ACS Earth and Space Chemistry最新文献

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Elucidating Details of the Transformation of Birnessite into a Tunnel Structure in the Presence of Tl(I) 阐明桦褐铁矿在钛(I)存在下转变为隧道结构的细节
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-30 DOI: 10.1021/acsearthspacechem.4c0022710.1021/acsearthspacechem.4c00227
Rodrigo J. Martínez, Teresa Pi-Puig and Mario Villalobos*, 
{"title":"Elucidating Details of the Transformation of Birnessite into a Tunnel Structure in the Presence of Tl(I)","authors":"Rodrigo J. Martínez,&nbsp;Teresa Pi-Puig and Mario Villalobos*,&nbsp;","doi":"10.1021/acsearthspacechem.4c0022710.1021/acsearthspacechem.4c00227","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00227https://doi.org/10.1021/acsearthspacechem.4c00227","url":null,"abstract":"<p >The affinity between highly toxic Tl<sup>+</sup> and birnessite has been a matter of active research because the sorption mechanism involved seems to depend upon the doses of applied Tl<sup>+</sup> per Mn present, which also affects how birnessite is transformed. Aqueous Tl<sup>+</sup> is very mobile; therefore, its transformation and strong immobilization by Mn oxides is of high interest for environmental research. Birnessites are laminar Mn oxides that show a complex sorption behavior, which involves binding to internal sites of the structure and external surface groups and a high oxidation potential. In the present short investigation, we report some important issues not resolved over the mechanism involved when small Tl<sup>+</sup>/Mn interacts, in which the laminar structure changes to a tunneled structure. Specifically, because very little Tl<sup>+</sup> is oxidized (as opposed to when higher ratios are involved), water was experimentally confirmed as the reducing agent and the probable mechanism involved was theoretically worked out. Also, the irreversible nature of Tl(I) sorption inside the transformed tunneled structure was tested, which confirmed the extremely high affinity of the Mn oxide tunnels for dehydrated Tl(I).</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"8 11","pages":"2117–2122 2117–2122"},"PeriodicalIF":2.9,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.4c00227","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Spectroscopic Evidence of Ultrafast Topological Phase Transition by Light-Driven Strain 光驱动应变实现超快拓扑相变的光谱学证据
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c0625310.1021/acsnano.4c06253
Tae Gwan Park, Seungil Baek, Junho Park, Eui-Cheol Shin, Hong Ryeol Na, Eon-Taek Oh, Seung-Hyun Chun, Yong-Hyun Kim*, Sunghun Lee* and Fabian Rotermund*, 
{"title":"Spectroscopic Evidence of Ultrafast Topological Phase Transition by Light-Driven Strain","authors":"Tae Gwan Park,&nbsp;Seungil Baek,&nbsp;Junho Park,&nbsp;Eui-Cheol Shin,&nbsp;Hong Ryeol Na,&nbsp;Eon-Taek Oh,&nbsp;Seung-Hyun Chun,&nbsp;Yong-Hyun Kim*,&nbsp;Sunghun Lee* and Fabian Rotermund*,&nbsp;","doi":"10.1021/acsnano.4c0625310.1021/acsnano.4c06253","DOIUrl":"https://doi.org/10.1021/acsnano.4c06253https://doi.org/10.1021/acsnano.4c06253","url":null,"abstract":"<p >Enabling reversible control over the topological invariants, transitioning them from nontrivial to trivial states, has fundamental implications for quantum information processing and spintronics. It offers a promising avenue for establishing an efficient on/off switch mechanism for robust and dissipationless spin-currents. While mechanical strain has traditionally been advantageous for such manipulation of topological invariants, it often comes with the drawback of in-plane fractures, rendering it unsuitable for high-speed, time-dependent operations. This study employs ultrafast optical and THz spectroscopy to explore topological phase transitions induced by light-driven strain in Bi<sub>2</sub>Se<sub>3</sub>. Bi<sub>2</sub>Se<sub>3</sub> requires substantial strain for Z<sub>2</sub> switching. Our observations provide experimental evidence of ultrafast switching behavior, demonstrating a transition from a topological insulator with spin-momentum-locked surfaces to hybridized states and normal insulating phases under ambient conditions. Notably, applying light-induced strong out-of-plane strain effectively suppresses surface-bulk coupling, facilitating the differentiation of surface and bulk conductance even at room temperature─significantly surpassing the Debye temperature. We expect various time-dependent sequences of transient hybridization and manipulation of topological invariant through photoexcitation intensity adjustments. The sudden surface and bulk transport alterations near the transition point enable coherent conductance modulation at hypersound frequencies. Our findings on the potential of light-triggered ultrafast switching of topological invariants hold promise for high-speed topological switching and its related applications.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"30966–30977 30966–30977"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Noncontact 3D Bioprinting of Proteinaceous Microarrays for Highly Sensitive Immunofluorescence Detection within Clinical Samples 用于临床样本高灵敏度免疫荧光检测的蛋白质微阵列非接触式三维生物打印技术
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c1246010.1021/acsnano.4c12460
Amid Shakeri, Lubna Najm, Shadman Khan, Lei Tian, Liane Ladouceur, Hareet Sidhu, Nadine Al-Jabouri, Zeinab Hosseinidoust* and Tohid F. Didar*, 
{"title":"Noncontact 3D Bioprinting of Proteinaceous Microarrays for Highly Sensitive Immunofluorescence Detection within Clinical Samples","authors":"Amid Shakeri,&nbsp;Lubna Najm,&nbsp;Shadman Khan,&nbsp;Lei Tian,&nbsp;Liane Ladouceur,&nbsp;Hareet Sidhu,&nbsp;Nadine Al-Jabouri,&nbsp;Zeinab Hosseinidoust* and Tohid F. Didar*,&nbsp;","doi":"10.1021/acsnano.4c1246010.1021/acsnano.4c12460","DOIUrl":"https://doi.org/10.1021/acsnano.4c12460https://doi.org/10.1021/acsnano.4c12460","url":null,"abstract":"<p >Immunofluorescence assays are extensively used for the detection of disease-associated biomarkers within patient samples for direct diagnosis. Unfortunately, these 2D microarrays suffer from low repeatability and fail to attain the low limits of detection (LODs) required to accurately discern disease progression for clinical monitoring. While three-dimensional microarrays with increased biorecognition molecule density stand to circumvent these limitations, their viscous component materials are not compatible with current microarray fabrication protocols. Herein, we introduce a platform for 3D microarray bioprinting, wherein a two-step printing approach enables the high-throughput fabrication of immunosorbent hydrogels. The hydrogels are composed entirely of cross-linked proteins decorated with clinically relevant capture antibodies. Compared to two-dimensional microarrays, these proteinaceous microarrays offer 3-fold increases in signal intensity. When tested with clinically relevant biomarkers, ultrasensitive single-plex and multiplex detection of interleukin-6 (LOD 0.3 pg/mL) and tumor necrosis factor receptor 1 (LOD 1 pg/mL) is observed. When challenged with clinical samples, these hydrogel microarrays consistently discern elevated levels of interleukin-6 in blood plasma derived from patients with systemic blood infections. Given their easy-to-implement, high-throughput fabrication, and ultrasensitive detection, these three-dimensional microarrays will enable better clinical monitoring of disease progression, yielding improved patient outcomes.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31506–31523 31506–31523"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608908","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Controlled Spalling of 4H Silicon Carbide with Investigated Spin Coherence for Quantum Engineering Integration 研究自旋相干的 4H 碳化硅受控剥落,实现量子工程集成
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c1097810.1021/acsnano.4c10978
Connor P. Horn, Christina Wicker, Antoni Wellisz, Cyrus Zeledon, Pavani Vamsi Krishna Nittala, F. Joseph Heremans, David D. Awschalom and Supratik Guha*, 
{"title":"Controlled Spalling of 4H Silicon Carbide with Investigated Spin Coherence for Quantum Engineering Integration","authors":"Connor P. Horn,&nbsp;Christina Wicker,&nbsp;Antoni Wellisz,&nbsp;Cyrus Zeledon,&nbsp;Pavani Vamsi Krishna Nittala,&nbsp;F. Joseph Heremans,&nbsp;David D. Awschalom and Supratik Guha*,&nbsp;","doi":"10.1021/acsnano.4c1097810.1021/acsnano.4c10978","DOIUrl":"https://doi.org/10.1021/acsnano.4c10978https://doi.org/10.1021/acsnano.4c10978","url":null,"abstract":"<p >We detail scientific and engineering advances which enable the controlled spalling and layer transfer of single crystal 4H silicon carbide (4H-SiC) from bulk substrates. 4H-SiC’s properties, including high thermal conductivity and a wide bandgap, make it an ideal semiconductor for power electronics. Moreover, 4H-SiC is an excellent host of solid-state atomic defect qubits for quantum computing and quantum networking. Because 4H-SiC substrates are expensive (due to long growth times and limited yield), techniques for removal and transfer of bulk-quality films are desirable for substrate reuse and integration of the separated films. In this work, we utilize updated approaches for stressor layer thickness control and spalling crack initiation to demonstrate controlled spalling of 4H-SiC, the highest fracture toughness crystal spalled to date. We achieve coherent spin control of neutral divacancy (VV<sup>0</sup>) qubit ensembles and measure a quasi-bulk spin T<sub>2</sub> of 79.7 μs in the spalled films.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31381–31389 31381–31389"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c10978","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Route to Enhancing Remote Epitaxy of Perovskite Complex Oxide Thin Films 增强过氧化物复合氧化物薄膜远程外延的途径
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c0944510.1021/acsnano.4c09445
Sangho Lee, Xinyuan Zhang, Pooya Abdollahi, Matthew R. Barone, Chengye Dong, Young Jin Yoo, Min-Kyu Song, Doyoon Lee, Jung-El Ryu, Jun-Hui Choi, Jae-Hyun Lee, Joshua A. Robinson, Darrell G. Schlom, Hyun S. Kum, Celesta S. Chang*, Ambrose Seo* and Jeehwan Kim*, 
{"title":"Route to Enhancing Remote Epitaxy of Perovskite Complex Oxide Thin Films","authors":"Sangho Lee,&nbsp;Xinyuan Zhang,&nbsp;Pooya Abdollahi,&nbsp;Matthew R. Barone,&nbsp;Chengye Dong,&nbsp;Young Jin Yoo,&nbsp;Min-Kyu Song,&nbsp;Doyoon Lee,&nbsp;Jung-El Ryu,&nbsp;Jun-Hui Choi,&nbsp;Jae-Hyun Lee,&nbsp;Joshua A. Robinson,&nbsp;Darrell G. Schlom,&nbsp;Hyun S. Kum,&nbsp;Celesta S. Chang*,&nbsp;Ambrose Seo* and Jeehwan Kim*,&nbsp;","doi":"10.1021/acsnano.4c0944510.1021/acsnano.4c09445","DOIUrl":"https://doi.org/10.1021/acsnano.4c09445https://doi.org/10.1021/acsnano.4c09445","url":null,"abstract":"<p >Remote epitaxy is taking center stage in creating freestanding complex oxide thin films with high crystallinity that could serve as an ideal building block for stacking artificial heterostructures with distinctive functionalities. However, there exist technical challenges, particularly in the remote epitaxy of perovskite oxides associated with their harsh growth environments, making the graphene interlayer difficult to survive. Transferred graphene, typically used for creating a remote epitaxy template, poses limitations in ensuring the yield of perovskite films, especially when pulsed laser deposition (PLD) growth is carried out, since graphene degradation can be easily observed. Here, we employ spectroscopic ellipsometry to determine the critical factors that damage the integrity of graphene during PLD by tracking the change in optical properties of graphene <i>in situ</i>. To mitigate the issues observed in the PLD process, we propose an alternative growth strategy based on molecular beam epitaxy to produce single-crystalline perovskite membranes.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31225–31233 31225–31233"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608727","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Self-Assembled Controllable Cu-Based Perovskite/Calcium Oxide Hybrids with Strong Interfacial Interactions for Enhanced CH4 Electrosynthesis 具有强界面相互作用的自组装可控铜基过氧化物/氧化钙杂化物用于增强甲烷电合成
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c1145910.1021/acsnano.4c11459
Yu Zhang, Yunze Xu, Zitao Chen, Zhenbao Zhang, Xiangjian Liu, Zhen Xue, Xuezeng Tian, Xuedong Bai, Xue Wang, Minghua Huang, Jiawei Zhu*, Heqing Jiang and Yongfa Zhu, 
{"title":"Self-Assembled Controllable Cu-Based Perovskite/Calcium Oxide Hybrids with Strong Interfacial Interactions for Enhanced CH4 Electrosynthesis","authors":"Yu Zhang,&nbsp;Yunze Xu,&nbsp;Zitao Chen,&nbsp;Zhenbao Zhang,&nbsp;Xiangjian Liu,&nbsp;Zhen Xue,&nbsp;Xuezeng Tian,&nbsp;Xuedong Bai,&nbsp;Xue Wang,&nbsp;Minghua Huang,&nbsp;Jiawei Zhu*,&nbsp;Heqing Jiang and Yongfa Zhu,&nbsp;","doi":"10.1021/acsnano.4c1145910.1021/acsnano.4c11459","DOIUrl":"https://doi.org/10.1021/acsnano.4c11459https://doi.org/10.1021/acsnano.4c11459","url":null,"abstract":"<p >Cu-based perovskite oxide catalysts show promise for CO<sub>2</sub> electromethanation, but suffer from unsatisfactory CH<sub>4</sub> selectivity and poor stability. Here, we report self-assembled, controllable Cu-based perovskite/calcium oxide hybrids with strongly interacting interfaces for high-performance CH<sub>4</sub> electrosynthesis. As proof-of-concept catalysts, the La<sub>2</sub>CuO<sub>4</sub>/(CaO)<i><sub>x</sub></i> (<i>x</i> from 0.2 to 1.2) series has tunable CaO phase concentrations and thus controllable interface sizes. The La<sub>2</sub>CuO<sub>4</sub> and CaO components are intimately connected at the interface, leading to strong interfacial interactions mainly manifested by marked electron transfer from Ca<sup>2+</sup> to Cu<sup>2+</sup>. In CH<sub>4</sub> electrosynthesis, their activity and selectivity show a volcano-type dependence on the CaO phase concentrations and are positively correlated with the interface sizes. Among them, the La<sub>2</sub>CuO<sub>4</sub>/(CaO)<sub>0.8</sub> delivers the optimal activity and selectivity for CH<sub>4</sub>, together with good stability, much better than those of a physical-mixture counterpart and most reported Cu-based perovskite oxides. Moreover, La<sub>2</sub>CuO<sub>4</sub>/(CaO)<sub>0.8</sub> stands out as one of the most effective Cu-based catalysts for CH<sub>4</sub> electrosynthesis, achieving a high CH<sub>4</sub> selectivity of 77.6% at 300 mA cm<sup>–2</sup>. Our experiments and theoretical calculations highlight the significant role of self-assembly-induced strong interfacial interactions in promoting *CO adsorption/hydrogenation, intensifying resistance to structural degradation, and consequently underpinning the achievement of such optimized performance.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31466–31477 31466–31477"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608962","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Room Temperature Magnetic Skyrmions in Gradient-Composition Engineered CoPt Single Layers 梯度沉积工程 CoPt 单层中的室温磁天幕
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c1014510.1021/acsnano.4c10145
Adam Erickson, Qihan Zhang, Hamed Vakili, Chaozhong Li, Suchit Sarin, Suvechhya Lamichhane, Lanxin Jia, Ilja Fescenko, Edward Schwartz, Sy-Hwang Liou, Jeffrey E. Shield, Guozhi Chai, Alexey A. Kovalev, Jingsheng Chen* and Abdelghani Laraoui*, 
{"title":"Room Temperature Magnetic Skyrmions in Gradient-Composition Engineered CoPt Single Layers","authors":"Adam Erickson,&nbsp;Qihan Zhang,&nbsp;Hamed Vakili,&nbsp;Chaozhong Li,&nbsp;Suchit Sarin,&nbsp;Suvechhya Lamichhane,&nbsp;Lanxin Jia,&nbsp;Ilja Fescenko,&nbsp;Edward Schwartz,&nbsp;Sy-Hwang Liou,&nbsp;Jeffrey E. Shield,&nbsp;Guozhi Chai,&nbsp;Alexey A. Kovalev,&nbsp;Jingsheng Chen* and Abdelghani Laraoui*,&nbsp;","doi":"10.1021/acsnano.4c1014510.1021/acsnano.4c10145","DOIUrl":"https://doi.org/10.1021/acsnano.4c10145https://doi.org/10.1021/acsnano.4c10145","url":null,"abstract":"<p >Topologically protected magnetic skyrmions in magnetic materials are stabilized by an interfacial or bulk Dzyaloshinskii–Moriya interaction (DMI). Interfacial DMI decays with an increase of the magnetic layer thickness in just a few nanometers, and bulk DMI typically stabilizes magnetic skyrmions at low temperatures. Consequently, more flexibility in the manipulation of DMI is required for utilizing nanoscale skyrmions in energy-efficient memory and logic devices at room temperature (RT). Here, we demonstrate the observation of RT skyrmions stabilized by gradient DMI (g-DMI) in composition gradient-engineered CoPt single-layer films by employing the topological Hall effect, magnetic force microscopy, and nitrogen-vacancy scanning magnetometry. Skyrmions remain stable over a wide range of applied magnetic fields and are confirmed to be nearly Bloch-type from micromagnetic simulation and analytical magnetization reconstruction. Furthermore, we observe skyrmion pairs, which may be explained by skyrmion–antiskyrmion interactions. Our findings expand the family of magnetic materials hosting RT magnetic skyrmions by tuning g-DMI via gradient polarity and a choice of magnetic elements.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31261–31273 31261–31273"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608964","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Engineering Supramolecular Nanofiber Depots from a Glucagon-Like Peptide-1 Therapeutic 利用胰高血糖素样肽-1 治疗剂制造超分子纳米纤维储层
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c1024810.1021/acsnano.4c10248
Weike Chen, Sijie Xian, Bernice Webber, Emily L. DeWolf, Connor R. Schmidt, Rory Kilmer, Dongping Liu, Elizabeth M. Power and Matthew J. Webber*, 
{"title":"Engineering Supramolecular Nanofiber Depots from a Glucagon-Like Peptide-1 Therapeutic","authors":"Weike Chen,&nbsp;Sijie Xian,&nbsp;Bernice Webber,&nbsp;Emily L. DeWolf,&nbsp;Connor R. Schmidt,&nbsp;Rory Kilmer,&nbsp;Dongping Liu,&nbsp;Elizabeth M. Power and Matthew J. Webber*,&nbsp;","doi":"10.1021/acsnano.4c1024810.1021/acsnano.4c10248","DOIUrl":"https://doi.org/10.1021/acsnano.4c10248https://doi.org/10.1021/acsnano.4c10248","url":null,"abstract":"<p >Diabetes and obesity have emerged as major global health concerns. Glucagon-like peptide-1 (GLP-1), a natural incretin hormone, stimulates insulin production and suppresses glucagon secretion to stabilize and reduce blood glucose levels and control appetite. The therapeutic use of GLP-1 receptor agonists (e.g., semaglutide) has transformed the standard of care in recent years for treating type 2 diabetes and reversing obesity. The native GLP-1 sequence has a very short half-life, and therapeutic advances have come from molecular engineering to alter the pharmacokinetic profile of synthetic GLP-1 receptor agonists to enable once-weekly administration, reduce the frequency of injection, and improve adherence. Efforts to further extend this profile would offer additional convenience or enable entirely different treatment modalities. Here, an injectable GLP-1 receptor agonist depot is engineered through integration of a prosthetic self-assembling peptide motif to enable supramolecular nanofiber formation and hydrogelation. This supramolecular GLP-1 receptor agonistic (PA-GLP1) offers sustained release in vitro for multiple weeks, supporting long-lasting therapy. Moreover, in a rat model of type 2 diabetes, a single injection of the supramolecular PA-GLP1 formulation achieved sustained serum concentrations for at least 40 days, with an overall reduction in blood glucose levels and reduced weight gain, comparing favorably to daily injections of semaglutide. The general and modular approach is also extensible to other next-generation peptide therapies. Accordingly, the formation of supramolecular nanofiber depots offers a more convenient and long-lasting therapeutic option to manage diabetes and treat metabolic disorders.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31274–31285 31274–31285"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficient Energy Transfer Enabled by Dark States in van der Waals Heterostructures 范德瓦尔斯异质结构中暗态促成的高效能量转移
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c0940310.1021/acsnano.4c09403
Ziyu Luo, Xiao Yi, Ying Jiang, Nannan Luo, Bingjie Liu, Yangguang Zhong, Qin Tan, Qi Jiang, Xinfeng Liu, Shula Chen*, Yuerui Lu* and Anlian Pan*, 
{"title":"Efficient Energy Transfer Enabled by Dark States in van der Waals Heterostructures","authors":"Ziyu Luo,&nbsp;Xiao Yi,&nbsp;Ying Jiang,&nbsp;Nannan Luo,&nbsp;Bingjie Liu,&nbsp;Yangguang Zhong,&nbsp;Qin Tan,&nbsp;Qi Jiang,&nbsp;Xinfeng Liu,&nbsp;Shula Chen*,&nbsp;Yuerui Lu* and Anlian Pan*,&nbsp;","doi":"10.1021/acsnano.4c0940310.1021/acsnano.4c09403","DOIUrl":"https://doi.org/10.1021/acsnano.4c09403https://doi.org/10.1021/acsnano.4c09403","url":null,"abstract":"<p >Dark exciton states show great potential in condensed matter physics and optoelectronics because of their long lifetime and rich distribution in band structures. Therefore, they can theoretically serve as efficient energy reservoirs, providing a platform for future applications. However, their optical-transition-forbidden nature severely limits their experimental exploration and hinders their current application. Here, we demonstrate a universal dark state nonlinear energy transfer (ET) mechanism in monolayer WS<sub>2</sub>/CsPbBr<sub>3</sub> van der Waals heterostructures under two-photon excitation, which successfully utilizes the enormous energy reserved in the dark exciton state of CsPbBr<sub>3</sub> to significantly improve the photoelectric performance of monolayer WS<sub>2</sub>. We first propose the scenario of resonant ET between the dark state of CsPbBr<sub>3</sub> and WS<sub>2</sub>, and then reveal that this is a typical Förster resonant ET and belongs to the 2D-2D category. Interestingly, the dark state ET in CsPbBr<sub>3</sub> is identified as a long-range donor–bridge–acceptor hopping mode, with a potential distance exceeding 200 nm. Finally, we successfully achieve nearly an order of magnitude enhancement in the near-infrared detection performance of monolayer WS<sub>2</sub>. Our results enrich the theory of dark exciton states and ET, and they provide a way of using dark exciton states for future practical applications.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31215–31224 31215–31224"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Uniform Diffusion of Cooper Pairing Mediated by Hole Carriers in Topological Sb2Te3/Nb 拓扑 Sb2Te3/Nb 中由空穴载流子介导的库珀配对均匀扩散
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-29 DOI: 10.1021/acsnano.4c1053310.1021/acsnano.4c10533
Joseph A. Hlevyack, Sahand Najafzadeh, Yao Li, Tsubaki Nagashima, Akifumi Mine, Yigui Zhong, Takeshi Suzuki, Akiko Fukushima, Meng-Kai Lin, Soorya Suresh Babu, Jinwoong Hwang, Ji-Eun Lee, Sung-Kwan Mo, James N. Eckstein, Shik Shin, Kozo Okazaki* and Tai-Chang Chiang*, 
{"title":"Uniform Diffusion of Cooper Pairing Mediated by Hole Carriers in Topological Sb2Te3/Nb","authors":"Joseph A. Hlevyack,&nbsp;Sahand Najafzadeh,&nbsp;Yao Li,&nbsp;Tsubaki Nagashima,&nbsp;Akifumi Mine,&nbsp;Yigui Zhong,&nbsp;Takeshi Suzuki,&nbsp;Akiko Fukushima,&nbsp;Meng-Kai Lin,&nbsp;Soorya Suresh Babu,&nbsp;Jinwoong Hwang,&nbsp;Ji-Eun Lee,&nbsp;Sung-Kwan Mo,&nbsp;James N. Eckstein,&nbsp;Shik Shin,&nbsp;Kozo Okazaki* and Tai-Chang Chiang*,&nbsp;","doi":"10.1021/acsnano.4c1053310.1021/acsnano.4c10533","DOIUrl":"https://doi.org/10.1021/acsnano.4c10533https://doi.org/10.1021/acsnano.4c10533","url":null,"abstract":"<p >Spin-helical Dirac Fermions at a doped topological insulator’s boundaries can support Majorana quasiparticles when coupled with <i>s</i>-wave superconductors, but in <i>n</i>-doped systems, the requisite induced Cooper pairing in topological states is often buried at heterointerfaces or complicated by degenerate coupling with bulk conduction carriers. Rarely probed are <i>p</i>-doped topological structures with nondegenerate Dirac and bulk valence bands at the Fermi level, which may foster long-range superconductivity without sacrificing Majorana physics. Using ultrahigh-resolution photoemission, we report proximity pairing with a large decay length in <i>p</i>-doped topological Sb<sub>2</sub>Te<sub>3</sub> on superconducting Nb. Despite no momentum-space degeneracy, the topological and bulk states of Sb<sub>2</sub>Te<sub>3</sub>/Nb exhibit the same isotropic superconducting gaps at low temperatures. Our results unify principles for realizing accessible pairing in Dirac Fermions relevant to topological superconductivity.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31323–31331 31323–31331"},"PeriodicalIF":15.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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