ACS Materials AuPub Date : 2024-10-31eCollection Date: 2024-11-13DOI: 10.1021/acsmaterialsau.4c00103
Priscila Alessio, Milene K C da Silva, Vitoria Barossi, Celina M Miyazaki
{"title":"Nanostructured Thin Films Enhancing the Performance of New Organic Electronic Devices: Does It Make Sense?","authors":"Priscila Alessio, Milene K C da Silva, Vitoria Barossi, Celina M Miyazaki","doi":"10.1021/acsmaterialsau.4c00103","DOIUrl":"10.1021/acsmaterialsau.4c00103","url":null,"abstract":"<p><p>Electronics have evolved significantly with the development of semiconductor materials and devices, with emerging areas such as organic and flexible electronics showing great promise, particularly in applications such as wearable devices and environmental sensors. Since the discovery of conducting polymers in the late 1970s, organic electronics have paved the way for innovations such as organic field-effect transistors (OFETs), organic light-emitting diodes (OLEDs), and organic solar cells (OPVs). Recent advances have focused on nanostructuring techniques to enhance device properties, such as charge mobility and luminescence efficiency. The growing concern for sustainability has also led to the exploration of biodegradable organic electronics as a potential solution to electronic waste. This perspective briefly discusses the impact of nanostructuring on the performance of both conventional and biodegradable organic devices, exploring the challenges and opportunities associated with using alternative substrates like paper. This perspective emphasizes the importance of understanding molecular organization at the nanoscale to optimize device performance and ensure stability under practical conditions.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 6","pages":"574-581"},"PeriodicalIF":5.7,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11565282/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142649105","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":"Understanding Defect-Mediated Ion Migration in Semiconductors using Atomistic Simulations and Machine Learning.","authors":"Md Habibur Rahman, Maitreyo Biswas, Arun Mannodi-Kanakkithodi","doi":"10.1021/acsmaterialsau.4c00095","DOIUrl":"10.1021/acsmaterialsau.4c00095","url":null,"abstract":"<p><p>Ion migration in semiconductor devices is facilitated by the presence of point defects and has a major influence on electronic and optical properties. It is important to understand and identify ways to mitigate photoinduced and electrically induced defect-mediated ion migration in semiconductors. In this Perspective, we discuss the fundamental mechanisms of defect-mediated ion migration and diffusion as understood through atomistic simulations. The discussion covers a variety of case studies from the literature, with a special focus on metal halide perovskites, important materials for solar absorption and related optoelectronic applications. Tuning the perovskite composition and dimensionality and applying systematic strains are identified as ways to suppress phase segregation and ion migration. This Perspective delves into first-principles modeling approaches for defect migration and diffusion, presenting detailed case studies on the diffusion of defects and dopants in CdTe, hydrogen impurities in halide perovskites, and halogen migration in hybrid perovskites and emphasizing the importance of organic cations. The discussion further extends to accelerating the prediction of migration pathways and barriers through machine learning approaches, particularly the application of crystal-graph neural networks. By combining theoretical insights with practical case studies, this Perspective aims to provide an understanding of defect-mediated ion migration and suggestions for next-generation semiconductor discovery while considering ion migration suppression as one of many design objectives.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 6","pages":"557-573"},"PeriodicalIF":5.7,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11565286/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142649109","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":"High-Entropy Alloys in Catalysis: Progress, Challenges, and Prospects.","authors":"Liang Sun, Kaihua Wen, Guanjie Li, Xindan Zhang, Xiaohui Zeng, Bernt Johannessen, Shilin Zhang","doi":"10.1021/acsmaterialsau.4c00080","DOIUrl":"10.1021/acsmaterialsau.4c00080","url":null,"abstract":"<p><p>High-entropy alloys (HEAs) have become pivotal materials in the field of catalysis, offering unique advantages due to their diverse elemental compositions and complex atomic structures. Recent advances in computational techniques, particularly density functional theory (DFT) and machine learning (ML), have significantly enhanced our understanding and design of HEAs for use in catalysis. These innovative atomistic simulations shed light on the properties of HEAs, enabling the discovery and optimization of catalysis materials for solid-solution structures. This Perspective discusses recent studies that illustrate the progress of HEAs in catalysis. It offers an overview of the properties, constraints, and prospects of HEAs, emphasizing their roles in catalysis to enhance catalytic activity and selectivity. The discussion underscores the capabilities of HEAs as multifunctional catalysts with stable structures. The presented insights aim to inspire future computational and experimental efforts to address the challenges in fine-tuning HEAs properties for improved catalytic performance.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 6","pages":"547-556"},"PeriodicalIF":5.7,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11565283/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142649140","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}
ACS Materials AuPub Date : 2024-09-27eCollection Date: 2024-11-13DOI: 10.1021/acsmaterialsau.4c00098
Jiam Vuong, Shahab Derakhshan, Hadi Tavassol
{"title":"How Oxygen Deficiency and Its Ordering Control Electrical Conductivity in Sr<sub>2-<i>x</i></sub> Ca <sub><i>x</i></sub> Fe<sub>2</sub>O<sub>6-δ</sub> Perovskites as Related to Water Oxidation Electrocatalysis.","authors":"Jiam Vuong, Shahab Derakhshan, Hadi Tavassol","doi":"10.1021/acsmaterialsau.4c00098","DOIUrl":"10.1021/acsmaterialsau.4c00098","url":null,"abstract":"<p><p>We report on the analysis of oxygen vacancies (OVs) content and ordering of Sr<sub>2-<i>x</i></sub> Ca <sub><i>x</i></sub> Fe<sub>2</sub>O<sub>6-δ</sub> perovskites and explain how OVs change the electrical conductivity and oxygen evolution catalytic activity of these compounds. The structure and OV content are tuned by controlling the <i>A</i>-site composition and the reaction atmosphere. X-ray diffraction (XRD) and thermogravimetric analysis (TGA) are used to identify the crystal structures and to quantify bulk oxygen vacancy contents. Our analysis shows that OV content and crystal structure govern the electronic transport properties of the Sr<sub>2-<i>x</i></sub> Ca <sub><i>x</i></sub> Fe<sub>2</sub>O<sub>6-δ</sub> system. The electrical conductivity of oxygen-deficient perovskites (ODPs) is significantly higher than those in brownmillerites (by at least 2 orders of magnitude). Seebeck coefficient measurements identified that the Sr-rich ODPs and brownmillerites are <i>p</i>-type semiconductors, while Ca-rich brownmillerites are either insulators (within the experimental temperature range) or p-type semiconductors at lower temperatures (<750 K). Electrical conductivity of <i>p</i>-type semiconductors (Sr-rich compounds) reduces with higher OV content, and in brownmillerites with <i>x</i> ≥ 1.25, a transition to <i>n</i>-type semiconductor is observed at temperatures above 750 K. Our analysis shows that the hole and electron concentrations are similar in these brownmillerites, indicating major contributions from ionic transport. Finally, we show how oxygen deficiency alters the electrical conductivity and catalytic activity of the Sr<sub>2-<i>x</i></sub> Ca <sub><i>x</i></sub> Fe<sub>2</sub>O<sub>6-δ</sub> system in noncomplementary ways.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 6","pages":"654-663"},"PeriodicalIF":5.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11565281/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142650538","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}
ACS Materials AuPub Date : 2024-09-24eCollection Date: 2024-11-13DOI: 10.1021/acsmaterialsau.4c00062
Ewa M Iwanek Nee Wilczkowska, Leonarda Francesca Liotta, Giuseppe Pantaleo, Linje Hu, Shazam Williams, Donald W Kirk, Zbigniew Kaszkur
{"title":"Active Probing of a RuO<sub>2</sub>/CZ Catalyst Surface as a Tool for Bridging the Gap Between CO Oxidation Catalytic Tests in a Model and Realistic Exhaust Gas Stream.","authors":"Ewa M Iwanek Nee Wilczkowska, Leonarda Francesca Liotta, Giuseppe Pantaleo, Linje Hu, Shazam Williams, Donald W Kirk, Zbigniew Kaszkur","doi":"10.1021/acsmaterialsau.4c00062","DOIUrl":"10.1021/acsmaterialsau.4c00062","url":null,"abstract":"<p><p>Herein, we present a paper that attempts to bridge the gap between CO oxidation catalytic tests performed in a model stream and a more realistic exhaust gas stream by incorporating characterization methods that allow for active probing of the catalyst surface. The results have shown that it is not just the abundance of a given type of species on the surface that impacts the activity of a system but also the ease of extraction of ions from their surface (time-of-flight secondary ion mass spectrometry) and the response of the support to change in the feed composition (dynamic in situ X-ray diffraction (XRD) with variable atmosphere). The study utilizes the method of doping a catalyst (RuO<sub>2</sub>/CZ) with a small amount of alkali-metal (K<sup>+</sup> or Na<sup>+</sup>) carbonates in order to slightly modify its surface to gain insight into parameters that may cause discrepancies between model stream activity and complex stream activity. The most pronounced difference is that in the model stream, which contains only CO and O<sub>2</sub> in helium, both alkali ions improve the activity of the system at temperatures around 175 °C, whereas in the complex stream, which mimics the exhaust stream from a diesel engine under oxygen lean conditions, the K<sup>+</sup>-doped catalyst is slightly worse than RuO<sub>2</sub> /CZ and RuO<sub>2</sub> + Na<sup>+</sup>/CZ and much worse in propane combustion. The total hydrogen consumption values (temperature-programmed reduction) and the O<sub>ads</sub>/O<sub>latt</sub> ratios (X-ray photoelectron spectroscopy) both place the RuO<sub>2</sub> + K<sup>+</sup>/CZ system between the other two and hence provided no reason for the unusual behavior of the K<sup>+</sup>-doped catalyst. In contrast, both in situ XRD measurement tests and ToF SIMS results show a pronounced difference between the RuO<sub>2</sub> + K<sup>+</sup>/CZ catalyst and the other two systems, which indicates that the interaction of the surfaces with the reagents might be the cause of the discrepancy. The CO<sub>2</sub>-TPD results show that this system retains more CO<sub>2</sub>, i.e., the product, at adsorption sites, which might reduce the adsorption of other reagents, i.e., oxygen ions, CO, and propane, hence lowering the overall activity of the system.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 6","pages":"643-653"},"PeriodicalIF":5.7,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11565278/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142649136","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}
ACS Materials AuPub Date : 2024-09-05DOI: 10.1021/acsmaterialsau.4c00085
Jacob D. Hostert, Quincy Spitzer, Paola Giammattei, Julie N. Renner
{"title":"Correction to “Scalable Production of Peptides for Enhanced Struvite Formation via Expression on the Surface of Genetically Engineered Microbes”","authors":"Jacob D. Hostert, Quincy Spitzer, Paola Giammattei, Julie N. Renner","doi":"10.1021/acsmaterialsau.4c00085","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00085","url":null,"abstract":"We discovered that in our article published in 2023 (1) supplemental files describing the MEMP plasmid had the incorrect DNA sequence. In addition, while the MDEN sequence was correct in our supporting files, some annotations in the file describing the MDEN sequence were mislabeled. We have updated all Supporting Information documents with the correct MEMP plasmid sequence and annotations, as well as the correct MDEN sequence annotations. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsmaterialsau.4c00085. Schematic of experimental workflow, fluorescent assay results, supplemental SEM image, optical microscopy images, tables of statistical test outputs, pictures of precipitates, TGA curves, results of MINTEQ simulation with varying pH, raw DNA sequences of plasmids, and DNA sequences (PDF) Annotated DNA sequence of the MDEN plasmid (PDF) Annotated DNA sequence of the MEMP plasmid (PDF) Correction\u0000to “Scalable Production of Peptides\u0000for Enhanced Struvite Formation via Expression on the Surface of Genetically\u0000Engineered Microbes” <span> 0 </span><span> views </span> <span> 0 </span><span> shares </span> <span> 0 </span><span> downloads </span> Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. J.D.H. and Q.S. contributed equally. This article references 1 other publications. This article has not yet been cited by other publications.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"82 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142210834","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials AuPub Date : 2024-09-04DOI: 10.1021/acsmaterialsau.4c00036
Gyana Prakash Nanda, Rajan Suraksha, Pachaiyappan Rajamalli
{"title":"Role of Pyridine Nitrogen Position on the Moisture Sensitivity of Organic Emitters","authors":"Gyana Prakash Nanda, Rajan Suraksha, Pachaiyappan Rajamalli","doi":"10.1021/acsmaterialsau.4c00036","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00036","url":null,"abstract":"Moisture-sensitive fluorescent emitters are a class of smart materials that can change their emission behavior upon exposure to water. In this study, we have synthesized two highly fluorescent organic emitters, 4BPy-PTA and 2BPy-PTA, and showed how moisture sensitivity can be enhanced by molecular design modification. Owing to the different nitrogen atom positions in the acceptor units, the emitters show different degrees of moisture sensitivity. Upon moisture exposure, both emitters change their emission color from greenish-yellow to blue, but a larger shift was witnessed in 4BPy-PTA (81 nm) than in 2BPy-PTA (68 nm). Moisture exposure enhances the photoluminescence quantum yield (PLQY) of 4BPy-PTA from 37 to 48%, whereas it suppresses the PLQY of 2BPy-PTA from 59 to 15%. A shorter moisture sensing time, large emission color shift, and enhanced PLQY make 4BPy-PTA a better moisture-sensitive material than 2BPy-PTA. Interestingly, the emission colors of the emitters can be completely regained by heating and partially by applying mechanical force to the moisture-exposed solids. In addition, these emitters also show mechanochromic luminescence behavior with a completely reversible emission color switch between blue and green.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"11 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142210835","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials AuPub Date : 2024-08-16DOI: 10.1021/acsmaterialsau.4c00021
Tom Roussel, Daniel Ferry, Artemis Kosta, Dalila Miele, Giuseppina Sandri, Felista L. Tansi, Frank Steiniger, Paul Southern, Quentin A. Pankhurst, Ling Peng, Suzanne Giorgio
{"title":"Insight into the Internal Structure of High-Performance Multicore Magnetic Nanoparticles Used in Cancer Thermotherapy","authors":"Tom Roussel, Daniel Ferry, Artemis Kosta, Dalila Miele, Giuseppina Sandri, Felista L. Tansi, Frank Steiniger, Paul Southern, Quentin A. Pankhurst, Ling Peng, Suzanne Giorgio","doi":"10.1021/acsmaterialsau.4c00021","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00021","url":null,"abstract":"Multicore magnetic nanoparticles (MNPs), comprising iron oxide cores embedded in a sugar or starch matrix, are a class of nanomaterials with promising magnetic heating properties. Their internal structure, and particularly the strength of the internal core–core magnetic interactions, are believed to determine the functional properties, but there have been few detailed studies on this to date. We report here on an interlaboratory and multimodality transmission electron microscopy (TEM) and magnetic study of a high-performance MNP material (supplied by Resonant Circuits Limited, RCL) that is currently being used in a clinical study for the treatment of pancreatic cancer. TEM data were collected under a variety of conditions: conventional; high-resolution; scanning; cryogenic; and, for the first time, liquid phase. All the imaging modes showed mostly irregular dextran lamellae of lateral dimensions 30–90 nm, plus ca. 15% n/n of what appeared to be 30–60 nm long “nanorods”, and a multitude of well-dispersed ca. 3.7 nm diameter iron oxide cores. Cryogenic electron tomography indicated that the nanorods were edge-on lamellae, but in dried samples, tomography showed rod- or lath-shaped forms, possibly resulting from the collapse of lamellae during drying. High-resolution TEM (HRTEM) showed the dextran to be crystallized in the low-temperature hydrated dextran polymorph. Magnetic remanence Henkel-plot analysis indicated a weak core–core interaction field of ca. 4.8 kA/m. Theoretical estimates using a point-dipole model associated this field with a core-to-core separation distance of ca. 5 nm, which tallies well with the ca. 4–6 nm range of separation distances observed in liquid-cell TEM data. On this basis, we identify the structure–function link in the RCL nanoparticles to be the unusually well-dispersed multicore structure that leads to their strong heating capability. This insight provides an important design characteristic for the future development of bespoke nanomaterials for this significant clinical application.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"49 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142210955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials AuPub Date : 2024-08-16DOI: 10.1021/acsmaterialsau.4c0002110.1021/acsmaterialsau.4c00021
Tom Roussel, Daniel Ferry, Artemis Kosta, Dalila Miele, Giuseppina Sandri, Felista L. Tansi, Frank Steiniger, Paul Southern, Quentin A. Pankhurst*, Ling Peng* and Suzanne Giorgio*,
{"title":"Insight into the Internal Structure of High-Performance Multicore Magnetic Nanoparticles Used in Cancer Thermotherapy","authors":"Tom Roussel, Daniel Ferry, Artemis Kosta, Dalila Miele, Giuseppina Sandri, Felista L. Tansi, Frank Steiniger, Paul Southern, Quentin A. Pankhurst*, Ling Peng* and Suzanne Giorgio*, ","doi":"10.1021/acsmaterialsau.4c0002110.1021/acsmaterialsau.4c00021","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00021https://doi.org/10.1021/acsmaterialsau.4c00021","url":null,"abstract":"<p >Multicore magnetic nanoparticles (MNPs), comprising iron oxide cores embedded in a sugar or starch matrix, are a class of nanomaterials with promising magnetic heating properties. Their internal structure, and particularly the strength of the internal core–core magnetic interactions, are believed to determine the functional properties, but there have been few detailed studies on this to date. We report here on an interlaboratory and multimodality transmission electron microscopy (TEM) and magnetic study of a high-performance MNP material (supplied by Resonant Circuits Limited, RCL) that is currently being used in a clinical study for the treatment of pancreatic cancer. TEM data were collected under a variety of conditions: conventional; high-resolution; scanning; cryogenic; and, for the first time, liquid phase. All the imaging modes showed mostly irregular dextran lamellae of lateral dimensions 30–90 nm, plus ca. 15% n/n of what appeared to be 30–60 nm long “nanorods”, and a multitude of well-dispersed ca. 3.7 nm diameter iron oxide cores. Cryogenic electron tomography indicated that the nanorods were edge-on lamellae, but in dried samples, tomography showed rod- or lath-shaped forms, possibly resulting from the collapse of lamellae during drying. High-resolution TEM (HRTEM) showed the dextran to be crystallized in the low-temperature hydrated dextran polymorph. Magnetic remanence Henkel-plot analysis indicated a weak core–core interaction field of ca. 4.8 kA/m. Theoretical estimates using a point-dipole model associated this field with a core-to-core separation distance of ca. 5 nm, which tallies well with the ca. 4–6 nm range of separation distances observed in liquid-cell TEM data. On this basis, we identify the structure–function link in the RCL nanoparticles to be the unusually well-dispersed multicore structure that leads to their strong heating capability. This insight provides an important design characteristic for the future development of bespoke nanomaterials for this significant clinical application.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 5","pages":"489–499 489–499"},"PeriodicalIF":5.7,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00021","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161270","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":"Efficient Microwave Irradiation-Assisted Synthesis of Benzodioxinoquinoxaline and Its Donor-Variegated Derivatives Enabling Long-Lived Emission and Efficient Bipolar Charge Carrier Transport","authors":"Liliia Deva, Mariia Stanitska, Levani Skhirtladze, Amjad Ali, Glib Baryshnikov, Dmytro Volyniuk, Stepan Kutsiy, Mykola Obushak, Monika Cekaviciute, Pavlo Stakhira, Juozas Vidas Grazulevicius","doi":"10.1021/acsmaterialsau.4c00050","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00050","url":null,"abstract":"To enhance the usually low-charge carrier mobilities of highly twisted donor–acceptor-type compounds that exhibit thermally activated delayed fluorescence, we designed a rodlike acceptor benzodioxinoquinoxaline. This acceptor and two donor–acceptor–donor derivatives were synthesized via microwave Buchwald–Hartwig cross-coupling reactions with yields of up to 91%. The compounds exhibit three different types of photoluminescence, which is well-explained by quantum chemical calculations. Benzodioxinoquinoxaline shows blue fluorescence, with a very short lifetime of 0.64 ns. Its derivatives exhibit either green solid-state-enhanced thermally activated delayed fluorescence (SSE-TADF) or room-temperature phosphorescence (RTP) with lifetimes approaching 7 ms. When molecularly dispersed in a polymeric host, the compounds show a photoluminescence quantum yield close to 60%. The derivatives containing acridine or phenoxazine moieties exhibit bipolar charge transport. At an electric field of 5.8 × 10<sup>5</sup> V/cm, hole and electron mobilities of the phenoxazine-containing compound reach 3.2 × 10<sup>–4</sup> and 1.5 × 10<sup>–4</sup> cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup>, respectively. Among the studied SSE-TADF-based organic light-emitting diodes, the device containing this compound shows the highest external quantum efficiency of 12.3% due to the good charge-transporting and SSE-TADF parameters of the emitter.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142210944","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}