ACS Nanoscience Au最新文献

{"title":"Acoustically Powered Nano- and Microswimmers: From Individual to Collective Behavior","authors":"Jeffrey M. McNeill,&nbsp; and ,&nbsp;Thomas E. Mallouk*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00038","DOIUrl":"10.1021/acsnanoscienceau.3c00038","url":null,"abstract":"<p >Micro- and nanoscopic particles that swim autonomously and self-assemble under the influence of chemical fuels and external fields show promise for realizing systems capable of carrying out large-scale, predetermined tasks. Different behaviors can be realized by tuning swimmer interactions at the individual level in a manner analogous to the emergent collective behavior of bacteria and mammalian cells. However, the limited toolbox of weak forces with which to drive these systems has made it difficult to achieve useful collective functions. Here, we review recent research on driving swimming and particle self-organization using acoustic fields, which offers capabilities complementary to those of the other methods used to power microswimmers. With either chemical or acoustic propulsion (or a combination of the two), understanding individual swimming mechanisms and the forces that arise between individual particles is a prerequisite to harnessing their interactions to realize collective phenomena and macroscopic functionality. We discuss here the ingredients necessary to drive the motion of microscopic particles using ultrasound, the theory that describes that behavior, and the gaps in our understanding. We then cover the combination of acoustically powered systems with other cross-compatible driving forces and the use of ultrasound in generating collective behavior. Finally, we highlight the demonstrated applications of acoustically powered microswimmers, and we offer a perspective on the state of the field, open questions, and opportunities. We hope that this review will serve as a guide to students beginning their work in this area and motivate others to consider research in microswimmers and acoustic fields.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 6","pages":"424–440"},"PeriodicalIF":0.0,"publicationDate":"2023-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135800520","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hafnium, Titanium, and Zirconium Intercalation in 2D Layered Nanomaterials","authors":"Vicky Huynh,&nbsp;Kevin Rodriguez Rivera,&nbsp;Tiffany Teoh,&nbsp;Ethan Chen,&nbsp;Jared Ura and Kristie J. Koski*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00027","DOIUrl":"10.1021/acsnanoscienceau.3c00027","url":null,"abstract":"<p >Altering the physical and chemical properties of a layered material through intercalation has emerged as a unique strategy toward tunable applications. In this work, we demonstrate a wet chemical method to intercalate titanium, hafnium, and zirconium into 2D layered nanomaterials. The metals are intercalated using bis-tetrahydrofuran metal halide complexes. Metal intercalation is demonstrated in nanomaterials of Bi₂Se₃, Si₂Te₃, MoO₃, and GeS. This strategy intercalates, on average, 3 atm % or less of Hf, Ti, and Zr that share charge with the host nanomaterial. This methodology is used to chemochromically alter MoO₃ from transparent white to dark blue.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 6","pages":"475–481"},"PeriodicalIF":0.0,"publicationDate":"2023-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00027","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136130292","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Quantum Diamonds at the Beach: Chemical Insights into Silica Growth on Nanoscale Diamond using Multimodal Characterization and Simulation","authors":"Perla J. Sandoval,&nbsp;Karen Lopez,&nbsp;Andres Arreola,&nbsp;Anida Len,&nbsp;Nedah Basravi,&nbsp;Pomaikaimaikalani Yamaguchi,&nbsp;Rina Kawamura,&nbsp;Camron X. Stokes,&nbsp;Cynthia Melendrez,&nbsp;Davida Simpson,&nbsp;Sang-Jun Lee,&nbsp;Charles James Titus,&nbsp;Virginia Altoe,&nbsp;Sami Sainio,&nbsp;Dennis Nordlund,&nbsp;Kent Irwin and Abraham Wolcott*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00033","DOIUrl":"10.1021/acsnanoscienceau.3c00033","url":null,"abstract":"<p >Surface chemistry of materials that host quantum bits such as diamond is an important avenue of exploration as quantum computation and quantum sensing platforms mature. Interfacing diamond in general and nanoscale diamond (ND) in particular with silica is a potential route to integrate room temperature quantum bits into photonic devices, fiber optics, cells, or tissues with flexible functionalization chemistry. While silica growth on ND cores has been used successfully for quantum sensing and biolabeling, the surface mechanism to initiate growth was unknown. This report describes the surface chemistry responsible for silica bond formation on diamond and uses X-ray absorption spectroscopy (XAS) to probe the diamond surface chemistry and its electronic structure with increasing silica thickness. A modified Stöber (Cigler) method was used to synthesize 2–35 nm thick shells of SiO₂ onto carboxylic acid-rich ND cores. The diamond morphology, surface, and electronic structure were characterized by overlapping techniques including electron microscopy. Importantly, we discovered that SiO₂ growth on carboxylated NDs eliminates the presence of carboxylic acids and that basic ethanolic solutions convert the ND surface to an alcohol-rich surface prior to silica growth. The data supports a mechanism that alcohols on the ND surface generate silyl–ether (ND–O–Si–(OH)₃) bonds due to rehydroxylation by ammonium hydroxide in ethanol. The suppression of the diamond electronic structure as a function of SiO₂ thickness was observed for the first time, and a maximum probing depth of ∼14 nm was calculated. XAS spectra based on the Auger electron escape depth was modeled using the NIST database for the Simulation of Electron Spectra for Surface Analysis (SESSA) to support our experimental results. Additionally, resonant inelastic X-ray scattering (RIXS) maps produced by the transition edge sensor reinforces the chemical analysis provided by XAS. Researchers using diamond or high-pressure high temperature (HPHT) NDs and other exotic materials (e.g., silicon carbide or cubic-boron nitride) for quantum sensing applications may exploit these results to design new layered or core–shell quantum sensors by forming covalent bonds via surface alcohol groups.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 6","pages":"462–474"},"PeriodicalIF":0.0,"publicationDate":"2023-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135394487","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Using the Photoluminescence Color Change in Cesium Lead Iodide Nanoparticles to Monitor the Kinetics of an External Organohalide Chemical Reaction by Halide Exchange","authors":"Tennyson L. Doane,&nbsp;Kevin J. Cruz,&nbsp;Tsung-Hsing Chiang and Mathew M. Maye*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00026","DOIUrl":"10.1021/acsnanoscienceau.3c00026","url":null,"abstract":"<p >In this work, we demonstrate a photoluminescence-based method to monitor the kinetics of an organohalide reaction by way of detecting released bromide ions at cesium lead halide nanoparticles. Small aliquots of the reaction are added to an assay with known concentrations of CsPbI₃, and the resulting Br-to-I halide exchange (HE) results in rapid and sensitive wavelength blueshifts (Δλ) due to CsPbBr_<i>x</i>I_3<i>–x</i> intermediate concentrations, the wavelengths of which are proportional to concentrations. An assay response factor, <i>C</i>, relates Δλ to Br^– concentration as a function of CsPbI₃ concentration. The observed kinetics, as well as calculated rate constants, equilibrium, and activation energy of the solvolysis reaction tested correspond closely to synthetic literature values, validating the assay. Factors that influence the sensitivity and performance of the assay, such as CsPbI₃ size, morphology, and concentration, are discussed.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 5","pages":"418–423"},"PeriodicalIF":0.0,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00026","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44027656","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced Charge Transfer from Coinage Metal Doped InP Quantum Dots","authors":"Forrest W. Eagle,&nbsp;Samantha Harvey,&nbsp;Ryan Beck,&nbsp;Xiaosong Li,&nbsp;Daniel R. Gamelin and Brandi M. Cossairt*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00029","DOIUrl":"10.1021/acsnanoscienceau.3c00029","url":null,"abstract":"<p >This paper describes coinage-metal-doped InP quantum dots (QDs) as a platform for enhanced electron transfer to molecular acceptors relative to undoped QDs. A synthetic strategy is developed to prepare doped InP/ZnSe QDs. First-principles DFT calculations show that Ag⁺ and Cu⁺ dopants localize photoexcited holes while leaving electrons delocalized. This charge carrier wave function modulation is leveraged to enhance electron transfer to molecular acceptors by up to an order of magnitude. Examination of photoluminescence quenching data suggests that larger electron acceptors, such as anthraquinone and methyl viologen, bind to the QD surface in two ways: by direct adsorption to the surface and by adsorption following displacement of a weakly bound surface cation-ligand complex. Reactions with larger acceptors show the greatest increases in electron transfer between doped and undoped quantum dots, while smaller acceptors show smaller enhancements. Specifically, benzoquinone shows the smallest, followed by naphthoquinone and then methyl viologen and anthraquinone. These results demonstrate the benefits of dopant-induced excited-state carrier localization on photoinduced charge transfer and highlight design principles for improved implementation of quantum dots in photoredox catalysis.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 6","pages":"451–461"},"PeriodicalIF":0.0,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00029","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49179002","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Using 19F NMR to Investigate Cationic Carbon Dot Association with Per- and Polyfluoroalkyl Substances (PFAS)","authors":"Riley E. Lewis,&nbsp;Cheng-Hsin Huang,&nbsp;Jason C. White and Christy L. Haynes*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00022","DOIUrl":"10.1021/acsnanoscienceau.3c00022","url":null,"abstract":"<p >There is much concern about per- and polyfluoroalkyl substances (PFAS) based on their environmental persistence and toxicity, resulting in an urgent need for remediation technologies. This study focused on determining if nanoscale polymeric carbon dots are a viable sorbent material for PFAS and developing fluorine nuclear magnetic resonance spectroscopy (¹⁹F NMR) methods to probe interactions between carbon dots and PFAS at the molecular scale. Positively charged carbon dots (PEI-CDs) were synthesized using branched polyethyleneimine to target anionic PFAS by promoting electrostatic interactions. PEI-CDs were exposed to perfluorooctanoic acid (PFOA) to assess their potential as a PFAS sorbent material. After exposure to PFOA, the average size of the PEI-CDs increased (1.6 ± 0.5 to 7.8 ± 1.8 nm) and the surface charge decreased (+38.6 ± 1.1 to +26.4 ± 0.8 mV), both of which are consistent with contaminant sorption. ¹⁹F NMR methods were developed to gain further insight into PEI-CD affinity toward PFAS without any complex sample preparation. Changes in PFOA peak intensity and chemical shift were monitored at various PEI-CD concentrations to establish binding curves and determine the chemical exchange regime. ¹⁹F NMR spectral analysis indicates slow-intermediate chemical exchange between PFOA and CDs, demonstrating a high-affinity interaction. The α-fluorine had the greatest change in chemical shift and highest affinity, suggesting electrostatic interactions are the dominant sorption mechanism. PEI-CDs demonstrated affinity for a wide range of analytes when exposed to a mixture of 24-PFAS, with a slight preference toward perfluoroalkyl sulfonates. Overall, this study shows that PEI-CDs are an effective PFAS sorbent material and establishes ¹⁹F NMR as a suitable method to screen for novel sorbent materials and elucidate interaction mechanisms.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 5","pages":"408–417"},"PeriodicalIF":0.0,"publicationDate":"2023-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00022","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"42177832","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Controlling Morphology and Excitonic Disorder in Monolayer WSe2 Grown by Salt-Assisted CVD Methods","authors":"Reynolds Dziobek-Garrett,&nbsp;Sachi Hilliard,&nbsp;Shreya Sriramineni,&nbsp;Ona Ambrozaite,&nbsp;Yifei Zhu,&nbsp;Bethany M. Hudak,&nbsp;Todd H. Brintlinger,&nbsp;Tomojit Chowdhury and Thomas J. Kempa*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00028","DOIUrl":"10.1021/acsnanoscienceau.3c00028","url":null,"abstract":"<p >Chemical synthesis is a compelling alternative to top-down fabrication for controlling the size, shape, and composition of two-dimensional (2D) crystals. Precision tuning of the 2D crystal structure has broad implications for the discovery of new phenomena and the reliable implementation of these materials in optoelectronic, photovoltaic, and quantum devices. However, precise and predictable manipulation of the edge structure in 2D crystals through gas-phase synthesis is still a formidable challenge. Here, we demonstrate a salt-assisted low-pressure chemical vapor deposition method that enables tuning W metal flux during growth of 2D WSe₂ monolayers and, thereby, direct control of their edge structure and optical properties. The degree of structural disorder in 2D WSe₂ is a direct function of the W metal flux, which is controlled by adjusting the mass ratio of WO₃ to NaCl. This edge disorder then couples to excitonic disorder, which manifests as broadened and spatially varying emission profiles. Our work links synthetic parameters with analyses of material morphology and optical properties to provide a unified understanding of intrinsic limits and opportunities in synthetic 2D materials.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 6","pages":"441–450"},"PeriodicalIF":0.0,"publicationDate":"2023-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00028","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"45309423","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The Artistic Side of ACS Nanoscience Au: Our Cover Art Collection and Tips for Authors","authors":"Amelia Newman,&nbsp; and ,&nbsp;Raymond E. Schaak*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00034","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.3c00034","url":null,"abstract":"","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 4","pages":"266–268"},"PeriodicalIF":0.0,"publicationDate":"2023-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00034","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49768020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Two-Dimensional Electrically Conductive Metal–Organic Frameworks as Chemiresistive Sensors","authors":"Chungseong Park,&nbsp;Jong Won Baek,&nbsp;Euichul Shin and Il-Doo Kim*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00024","DOIUrl":"10.1021/acsnanoscienceau.3c00024","url":null,"abstract":"<p >Metal–organic frameworks (MOFs) have emerged as attractive chemical sensing materials due to their exceptionally high porosity and chemical diversity. Nevertheless, the utilization of MOFs in chemiresistive type sensors has been hindered by their inherent limitation in electrical conductivity. The recent emergence of two-dimensional conductive MOFs (2D c-MOFs) has addressed this limitation by offering enhanced electrical conductivity, while still retaining the advantageous properties of MOFs. In particular, c-MOFs have shown promising advantages for the fabrication of sensors capable of operating at room temperature. Thus, active research on gas sensors utilizing c-MOFs is currently underway, focusing on enhancing sensitivity and selectivity. To comprehend the potential of MOFs as chemiresistive sensors for future applications, it is crucial to understand not only the fundamental properties of conductive MOFs but also the state-of-the-art works that contribute to improving their performance. This comprehensive review delves into the distinctive characteristics of 2D c-MOFs as a new class of chemiresistors, providing in-depth insights into their unique sensing properties. Furthermore, we discuss the proposed sensing mechanisms associated with 2D c-MOFs and provide a concise summary of the strategies employed to enhance the sensing performance of 2D c-MOFs. These strategies encompass a range of approaches, including the design of metal nodes and linkers, morphology control, and the synergistic use of composite materials. In addition, the review thoroughly explores the prospects of 2D c-MOFs as chemiresistors and elucidates their remarkable potential for further advancements. The insights presented in this review shed light on future directions and offer valuable opportunities in the chemical sensing research field.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 5","pages":"353–374"},"PeriodicalIF":0.0,"publicationDate":"2023-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00024","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"45784864","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"UTILE-Gen: Automated Image Analysis in Nanoscience Using Synthetic Dataset Generator and Deep Learning","authors":"André Colliard-Granero*,&nbsp;Jenia Jitsev,&nbsp;Michael H. Eikerling,&nbsp;Kourosh Malek and Mohammad J. Eslamibidgoli*,&nbsp;","doi":"10.1021/acsnanoscienceau.3c00020","DOIUrl":"10.1021/acsnanoscienceau.3c00020","url":null,"abstract":"<p >This work presents the development and implementation of a deep learning-based workflow for autonomous image analysis in nanoscience. A versatile, agnostic, and configurable tool was developed to generate instance-segmented imaging datasets of nanoparticles. The synthetic generator tool employs domain randomization to expand the image/mask pairs dataset for training supervised deep learning models. The approach eliminates tedious manual annotation and allows training of high-performance models for microscopy image analysis based on convolutional neural networks. We demonstrate how the expanded training set can significantly improve the performance of the classification and instance segmentation models for a variety of nanoparticle shapes, ranging from spherical-, cubic-, to rod-shaped nanoparticles. Finally, the trained models were deployed in a cloud-based analytics platform for the autonomous particle analysis of microscopy images.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"3 5","pages":"398–407"},"PeriodicalIF":0.0,"publicationDate":"2023-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.3c00020","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43673018","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}