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Emergence of Compact Oligomers inside the Small-World Network of TDP-43 Condensates. TDP-43凝析油小世界网络中致密低聚物的出现
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-25 DOI: 10.1021/acs.jpclett.5c01627
Huayuan Tang,Yunxiang Sun,Lei Wang,Pu Chun Ke,Feng Ding
{"title":"Emergence of Compact Oligomers inside the Small-World Network of TDP-43 Condensates.","authors":"Huayuan Tang,Yunxiang Sun,Lei Wang,Pu Chun Ke,Feng Ding","doi":"10.1021/acs.jpclett.5c01627","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01627","url":null,"abstract":"Liquid-liquid phase separation (LLPS) of TDP-43 mediates the formation of pathological inclusions in various neurodegenerative diseases, with the condensate structures and related amyloid aggregation remaining elusive. Here, by developing a data-driven bottom-up coarse-grained model using discrete molecular dynamics simulations, we found proteins in the condensates of TDP-43 forming a dynamic network of fluctuating sizes. While dominated by peptides engaged with a small number of peptides connected by a low number of interpeptide contacts, the condensates also contained peptides with large numbers of connections, serving as hubs of a small-world network. Importantly, peptides in these high-contact states were intertwined to form oligomers that were stable for relatively long periods inside the weakly connected network. These oligomers were likely the aggregation intermediates toward nucleation of amyloid fibrils. Therefore, this transferable coarse-grained model may serve as a powerful tool for unraveling the inner workings of LLPS and amyloid aggregation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"9 1","pages":"7797-7806"},"PeriodicalIF":6.475,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701178","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Impact of Dark Polariton States on Collective Strong Light-Matter Coupling in Molecules. 暗极化态对分子中集体强光-物质耦合的影响。
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-25 DOI: 10.1021/acs.jpclett.5c01480
Lucas Borges,Thomas Schnappinger,Markus Kowalewski
{"title":"Impact of Dark Polariton States on Collective Strong Light-Matter Coupling in Molecules.","authors":"Lucas Borges,Thomas Schnappinger,Markus Kowalewski","doi":"10.1021/acs.jpclett.5c01480","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01480","url":null,"abstract":"Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities, as demonstrated in numerous experiments over the past few years. These experiments are typically interpreted in terms of the Jaynes-Cummings or Tavis-Cummings models under the assumption that the molecular ensemble is only excited by a single photon. In such a model, two polariton states compete with an overwhelming number of dark states, inhibiting polaritonic reactions entropically. We analyze the higher excitation manifolds of the Tavis-Cummings model along with a three-level system that resembles photochemical reactions. We demonstrate that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"114 1","pages":"7807-7815"},"PeriodicalIF":6.475,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701174","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
(Photo)redox Processes Involving the Eu(II)/Eu(III) Couple. （图）涉及Eu(II)/Eu（III）偶联的氧化还原过程。
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-25 DOI: 10.1021/acs.jpclett.5c01800
Lea Gundorff Nielsen,Thomas Just Sørensen
{"title":"(Photo)redox Processes Involving the Eu(II)/Eu(III) Couple.","authors":"Lea Gundorff Nielsen,Thomas Just Sørensen","doi":"10.1021/acs.jpclett.5c01800","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01800","url":null,"abstract":"Processes involving electron transfer driven by differences in chemical potential and/or light hold promise for chemical transformation. One system that has been proposed for these applications is the versatile Eu(II)/Eu(III) redox couple, where either species has diverse and tunable optical and electrochemical properties. Here, the details of the processes involved in electron transfer from and to europium centers are considered and probed using seven differing organic dyes in dimethyl sulfoxide (DSMO)─the only solvent where all species are soluble and can be oxidized and reduced. Most dyes were reduced by Eu(II), but one dye, triazatriangulenium (TATA), enabled an experimental determination of quenching by Eu(III) and Eu(II) via photoelectron transfer quenching. It was found that while Eu(III) does not interact strongly with the organic dyes, Eu(II) is a potent reducing agent for organic molecules, disregarding whether the substrate is in the ground state or the excited state. We concluded that ground state reduction of any substrate by Eu(II) must be considered in all cases, where photoredox chemistry involving the Eu(II)/Eu(III) redox couple is explored. Finally, we advocate that the redox potentials of all involved species be determined if a mechanism is proposed.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"70 1","pages":"7816-7823"},"PeriodicalIF":6.475,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24
Zhi-Chao Huang-Fu, Yuqin Qian, Jesse B. Brown and Yi Rao*, 
{"title":"","authors":"Zhi-Chao Huang-Fu, Yuqin Qian, Jesse B. Brown and Yi Rao*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 29","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01570","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24
Renjie Zhu, Yuwei Zhang*, Tong Zhu and Fei Xia*, 
{"title":"","authors":"Renjie Zhu, Yuwei Zhang*, Tong Zhu and Fei Xia*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 29","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01226","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24
{"title":"","authors":"","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 29","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jzv016i029_1964189","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24
Tsung-Yen Lee, Lam Lam, Dhruv Patel-Tupper, Henry E. Lam, Krishna K. Niyogi and Graham R. Fleming*, 
{"title":"","authors":"Tsung-Yen Lee, Lam Lam, Dhruv Patel-Tupper, Henry E. Lam, Krishna K. Niyogi and Graham R. Fleming*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 29","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01473","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685279","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Molecular Entanglement Witness by Absorption Spectroscopy in Cavity QED. 腔QED中分子纠缠的吸收光谱见证。
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24 Epub Date: 2025-07-14 DOI: 10.1021/acs.jpclett.5c01392
Weijun Wu, Francesca Fassioli, David A Huse, Gregory D Scholes
{"title":"Molecular Entanglement Witness by Absorption Spectroscopy in Cavity QED.","authors":"Weijun Wu, Francesca Fassioli, David A Huse, Gregory D Scholes","doi":"10.1021/acs.jpclett.5c01392","DOIUrl":"10.1021/acs.jpclett.5c01392","url":null,"abstract":"<p><p>Producing and maintaining molecular entanglement at room temperature and detecting multipartite entanglement features of macroscopic molecular systems remain key challenges for understanding intermolecular quantum effects in chemistry. Here, we study the quantum Fisher information, as a multipartite entanglement witness. We generalize the entanglement witness functional related to quantum Fisher information regarding nonidentical local response operators. We demonstrate its effectiveness for intermolecular entanglement in ultrastrong light-matter coupling in cavity quantum electrodynamics, including near the superradiant phase transition. Additionally, we establish a connection between quantum Fisher information and the dipole correlator, indicating that entanglement could be detected through absorption spectroscopy. Our work proposes a general protocol to detect intermolecular entanglement in chemical systems at room temperature.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"7369-7375"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144625019","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24
Pankaj Kumar Samal, Jan Škvára, Matyas Výhonský, Lukáš Fusek, Michal Ronovský, Viktor Johánek, Maximilian Kastenmeier, Yaroslava Lykhach, Jörg Libuda, Olaf Brummel and Josef Mysliveček*, 
{"title":"","authors":"Pankaj Kumar Samal,&nbsp;Jan Škvára,&nbsp;Matyas Výhonský,&nbsp;Lukáš Fusek,&nbsp;Michal Ronovský,&nbsp;Viktor Johánek,&nbsp;Maximilian Kastenmeier,&nbsp;Yaroslava Lykhach,&nbsp;Jörg Libuda,&nbsp;Olaf Brummel and Josef Mysliveček*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 29","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01465","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-07-24
Jiaxin Liu, Guangmin Ren*, Guojing Hu, Chengwei Wang, Tuo Guo*, Qingjie Guo* and Pei Sean Goh, 
{"title":"","authors":"Jiaxin Liu,&nbsp;Guangmin Ren*,&nbsp;Guojing Hu,&nbsp;Chengwei Wang,&nbsp;Tuo Guo*,&nbsp;Qingjie Guo* and Pei Sean Goh,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 29","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01551","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
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