The Journal of Physical Chemistry Letters最新文献

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Bayesian Optimization with Gaussian Processes Assisted by Deep Learning for Material Designs. 基于深度学习的高斯过程贝叶斯优化材料设计。
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-18 DOI: 10.1021/acs.jpclett.5c00592
Shin Kiyohara,Yu Kumagai
{"title":"Bayesian Optimization with Gaussian Processes Assisted by Deep Learning for Material Designs.","authors":"Shin Kiyohara,Yu Kumagai","doi":"10.1021/acs.jpclett.5c00592","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00592","url":null,"abstract":"Machine learning (ML) approaches have become ubiquitous in the search for new materials in recent years. Bayesian optimization (BO) based on Gaussian processes (GPs) has become a widely recognized approach in material exploration. However, feature engineering has critical impacts on the efficiency of GP-based BO, because GPs cannot automatically generate descriptors. To address this limitation, this study applies deep kernel learning (DKL), which combines a neural network with a GP, to BO. The efficiency of the DKL model was comparable to or significantly better than that of a standard GP in a data set of 922 oxide data sets, covering band gaps, ionic dielectric constants, and effective masses of electrons, as well as in experimental data sets, the band gaps of 610 hybrid organic-inorganic perovskite alloys. When searching for the alloy with the highest Curie temperature among 4560 alloys, the standard GP outperformed the DKL model because a strongly correlated descriptor of the Curie temperature could be directly utilized. Additionally, DKL supports transfer learning, which further enhances its efficiency. Thus, we believe that BO based on DKL paves the way for exploring diverse material spaces more effectively than GPs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"78 1","pages":"5244-5251"},"PeriodicalIF":6.475,"publicationDate":"2025-05-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087737","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
The Onset for Vibrationally Induced, Intramolecular Proton Transfer at Three Water Molecules in Microhydrated 4-Aminobenzoic Acid. 微水合4-氨基苯甲酸中三个水分子振动诱导的分子内质子转移的开始。
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-18 DOI: 10.1021/acs.jpclett.5c00701
Abhijit Rana,Payten A Harville,Thien Khuu,R Allen LaCour,Teresa Head-Gordon,Mark A Johnson
{"title":"The Onset for Vibrationally Induced, Intramolecular Proton Transfer at Three Water Molecules in Microhydrated 4-Aminobenzoic Acid.","authors":"Abhijit Rana,Payten A Harville,Thien Khuu,R Allen LaCour,Teresa Head-Gordon,Mark A Johnson","doi":"10.1021/acs.jpclett.5c00701","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00701","url":null,"abstract":"Protonation of 4-aminobenzoic acid occurs at either the amino group (the N-protomer, N) or at the carboxylic acid C═O group (the O-protomer or O). N lies higher in energy than O in the isolated ion but becomes the more stable of the 4ABAH+·(H2O)n clusters in the size range n ∼ 5. We report the size-dependent onset of intramolecular proton transfer upon vibrational excitation of cold (20 K), size-selected 4ABAH+·(H2O)n clusters in a cryogenically cooled ion trap. The onset occurs with three water molecules, which are retained after protomer interconversion. While we do not definitively identify a mechanism for the transfer, path integral molecular dynamics simulations indicate that it may proceed by proton shuttling across a bridge of at least three water molecules. By capturing protomer interconversion in a closed, finite system with well-defined internal energy, we provide a useful benchmark for furthering our understanding of water-mediated proton transport.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"54 1","pages":"5252-5257"},"PeriodicalIF":6.475,"publicationDate":"2025-05-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087736","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
Photoinduced Dissociation of Halobenzenes: Nonadiabatic Molecular Dynamics Simulations Reveal Key Pathways 光致卤苯解离:非绝热分子动力学模拟揭示关键途径
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-17 DOI: 10.1021/acs.jpclett.5c00622
Donghwan Im, Alekos Segalina, Hyotcherl Ihee
{"title":"Photoinduced Dissociation of Halobenzenes: Nonadiabatic Molecular Dynamics Simulations Reveal Key Pathways","authors":"Donghwan Im, Alekos Segalina, Hyotcherl Ihee","doi":"10.1021/acs.jpclett.5c00622","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00622","url":null,"abstract":"Aryl halides are prototypical molecules for studying photodissociation, yet the role of spin–orbit coupling (SOC) in their dynamics remains incompletely understood. Using state-of-the-art <i>ab initio</i> calculations and excited-state dynamics simulations, we explore the photodissociation pathways of iodobenzene (PhI) and bromobenzene (PhBr). For PhI, two dissociation pathways, direct and indirect modes, are identified, consistent with gas-phase experiments. In contrast, photodissociation of PhBr occurs only after overcoming the energy barrier between bound and repulsive states, which requires activation of specific vibrational modes, particularly those associated with boat-like out-of-plane motion. While previous studies have suggested that SOC primarily accelerates intersystem crossing and photodissociation in heavier halogens, our results show that, in addition to SOC, the activation of specific vibrational modes also plays a crucial role in the dissociation process. These findings enhance our understanding of how SOC influences excited-state dynamics, providing insight into controlling photochemical reactivity in halogenated organic compounds.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"206 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144067274","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
Synergistic Surface Reconstruction and Defect Passivation via Guanidine Sulfonate for High-Efficiency Perovskite Photovoltaics 高效钙钛矿光伏的胍磺酸盐协同表面重构和缺陷钝化
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-17 DOI: 10.1021/acs.jpclett.5c01155
Shuai Xu, Yanqiang Hu, Yiqiong Zhang, Jiapei Xu, Qiang Huang, Jing Li, Minmin Wang
{"title":"Synergistic Surface Reconstruction and Defect Passivation via Guanidine Sulfonate for High-Efficiency Perovskite Photovoltaics","authors":"Shuai Xu, Yanqiang Hu, Yiqiong Zhang, Jiapei Xu, Qiang Huang, Jing Li, Minmin Wang","doi":"10.1021/acs.jpclett.5c01155","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01155","url":null,"abstract":"Perovskite films have long suffered from various defects located at grain boundaries and surfaces (GBS), especially residual lead iodide (PbI<sub>2</sub>), which can seriously impair the photoelectric conversion efficiency (PCE) and long-term stability of the corresponding photovoltaic devices. Herein, guanidine sulfamate (GSM), with desired −NH<sub>2</sub>, S═O, and Gua<sup>+</sup> functional groups, is introduced to the perovskite surface by a post-treatment process to achieve high-quality films with fewer defects. It was found that −NH<sub>2</sub> and S═O in GSM contribute to the passivation of various defects in perovskites and suppress non-radiative recombination, thus improving the interfacial carrier transport efficiency. Meanwhile, the guanidine (Gua<sup>+</sup>) cations promote grain fusion during post-treatment to achieve large-sized grains and effectively reduce residual PbI<sub>2</sub> content. Moreover, the optimized perovskite films also exhibited better energy level alignment and surface hydrophobicity. Consequently, the champion PCE of the optimized perovskite solar cells (PSCs) was increased from 21.69 to 23.85% at the appropriate GMS post-treatment concentration, along with a significant improvement in storage stability and light stability.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"54 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144067512","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
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 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c00914
Rong-Yao Gao,Yan-Ping Shi,Jian-Wei Zou,Dan-Hong Li,Hao-Yi Wang,Junrong Zheng,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,Jian-Ping Zhang","doi":"10.1021/acs.jpclett.5c00914","DOIUrl":"https://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":"14 1","pages":"5144-5152"},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143982510","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
The Influence of Passivating Ligand Identity on Au25(SR)18 Spin-Polarized Emission 钝化配体对Au25(SR)18自旋极化发射的影响
IF 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0072310.1021/acs.jpclett.5c00723
Nathanael L. Smith, Patrick J. Herbert, Marcus A. Tofanelli, Jane A. Knappenberger, Christopher J. Ackerson and Kenneth L. Knappenberger Jr.*, 
{"title":"The Influence of Passivating Ligand Identity on Au25(SR)18 Spin-Polarized Emission","authors":"Nathanael L. Smith,&nbsp;Patrick J. Herbert,&nbsp;Marcus A. Tofanelli,&nbsp;Jane A. Knappenberger,&nbsp;Christopher J. Ackerson and Kenneth L. Knappenberger Jr.*,&nbsp;","doi":"10.1021/acs.jpclett.5c0072310.1021/acs.jpclett.5c00723","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00723https://doi.org/10.1021/acs.jpclett.5c00723","url":null,"abstract":"<p >Magnetic circular photoluminescence (MCPL) spectra were collected following 3.1 eV excitation of two ligand-passivated Au<sub>25</sub>(SR)<sub>18</sub> monolayer-protected clusters (MPCs). Both clusters generated spin-polarized emission; however, the degree of circular polarization noted for Au<sub>25</sub>(SC<sub>8</sub>H<sub>9</sub>)<sub>18</sub>, which was passivated with the aromatic phenylethanethiol ligand, was 5× that obtained for Au<sub>25</sub>(SC3)<sub>18</sub>, whose passivating ligand was aliphatic. Variable-magnetic field data were analyzed to determine Landé g-factors and spectroscopic term symbols for observable transitions contributing to the clusters’ MCPL spectra. For Au<sub>25</sub>(PET)<sub>18</sub>, transitions originated from one doublet and two quartet fine-structure superatomic electronic states; by comparison, the Au<sub>25</sub>(SC3)<sub>18</sub> spectrum contained only two components, both of which arose from doublet superatomic electronic states. Additionally, Faraday B-term contributions, which report on field-induced mixing, were more pronounced for Au<sub>25</sub>(SC3)<sub>18</sub> spectral components. Therefore, the decreased spin-polarized emission by Au<sub>25</sub>(SC3)<sub>18</sub> was attributed to stronger coupling to nonradiative decay channels. These results suggest the Au<sub>25</sub>(SR)<sub>18</sub> cluster’s passivating ligand can be used to tune the relative populations of emissive fine-structure states, the extent of mixing between radiative and nonradiative states, and the amplitude of spin-polarized emission in MPCs.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 20","pages":"5168–5172 5168–5172"},"PeriodicalIF":4.8,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104960","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
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 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c00576
Robert P C Bauer,Danny Rodriguez,Santanu Pathak,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,John S Tse","doi":"10.1021/acs.jpclett.5c00576","DOIUrl":"https://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":"75 1","pages":"5160-5167"},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143991959","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 4.8 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c0108510.1021/acs.jpclett.5c01085
Riu Riu Wary, Abinash Das*, Emir S. Amirov, Dongyu Liu, Shriya Gumber, Elena A. Kazakova, Andrey S. Vasenko and 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,&nbsp;Abinash Das*,&nbsp;Emir S. Amirov,&nbsp;Dongyu Liu,&nbsp;Shriya Gumber,&nbsp;Elena A. Kazakova,&nbsp;Andrey S. Vasenko and Oleg V. Prezhdo*,&nbsp;","doi":"10.1021/acs.jpclett.5c0108510.1021/acs.jpclett.5c01085","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01085https://doi.org/10.1021/acs.jpclett.5c01085","url":null,"abstract":"<p >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<sup>–2</sup> 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.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 20","pages":"5180–5187 5180–5187"},"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.5c01085","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104959","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
The Influence of Passivating Ligand Identity on Au25(SR)18 Spin-Polarized Emission. 钝化配体对Au25(SR)18自旋极化发射的影响。
IF 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c00723
Nathanael L Smith,Patrick J Herbert,Marcus A Tofanelli,Jane A Knappenberger,Christopher J Ackerson,Kenneth L Knappenberger
{"title":"The Influence of Passivating Ligand Identity on Au25(SR)18 Spin-Polarized Emission.","authors":"Nathanael L Smith,Patrick J Herbert,Marcus A Tofanelli,Jane A Knappenberger,Christopher J Ackerson,Kenneth L Knappenberger","doi":"10.1021/acs.jpclett.5c00723","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00723","url":null,"abstract":"Magnetic circular photoluminescence (MCPL) spectra were collected following 3.1 eV excitation of two ligand-passivated Au25(SR)18 monolayer-protected clusters (MPCs). Both clusters generated spin-polarized emission; however, the degree of circular polarization noted for Au25(SC8H9)18, which was passivated with the aromatic phenylethanethiol ligand, was 5× that obtained for Au25(SC3)18, whose passivating ligand was aliphatic. Variable-magnetic field data were analyzed to determine Landé g-factors and spectroscopic term symbols for observable transitions contributing to the clusters' MCPL spectra. For Au25(PET)18, transitions originated from one doublet and two quartet fine-structure superatomic electronic states; by comparison, the Au25(SC3)18 spectrum contained only two components, both of which arose from doublet superatomic electronic states. Additionally, Faraday B-term contributions, which report on field-induced mixing, were more pronounced for Au25(SC3)18 spectral components. Therefore, the decreased spin-polarized emission by Au25(SC3)18 was attributed to stronger coupling to nonradiative decay channels. These results suggest the Au25(SR)18 cluster's passivating ligand can be used to tune the relative populations of emissive fine-structure states, the extent of mixing between radiative and nonradiative states, and the amplitude of spin-polarized emission in MPCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"26 1","pages":"5168-5172"},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143991956","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 6.475 2区 化学
The Journal of Physical Chemistry Letters Pub Date : 2025-05-15 DOI: 10.1021/acs.jpclett.5c01092
Jiajia Zhang,Xinhao Duan,Zhuang Hu,Xiang Li,Lin Zhang,Shuisheng Chen
{"title":"Intrinsic Defect Tolerance in Inorganic Tin-Lead Perovskites.","authors":"Jiajia Zhang,Xinhao Duan,Zhuang Hu,Xiang Li,Lin Zhang,Shuisheng Chen","doi":"10.1021/acs.jpclett.5c01092","DOIUrl":"https://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":"30 1","pages":"5208-5212"},"PeriodicalIF":6.475,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144065658","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
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