The Journal of Physical Chemistry Letters最新文献

{"title":"","authors":"Nataraju Bodappa*, Zixiao Zhang, Ramin Yazdaanpanah, Wyatt Behn, Kirk H. Bevan, Gregory Jerkiewicz and Peter Grutter, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c00053","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469094","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}

{"title":"","authors":"Beibei Yuan, Jidong Zhang and Haibo Wang*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01348","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469104","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}

{"title":"Origin of Stabilization of Ligand-Centered Mixed Valence Ruthenium Azopyridine Complexes: DFT Insights for Neuromorphic Applications.","authors":"A Avilés, S Perez Beltran, M Ghotbi, A J Ferguson, J L Blackburn, M Y Darensbourg, P B Balbuena","doi":"10.1021/acs.jpclett.5c00812","DOIUrl":"10.1021/acs.jpclett.5c00812","url":null,"abstract":"<p><p>Redox-driven conductance changes are critical processes in molecular- and coordination-complex-based memristive thin films and devices that are envisioned for neuromorphic technologies, but fundamental mechanisms of conductance switching are not fully understood. Here, we explore charge disproportionation (CD) processes in [Ru^IIL₂](PF₆)₂ molecular systems that intrinsically involve interfragment charge transfer (IFCT). Using a combination of <i>ab initio</i> molecular dynamics simulation (AIMD), time-dependent density functional theory (TD-DFT), and density functional theory (DFT) calculations, we investigate the electron transfer mechanisms and the roles of temperature and cell volumetric expansion in facilitating the counterion movements and electronic transitions required for low-cost IFCT and charge redistribution. A detailed analysis of the density of states and TD-DFT calculations highlights that unpaired electrons play a crucial role in low-energy transitions, with the azo (N═N) groups of the ligand serving as the primary sites for electronic transport between molecular fragments, further stabilizing the asymmetric state. Localization of added electrons on azo ligands occurs with negligible change at the Ru centers, supported by atomic volume expansions up to +4.74 bohr³, and goes along with a progressive reduction of the HOMO-LUMO gap across redox states, suggesting enhanced conductivity. The TD-DFT analysis reveals a dominant IFCT excitation at 2082.76 nm in the doubly reduced (22) state, while a stabilization energy of 1.20 eV of the asymmetric (13) state relative to the symmetric (22) state is predicted by constrained DFT. Periodic DFT and AIMD simulations emulating a molecular film show that the stabilization of the asymmetric state, relative to a symmetric one, translates in net charge separation values (order of ∼0.33 e) that are strongly linked to increased counterion mobility (average counterion displacements exceeding 0.7 Å per atom during CD events) and the involvement of azo groups in electron redistribution. These findings, which align with previously reported experimental and computational data, provide key insights into the IFCT mechanisms and electronic transport facilitated by azo groups, with important implications for redox-driven memristive and neuromorphic technologies.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6125-6137"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256775","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}

{"title":"Enhanced Quantum Yield and Long-Term Stability of Eco-Friendly Water-Dispersed InP/ZnSe/ZnS Quantum Dots via Photochemical Surface Passivation.","authors":"Hyeonmin Yim, Borim Shim, Hyeongwoo Kim, Seokyu Park, Cheolwan Park, Woo-Byoung Kim","doi":"10.1021/acs.jpclett.5c00188","DOIUrl":"10.1021/acs.jpclett.5c00188","url":null,"abstract":"<p><p>Quantum dots (QDs) are essential in fields such as bioimaging and electronics due to their unique optical properties. However, traditional cadmium (Cd)-based QDs pose significant environmental and health risks. This study aimed to develop efficient, Cd-free QDs suitable for water dispersion and long-term stability. We synthesized InP/ZnSe/ZnS multi-shell QDs and employed a photochemical surface passivation method using a halogen lamp to enhance their photoluminescence. For water dispersion, we used ligand exchange with hydrophilic agents, such as 3-mercaptopropionic acid (3-MPA) and 11-mercaptoundecanoic acid (11-MUA). This process facilitated the dispersion of QDs in water while maintaining their quantum yield (QY). The results revealed that the water-dispersed QDs retained 92.5% of their initial QY after 2 months, a notable improvement compared to the 47.3% retention of QDs dispersed in chloroform solvents. This demonstrates that our photochemical passivation method and ligand exchange effectively stabilize QDs in aqueous environments. These Cd-free, water-dispersed QDs offer significant advantages for sustainable electronics, water treatment, and biomedical applications. The study highlights the potential for broader commercialization and further research into optimizing QD performance through advanced ligand and synthesis techniques.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6008-6014"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256814","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}

{"title":"Insights into the Influence of the Potassium Ion on the Charge Carrier Kinetics of Potassium Poly(heptazine imides).","authors":"Yuna Kang, Rong Lu, Xin Zou, Jun Lin, Anchi Yu","doi":"10.1021/acs.jpclett.5c01209","DOIUrl":"10.1021/acs.jpclett.5c01209","url":null,"abstract":"<p><p>Understanding the influence of potassium ions (K⁺) on the charge carrier kinetics of potassium poly(heptazine imide) (K-PHI) is crucial for the rational design of efficient PHI-based photocatalytic materials. Herein, we prepare a series of K-PHI photocatalysts with varying K⁺ contents while maintaining constant cyanamide group content and conduct comprehensive femtosecond transient absorption (fs-TA) studies on them. The successful modulation of the K⁺ content in K-PHI samples was confirmed through FTIR, XRD, SEM-EDX, and ICP-OES measurements. A decay process with an ∼62 ps time constant was observed in the fs-TA kinetics of K-PHI samples, in which its amplitude increases linearly with K⁺ content in K-PHI samples, indicating that K⁺ plays a crucial role in modulating the ∼62 ps decay process of K-PHI materials. These findings provide valuable insights into the influence of K⁺ on the charge carrier kinetics and photophysical properties of K-PHI, offering a theoretical foundation for the design of efficient PHI-based photocatalytic materials.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6146-6154"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144264871","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}

{"title":"","authors":"Tong Xiang,&nbsp;Qiao Wang,&nbsp;Biwen He,&nbsp;Jibo Zhang,&nbsp;Xixi Huang,&nbsp;Wei Chen,&nbsp;Siwei Luo* and Xiang Qi,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01197","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144357880","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}

{"title":"","authors":"Hiroki Komiya,&nbsp;Swastik Laha,&nbsp;Keisuke Obata,&nbsp;Kalishankar Bhattacharyya and Kazuhiro Takanabe*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c00704","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144429037","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}

{"title":"","authors":"Caoyu Long,&nbsp;Qiming Lei,&nbsp;Erming Feng,&nbsp;Jianhui Chang,&nbsp;Yang Ding,&nbsp;Yuanji Gao,&nbsp;Siyuan Lu,&nbsp;Xinyue Wang,&nbsp;Hengyue Li* and Junliang Yang*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c00961","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469090","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}

{"title":"","authors":"H. da Silva Jr.,&nbsp;B. K. Kendrick,&nbsp;H. Li,&nbsp;S. Kotochigova and N. Balakrishnan*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01083","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469091","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}

{"title":"","authors":"Qianli Xue,&nbsp; and ,&nbsp;Kenji Mochizuki*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01091","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469095","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}