The Journal of Physical Chemistry Letters最新文献_第10页

An Aggregation Accelerable Pathway of Triplet Excitation Transfer Newly Identified in the LHCII Complexes from Spinach and Bryopsis corticulans 新发现的菠菜和苔藓LHCII复合物中三重态激发传递的聚集加速途径

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0091410.1021/acs.jpclett.5c00914

Rong-Yao Gao, Yan-Ping Shi, Jian-Wei Zou, Dan-Hong Li, Hao-Yi Wang, Junrong Zheng* and Jian-Ping Zhang*,

{"title":"An Aggregation Accelerable Pathway of Triplet Excitation Transfer Newly Identified in the LHCII Complexes from Spinach and Bryopsis corticulans","authors":"Rong-Yao Gao, Yan-Ping Shi, Jian-Wei Zou, Dan-Hong Li, Hao-Yi Wang, Junrong Zheng* and Jian-Ping Zhang*, ","doi":"10.1021/acs.jpclett.5c0091410.1021/acs.jpclett.5c00914","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00914https://doi.org/10.1021/acs.jpclett.5c00914","url":null,"abstract":"Oxygenic photosynthetic organisms employ multiple photoprotection mechanisms. The major light-harvesting complex of photosystem II of Bryopsis corticulans (B-LHCII) and that of spinach (S-LHCII) are structurally analogous but differ in their pigment compositions. We have attempted to compare, by evaluating the rate of chlorophyll (Chl)-to-carotenoid (Car) triplet excitation transfer (TET), the photoprotection of B- and S-LHCII in light-harvesting and energy-quenched states and observed a fast and a slow TET pathway for the LHCIIs irrespective of the functional states. The fast one in a sub-nanosecond time scale is attributed to the TET from Chl a612 (a603) to L1-Car (L2-Car), whereas the slow one in ∼10 ns is assigned to the TET from Chl a613 to L1-Car. Ongoing from the light-harvesting to the quenched state, the slow TET is accelerated from (14.0 ns)−1 to (4.7 ns)−1 for S-LHCII and from (25.0 ns)−1 to (17.0 ns)−1 for B-LHCII, becoming dominant for photoprotection at the L1 site. Thus, the TET enhancement and energy-quenching reactivity constitute the synergistic photoprotection of the LHCIIs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 20","pages":"5144–5152 5144–5152"},"PeriodicalIF":4.8,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104961","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

Intrinsic Defect Tolerance in Inorganic Tin–Lead Perovskites 无机锡铅钙钛矿的内在缺陷容忍度

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0109210.1021/acs.jpclett.5c01092

Jiajia Zhang*, Xinhao Duan, Zhuang Hu, Xiang Li, Lin Zhang and Shuisheng Chen*,

{"title":"Intrinsic Defect Tolerance in Inorganic Tin–Lead Perovskites","authors":"Jiajia Zhang*, Xinhao Duan, Zhuang Hu, Xiang Li, Lin Zhang and Shuisheng Chen*, ","doi":"10.1021/acs.jpclett.5c0109210.1021/acs.jpclett.5c01092","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01092https://doi.org/10.1021/acs.jpclett.5c01092","url":null,"abstract":"Experimentally, inorganic tin–lead (Sn–Pb) perovskites exhibit an extremely short carrier lifetime of mere nanoseconds, primarily attributed to strong nonradiative recombination induced by high-density defects. This has led to the belief that they are highly defect-sensitive. Here, we argue that inorganic Sn–Pb perovskites are intrinsically defect-tolerant. We substantiate this claim by performing rigorous first-principles calculations for a prototypical composition CsSn0.5Pb0.5I3. Our results show that this material possesses an ultralong nonradiative lifetime of 10 μs, even under the assumption of a high defect concentration of 1016 cm–3. The alteration in band edge energies arising from the mixing of CsSnI3 and CsPbI3 is proven to contribute to the remarkable defect tolerance. We ascribe the poor photoelectric performance observed in inorganic Sn–Pb perovskites to inadequate miscibility of their components. This study reveals the inherent superior properties of inorganic Sn–Pb perovskites that have thus far remained unrecognized by the research community and suggests that achieving phase-pure mixing systems is crucial to fully exploit their untapped potential.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5208–5212 5208–5212"},"PeriodicalIF":4.8,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166053","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

Highly Oriented Nitrogen-Doped Flower-like ZnO Nanostructures for Boosting Photocatalytic and Photoelectrochemical Performance: A Combined Experimental and DFT Study. 高取向氮掺杂花状ZnO纳米结构提高光催化和光电化学性能：实验与DFT相结合的研究。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c01085

Riu Riu Wary,Abinash Das,Emir S Amirov,Dongyu Liu,Shriya Gumber,Elena A Kazakova,Andrey S Vasenko,Oleg V Prezhdo

{"title":"Highly Oriented Nitrogen-Doped Flower-like ZnO Nanostructures for Boosting Photocatalytic and Photoelectrochemical Performance: A Combined Experimental and DFT Study.","authors":"Riu Riu Wary,Abinash Das,Emir S Amirov,Dongyu Liu,Shriya Gumber,Elena A Kazakova,Andrey S Vasenko,Oleg V Prezhdo","doi":"10.1021/acs.jpclett.5c01085","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01085","url":null,"abstract":"A facile method to modify the ZnO catalyst by nitrogen doping and synthesis of a highly oriented flower-like structure is reported. The generated system exhibits an enhanced photoinduced charge separation through the lightning rod effect. A well-aligned structure and high aspect ratio of ZnO nanorods is confirmed by the XRD, FESEM and TEM analyses. Efficient photogenerated charge transfer is achieved upon light irradiation, as confirmed by PL and EIS studies. Density functional theory (DFT) calculations provide an atomistic understanding of the modified electronic structure of N-doped ZnO. N-doped ZnO with 5 wt % exhibits the best photocatalytic performance. When applied to the photoelectrochemical water splitting, the optimal catalyst can achieve a remarkable photocurrent density of 4.0 mAcm-2 at the lowest onset potential of 0.61 V vs Ag/AgCl (1.40 V vs RHE). The reported work demonstrates that rational design of doped materials opens up new avenues for catalyst development.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"40 1","pages":"5180-5187"},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143991939","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

Tracing Ion Migration in Halide Perovskites with Machine Learned Force Fields 用机器学习力场追踪卤化钙钛矿中的离子迁移

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0113910.1021/acs.jpclett.5c01139

Viren Tyagi, Mike Pols, Geert Brocks and Shuxia Tao*,

{"title":"Tracing Ion Migration in Halide Perovskites with Machine Learned Force Fields","authors":"Viren Tyagi, Mike Pols, Geert Brocks and Shuxia Tao*, ","doi":"10.1021/acs.jpclett.5c0113910.1021/acs.jpclett.5c01139","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01139https://doi.org/10.1021/acs.jpclett.5c01139","url":null,"abstract":"Halide perovskite optoelectronic devices suffer from chemical degradation and current–voltage hysteresis induced by migration of highly mobile charged defects. Atomic scale molecular dynamics simulations can capture the motion of these ionic defects, but classical force fields are too inflexible to describe their dynamical charge states. Using CsPbI3 as a case study, we train machine learned force fields from density functional theory calculations and study the diffusion of charged halide interstitial and vacancy defects in bulk CsPbI3. We find that negative iodide interstitials and positive iodide vacancies, the most stable charge states for their respective defect type, migrate at similar rates at room temperature. Neutral interstitials are faster, but neutral vacancies are 1 order of magnitude slower. Oppositely charged interstitials and vacancies, as they can occur in device operation or reverse bias conditions, are significantly slower and can be considered relatively immobile.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 20","pages":"5153–5159 5153–5159"},"PeriodicalIF":4.8,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.5c01139","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104934","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

Capturing Hydrate Formation Processes in Tetrahydrofuran/Water Mixtures with Temperature Resolved In Situ Synchrotron X-ray Diffraction and Infrared Spectroscopy 用原位同步加速器x射线衍射和红外光谱技术捕捉四氢呋喃/水混合物中水合物形成过程

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0057610.1021/acs.jpclett.5c00576

Robert P. C. Bauer, Danny Rodriguez, Santanu Pathak and John S. Tse*,

{"title":"Capturing Hydrate Formation Processes in Tetrahydrofuran/Water Mixtures with Temperature Resolved In Situ Synchrotron X-ray Diffraction and Infrared Spectroscopy","authors":"Robert P. C. Bauer, Danny Rodriguez, Santanu Pathak and John S. Tse*, ","doi":"10.1021/acs.jpclett.5c0057610.1021/acs.jpclett.5c00576","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00576https://doi.org/10.1021/acs.jpclett.5c00576","url":null,"abstract":"Understanding the mechanisms behind clathrate hydrate formation is of both practical and fundamental interest. Here, we report the formation of a clathrate hydrate from a tetrahydrofuran (THF)–water mixture of “ideal” stoichiometry, deposited cryogenically in ultrahigh vacuum and studied with in situ synchrotron X-ray diffraction and infrared spectroscopy on slightly deuterated water samples. The experiments provide complementary information on the evolution of the system’s local and long-range orders. They revealed distinctive structural transformations in different temperature regimes. The as-deposited sample showed a disordered diffraction pattern. Upon heating, THF segregated and crystallized, while solid water remained amorphous. Crystalline THF persisted until 110 K, then it melted and interacted with water to form type II clathrate without ice contamination. No new crystalline or amorphous phases were observed prior to the onset crystallization of the hydrate. This work provides atomic-level insight into molecular rearrangements during clathrate hydrate formation, highlighting molecular mobility even at low temperatures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 20","pages":"5160–5167 5160–5167"},"PeriodicalIF":4.8,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104962","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

Investigation of Intramolecular Triplet-Triplet Annihilation Upconversion by Double Sensitization. 双敏化作用下分子内三重态-三重态湮灭上转换的研究。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c00606

Aoi Haraguchi,Kenichi Goushi,Shoma Sasaki,Chihaya Adach

引用次数: 0

Tracing Ion Migration in Halide Perovskites with Machine Learned Force Fields 用机器学习力场追踪卤化钙钛矿中的离子迁移

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c01139

Viren Tyagi, Mike Pols, Geert Brocks, Shuxia Tao

引用次数: 0

Dual-Interface Passivation of Wide-Bandgap Perovskite Films for Efficient Four-Terminal Perovskite–Organic Tandem Solar Cells 高效四端钙钛矿-有机串联太阳能电池中宽带隙钙钛矿膜的双界面钝化

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c00756

Fawad Aslam, Hengyue Li, Jianhui Chang, Muhammad Tahir, Muhammad Zahid, Muhammad Irfan Sadiq, Xiang Liao, Qiang Zeng, Fangyang Liu, Junliang Yang

{"title":"Dual-Interface Passivation of Wide-Bandgap Perovskite Films for Efficient Four-Terminal Perovskite–Organic Tandem Solar Cells","authors":"Fawad Aslam, Hengyue Li, Jianhui Chang, Muhammad Tahir, Muhammad Zahid, Muhammad Irfan Sadiq, Xiang Liao, Qiang Zeng, Fangyang Liu, Junliang Yang","doi":"10.1021/acs.jpclett.5c00756","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00756","url":null,"abstract":"Interface defects in perovskite solar cells (PSCs) can significantly impair device efficiency by promoting nonradiative recombination, hindering charge transport, and facilitating ion migration. In this work, we introduce a dual-interface passivation strategy utilizing 2-(N-morpholino)ethanesulfonic acid potassium (MESK) and octylammonium iodide (OAI), targeting both the electron transport layer (ETL)/perovskite and perovskite/hole transport layer (HTL) interfaces to enhance the efficiency of wide-bandgap PSCs based on FA0.8Cs0.2Pb(I0.6Br0.4)3 with a bandgap of 1.77 eV. The sulfonic group in MESK passivates bottom interface defects through coordination with Pb ions, while the amine group in OAI interacts with Pb and halide ions to effectively passivate top interface defects. The dual-interface passivation strategy improves perovskite crystallinity, enlarges grain size, and reduces nonradiative recombination. As a result, the performance of PSCs is significantly enhanced, achieving a power conversion efficiency (PCE) of 23.69% in a four-terminal (4T) perovskite–organic tandem solar cell (TSC), which provides a promising and sustainable solution for the commercialization of TSCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"5 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144000618","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

Electrically Induced Topological Chirality Switching in Orbital-Engineered Covalent Organic Radical Framework Monolayers. 轨道工程共价有机自由基框架单层的电诱导拓扑手性开关。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c00802

Yifan Li,Kai Zhang,Yu Pan,Daoxiong Wu,Haifeng Lv,Xiaojun Wu,Jinlong Yang

{"title":"Electrically Induced Topological Chirality Switching in Orbital-Engineered Covalent Organic Radical Framework Monolayers.","authors":"Yifan Li,Kai Zhang,Yu Pan,Daoxiong Wu,Haifeng Lv,Xiaojun Wu,Jinlong Yang","doi":"10.1021/acs.jpclett.5c00802","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00802","url":null,"abstract":"Engineering the topological properties of a quantum anomalous Hall (QAH) insulator is crucial for advancing spintronics and quantum devices. Conventional methods relying on external magnetic fields face limitations in their scalability and energy efficiency. Here, we present the realization of bipolar topological magnetic semiconductor (BTMS) using two-dimensional covalent organic radical frameworks (2D CORFs) based on an orbital-engineering approach. These BTMS host spin-polarized Dirac cones and flat bands with opposite Chern numbers, enabling electrically driven chiral switching of the QAH phase. The triacene(TRI)-CORFs achieve reversible transitions between nontrivial flat-band insulators and QAH phase via carrier doping or heteroatom substitution (e.g., N/B doping), while maintaining robust room-temperature ferromagnetism (TC ≈ 508 K), where the chirality inversion of edge currents is confirmed by Berry curvature analysis. This work establishes 2D CORFs as a versatile platform for electrically tunable topological quantum devices, bridging the gap between organic chemistry and chiral spintronics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"96 1","pages":"5188-5194"},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143991961","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

Dual-Interface Passivation of Wide-Bandgap Perovskite Films for Efficient Four-Terminal Perovskite–Organic Tandem Solar Cells 高效四端钙钛矿-有机串联太阳能电池中宽带隙钙钛矿膜的双界面钝化

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0075610.1021/acs.jpclett.5c00756

Fawad Aslam, Hengyue Li*, Jianhui Chang, Muhammad Tahir, Muhammad Zahid, Muhammad Irfan Sadiq, Xiang Liao, Qiang Zeng, Fangyang Liu and Junliang Yang,

{"title":"Dual-Interface Passivation of Wide-Bandgap Perovskite Films for Efficient Four-Terminal Perovskite–Organic Tandem Solar Cells","authors":"Fawad Aslam, Hengyue Li*, Jianhui Chang, Muhammad Tahir, Muhammad Zahid, Muhammad Irfan Sadiq, Xiang Liao, Qiang Zeng, Fangyang Liu and Junliang Yang, ","doi":"10.1021/acs.jpclett.5c0075610.1021/acs.jpclett.5c00756","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00756https://doi.org/10.1021/acs.jpclett.5c00756","url":null,"abstract":"Interface defects in perovskite solar cells (PSCs) can significantly impair device efficiency by promoting nonradiative recombination, hindering charge transport, and facilitating ion migration. In this work, we introduce a dual-interface passivation strategy utilizing 2-(N-morpholino)ethanesulfonic acid potassium (MESK) and octylammonium iodide (OAI), targeting both the electron transport layer (ETL)/perovskite and perovskite/hole transport layer (HTL) interfaces to enhance the efficiency of wide-bandgap PSCs based on FA0.8Cs0.2Pb(I0.6Br0.4)3 with a bandgap of 1.77 eV. The sulfonic group in MESK passivates bottom interface defects through coordination with Pb ions, while the amine group in OAI interacts with Pb and halide ions to effectively passivate top interface defects. The dual-interface passivation strategy improves perovskite crystallinity, enlarges grain size, and reduces nonradiative recombination. As a result, the performance of PSCs is significantly enhanced, achieving a power conversion efficiency (PCE) of 23.69% in a four-terminal (4T) perovskite–organic tandem solar cell (TSC), which provides a promising and sustainable solution for the commercialization of TSCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5195–5201 5195–5201"},"PeriodicalIF":4.8,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166040","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