> samples via transient absorption spectroscopy. The localization rate of A<sup>–</sup> trions is five times faster than B excitons, which is attributed to the distinctions in the Bohr radius, diffusion rate, and multiphonon emission. Furthermore, we obtain unambiguous experimental evidence for the direct excitation of localized C excitons. Varying gap energy at the band-nesting region revealed by first-principles calculations explains the anomalous dependence of localized C exciton energy on delay time. We also find that the rapid dissociation of localized C excitons features a short characteristic time of ∼0.14 ps, while the measured relaxation time is much longer. Our results provide a comprehensive picture of the defect-mediated excitonic relaxation and localization dynamics in monolayer MoS<sub>2</sub>.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"26 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793535","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":"Biomimetic Extracellular Vesicles Based on Composite Bioactive Ions for the Treatment of Ischemic Bone Disease","authors":"Hongyi Jiang, Xinyi Zhu, Jiachen Yu, Weidan Wang, Yiwen Mao, Liting Jiang, Liang Zhu, Hanting Shen, Chao Lou, Chihao Lin, Zhongnan Lin, Zijian Yan, Yumeng Wang, Jilong Wang, Xinghe Xue, Xiaoyun Pan","doi":"10.1021/acsnano.4c13028","DOIUrl":"https://doi.org/10.1021/acsnano.4c13028","url":null,"abstract":"Extracellular vesicles (EVs) have demonstrated considerable potential in the treatment of ischemic bone diseases, such as glucocorticoid-induced osteonecrosis of the femoral head (GIONFH). However, the clinical application of EVs faces challenges such as low yield, poor bioactivity, and lack of targeting. Herein, we have developed a platform of multiengineered extracellular vesicle mimetics (EVMs) to address these challenges. By stimulating mesenchymal stem cells (MSCs) with multibioactive ions from TS (Trisilicate, a mixture of calcium silicate, magnesium silicate, and strontium silicate), we obtained endogenously modified TS-MSCs. From these, we further prepared a large quantity of bioactive EVM<sub>TS-MSCs</sub> through a straightforward extrusion method. Moreover, by integrating metabolic glycoengineering with click chemistry strategies, alendronate (ALN) was surface-modified on EVM<sub>TS-MSCs</sub> to further prepare ALN-EVM<sub>TS-MSCs</sub>. The engineered ALN-EVM<sub>TS-MSCs</sub> demonstrated bone-targeting effects, promoting osteogenesis and angiogenesis. This promoting effect is attributed to the rich presence of miR-21 in the TS-modified EVM, which further silences PTEN to activate the PI3K/AKT signaling pathway, thereby enhancing osteogenesis and angiogenesis. Our treatment strategy for ischemic bone diseases is based on a multiengineered, biomaterial-inspired, metabolic glycoengineering, and click chemistry-based platform of EVM. This study also provides an enhanced understanding of the development and application of engineered vesicles in disease treatment.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"21 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797618","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}
ACS NanoPub Date : 2024-12-09DOI: 10.1021/acsnano.4c12532
Saúl A. Herrera, Guillermo Parra-Martínez, Philipp Rosenzweig, Bharti Matta, Craig M. Polley, Kathrin Küster, Ulrich Starke, Francisco Guinea, José Ángel Silva-Guillén, Gerardo G. Naumis, Pierre A. Pantaleón
{"title":"Topological Superconductivity in Heavily Doped Single-Layer Graphene","authors":"Saúl A. Herrera, Guillermo Parra-Martínez, Philipp Rosenzweig, Bharti Matta, Craig M. Polley, Kathrin Küster, Ulrich Starke, Francisco Guinea, José Ángel Silva-Guillén, Gerardo G. Naumis, Pierre A. Pantaleón","doi":"10.1021/acsnano.4c12532","DOIUrl":"https://doi.org/10.1021/acsnano.4c12532","url":null,"abstract":"The existence of superconductivity (SC) appears to be established in both twisted and nontwisted graphene multilayers. However, whether their building block, single-layer graphene (SLG), can also host SC remains an open question. Earlier theoretical works predicted that SLG could become a chiral <i>d</i>-wave superconductor driven by electronic interactions when doped to its van Hove singularity, but questions such as whether the <i>d</i>-wave SC survives the strong band renormalizations seen in experiments, its robustness against the source of doping, or if it will occur at any reasonable critical temperature (<i>T</i><sub>c</sub>) have remained difficult to answer, in part due to uncertainties in model parameters. Furthermore, doping of graphene beyond its van Hove singularity remained experimentally challenging and was not demonstrated until recently. In this study, we <i>n</i> dope SLG past the van Hove singularity by employing Tb intercalation and derive structural models from angle-resolved photoemission spectroscopy measurements. We adopt a reliable numerical framework based on a random-phase approximation technique to investigate the emergence of unconventional SC in the heavily doped monolayer. We predict that robust <i>d</i> + <i>id</i> topological SC could arise in SLG doped by Tb, with a <i>T</i><sub>c</sub> up to 600 mK. We also employ first-principles calculations to investigate the possibility of realizing <i>d</i>-wave SC with other dopants, such as Li or Cs. We find that dopants that change the lattice symmetry of SLG are detrimental to the <i>d</i>-wave state. The stability of the <i>d</i>-wave SC predicted here in Tb-doped SLG could provide a valuable insight for guiding future experimental efforts aimed at exploring topological superconductivity in monolayer graphene.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"20 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797675","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}