The Journal of Physical Chemistry Letters最新文献

Exciton Fine Structure in Axially Symmetric Quantum Dots and Rods of III-V and II-VI Semiconductors. III-V 和 II-VI 半导体轴对称量子点和量子棒中的激子精细结构。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c02800

Serguei V Goupalov

{"title":"Exciton Fine Structure in Axially Symmetric Quantum Dots and Rods of III-V and II-VI Semiconductors.","authors":"Serguei V Goupalov","doi":"10.1021/acs.jpclett.4c02800","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02800","url":null,"abstract":"Both absorption and emission of light in semiconductor quantum dots occur through excitation or recombination of confined electron-hole pairs, or excitons, with tunable size-dependent resonant frequencies that are ideal for applications in various fields. Some of these applications require control over quantum dot shape uniformity, while for others, control over energy splittings among exciton states emitting light in different polarizations and/or between bright and dark exciton states is of key importance. These splittings, known as exciton fine structure, are very sensitive to the nanocrystal shape. Theoretically, nanocrystals of spheroidal shape are often considered, and their nonsphericity is treated perturbatively as stemming from a linear uniaxial deformation of a sphere. Here, we compare this treatment with a nonperturbative model of a cylindrical box, free of any restrictions on the cylinder's aspect ratio. This comparison allows one to understand the limits of validity of the traditional perturbative model and offers insights into the relative importance of various mechanisms controlling the exciton fine structure. These insights are relevant to both colloidal nanocrystals and epitaxial quantum dots of III-V and II-VI semiconductors.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11753-11759"},"PeriodicalIF":4.8,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646532","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

Nanopore Identification of Polyglutamine Length via Cross-Slit Sensing. 通过交叉光斑传感纳米孔鉴定多聚谷氨酰胺长度

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c02681

Changxiong Huang, Huan Chen, Jun Luo, Ninggui Ma, Zhen Li, Xiao Cheng Zeng, Jun Fan

{"title":"Nanopore Identification of Polyglutamine Length via Cross-Slit Sensing.","authors":"Changxiong Huang, Huan Chen, Jun Luo, Ninggui Ma, Zhen Li, Xiao Cheng Zeng, Jun Fan","doi":"10.1021/acs.jpclett.4c02681","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02681","url":null,"abstract":"Nanopore sensing is now reshaping analytical proteomics with its simplicity, convenience, and high sensitivity. Determining the length of polyglutamine (polyQ) is crucial for the rapid screening of Huntington's disease. In this computational study, we present a cross-nanoslit detection approach to determine the polyQ length, where the nanoslit is carved within a two-dimensional (2D) in-plane heterostructure of graphene (GRA) and hexagonal boron nitride (hBN). We designed a heterostructure with an hBN strip embedded in the graphene sheet. With such a design, polyQ peptides can spontaneously and linearly stretch out on the hBN stripe. By tuning the strength of an external in-plane electric field, molecular transportation of polyQ peptides along the hBN stripe can be effectively regulated. Subsequent cross-nanoslit motion can be applied to record time-dependent electric signals. The signal features are then utilized to train the machine learning classification models. The machine-learning-assisted recognition enables accurate determination of the protein's length. This nanoslit-sensing method may offer theoretical guidance on 2D heterostructure design for the detection of polyQ peptide lengths and rapid screening of protein-related diseases.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11792-11800"},"PeriodicalIF":4.8,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646534","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

Self-Powered Broadband Photodetection Ranging from X-ray to UV-Vis Light in a Polar Perovskite Induced by Bulk Photovoltaic Effect. 利用块状光伏效应在极性透镜中实现从 X 射线到紫外可见光的自供电宽带光电探测。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c02567

Panpan Yu, Shihai You, Xitao Liu, Zeng-Kui Zhu, Ying Zeng, Junhua Luo

{"title":"Self-Powered Broadband Photodetection Ranging from X-ray to UV-Vis Light in a Polar Perovskite Induced by Bulk Photovoltaic Effect.","authors":"Panpan Yu, Shihai You, Xitao Liu, Zeng-Kui Zhu, Ying Zeng, Junhua Luo","doi":"10.1021/acs.jpclett.4c02567","DOIUrl":"10.1021/acs.jpclett.4c02567","url":null,"abstract":"Self-powered broadband photodetection has evoked increased interest in next-generation photoelectronic devices. However, realizing self-powered broadband photodetection in a single material is still a challenge because of the harsh requirements, including powerful built-in field, excellent charge transport behaviors, as well as the broad absorption. Herein, we first realize broadband photodetection in the range from X-ray to UV-vis light in a polar two-dimensional perovskite (2-FBA)2MAPb2I7 (2-FBA = 2-fluorobenzylamine, MA = methylamine) by incorporating an aromatic spacer into a three-dimensional prototype. As a result, (2-FBA)2MAPb2I7 exhibited a superior response to UV-vis light (377 to 637 nm) without voltage bias. Specifically, a high switching ratio of 1.05 × 104, an outstanding responsivity (R) of 1420 mA W-1, and detectivity (D*) of 1.59 × 1013 Jones were achieved under light illumination at 520 nm. Moreover, (2-FBA)2MAPb2I7 achieved a high sensitivity of 46.4 μC Gy-1 cm-2 without voltage bias, two times higher than that of a commercial α-Se film detector (20 μC Gy-1 cm-2). The sensitivity can be further improved to 3316 μC Gy-1 cm-2 at a 50 V bias. These results give insight into the design of 2D perovskites for self-powered broadband photodetection.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11767-11772"},"PeriodicalIF":4.8,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646536","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

Photocatalytic Mechanisms of Organic Thermally Activated Delayed Fluorescence Compounds. 有机热激活延迟荧光化合物的光催化机理。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c02670

Jiawen Zhang, Teng-Fei Xiao, Hongmei Zhao, Jie Kong, Zhuoran Kuang, Meng Zhou, Guo-Qiang Xu, Yang Li, Andong Xia

{"title":"Photocatalytic Mechanisms of Organic Thermally Activated Delayed Fluorescence Compounds.","authors":"Jiawen Zhang, Teng-Fei Xiao, Hongmei Zhao, Jie Kong, Zhuoran Kuang, Meng Zhou, Guo-Qiang Xu, Yang Li, Andong Xia","doi":"10.1021/acs.jpclett.4c02670","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02670","url":null,"abstract":"Reverse intersystem crossing (RISC) has become possible by minimizing the energy gap between the first excited singlet (S1) and triplet state (T1), which facilitates the thermally activated delayed fluorescence (TADF). Due to the small singlet-triplet energy gap, the S1 and T1 states exhibit comparable redox reactivity, leading organic TADF compounds to be potent photocatalysts. Here, we report such TADF compounds with multiple donor units designed as an efficient photocatalyst for the direct C(sp3)-H carbamoylation of saturated aza-heterocycles. The results obtained by photophysical investigations and chemical calculations confirm that both the S1 and T1 states are involved in the photocatalysis cycle, with the fast spin-flip from the S1 to triplet states being a crucial factor in the enhancement of catalytic performance. The findings will be beneficial for the design of novel, efficient organic photocatalysis with TADF characteristics and aid in the development of organic photocatalysis.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11784-11791"},"PeriodicalIF":4.8,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646535","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

Effects of Methyl Substitution on the Ultrafast Internal Conversion of Benzene. 甲基取代对苯超快内部转化的影响

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c02859

Kazuki Maeda, Alexie Boyer, Shutaro Karashima, Alexander Humeniuk, Toshinori Suzuki

引用次数: 0

Assessing Melting and Solid-Solid Transition Properties of Choline Chloride via Molecular Dynamics Simulations. 通过分子动力学模拟评估氯化胆碱的熔化和固固转换特性

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c03051

Gabriela B Correa, Dinis O Abranches, Eliseo Marin-Rimoldi, Yong Zhang, Edward J Maginn, Frederico W Tavares

引用次数: 0

Mechanism of Molecular Polariton Decoherence in the Collective Light-Matter Couplings Regime. 分子极化子在光-物质耦合集体状态下的退相干机制。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c03049

Benjamin X K Chng, Wenxiang Ying, Yifan Lai, A Nickolas Vamivakas, Steven T Cundiff, Todd D Krauss, Pengfei Huo

{"title":"Mechanism of Molecular Polariton Decoherence in the Collective Light-Matter Couplings Regime.","authors":"Benjamin X K Chng, Wenxiang Ying, Yifan Lai, A Nickolas Vamivakas, Steven T Cundiff, Todd D Krauss, Pengfei Huo","doi":"10.1021/acs.jpclett.4c03049","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03049","url":null,"abstract":"Molecular polaritons, the hybridization of electronic states in molecules with photonic excitation inside a cavity, play an important role in fundamental quantum science and technology. Understanding the decoherence mechanism of molecular polaritons is among the most significant fundamental questions. We theoretically demonstrate that hybridizing many molecular excitons in a cavity protects the overall quantum coherence from phonon-induced decoherence. The polariton coherence time can be prolonged up to 100 fs with a realistic collective Rabi splitting and quality factor at room temperature, compared to the typical electronic coherence time which is around 15 fs. Our numerically exact simulations and analytic theory suggest that the dominant decoherence mechanism is the population transfer from the upper polariton state to the dark state manifold. Increasing the collective coupling strength will increase the energy gap between these two sets of states and thus prolong the coherence lifetime. We further derived valuable scaling relations that directly indicate how polariton coherence depends on the number of molecules, Rabi splittings, and light-matter detunings.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11773-11783"},"PeriodicalIF":4.8,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646533","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

Polaron Pair-Mediated Radiative Recombination of Singlet Excitons in a Conjugated Polymer Aggregate by Plasmonic and Semiconductor Nanocrystals. 等离子体和半导体纳米晶体在共轭聚合物聚合体中由极龙对介导的单线激子辐射重组。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.jpclett.4c02662

Yeon Gyu Kim, Se Gyo Han, Guanning Shao, Taeyong Ha, Yunmo Sung, Minyoung Jeong, Hyuk Gu Yun, Jeong Yeon Ryu, Dong Hyeon Kim, Bora Kim, Mun Seok Jeong, Sungjee Kim, Young Jin Choi, Young Joon Hong, Kilwon Cho, Dongki Lee

{"title":"Polaron Pair-Mediated Radiative Recombination of Singlet Excitons in a Conjugated Polymer Aggregate by Plasmonic and Semiconductor Nanocrystals.","authors":"Yeon Gyu Kim, Se Gyo Han, Guanning Shao, Taeyong Ha, Yunmo Sung, Minyoung Jeong, Hyuk Gu Yun, Jeong Yeon Ryu, Dong Hyeon Kim, Bora Kim, Mun Seok Jeong, Sungjee Kim, Young Jin Choi, Young Joon Hong, Kilwon Cho, Dongki Lee","doi":"10.1021/acs.jpclett.4c02662","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02662","url":null,"abstract":"We investigated the excited-state dynamics of a conjugated polymer (CP:P3HT)-based ternary hybrid system containing P3HT-coated gold nanoparticles and quantum dots. Transient absorption spectroscopy results revealed that polaron pairs (PPs) originating from nonrelaxed singlet (S1) excitons of the CP aggregate in the ternary system have shorter electron-hole separation distances than those of PPs in the neat CP aggregate because of the photophysical effects of plasmonic and semiconductor nanocrystals. In particular, the shorter electron-hole distances of PPs led to more back-recombination to S1 excitons than dissociation into positive polarons in the ternary system, resulting in increased S1 radiative recombination compared with that in the neat CP system. Thus, the photoluminescence intensity of the CP aggregate in the ternary system increased. Our findings provide new insights into the excited-state dynamics of CPs and pave the way for the development of next-generation high-efficiency optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11806-11814"},"PeriodicalIF":4.8,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666639","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

Predicting Long-Term Stability from Short-Term Measurement: Insights from Modeling Degradation in Perovskite Solar Cells during Voltage Scans and Impedance Spectroscopy. 从短期测量预测长期稳定性：从电压扫描和阻抗谱分析过程中的 Perovskite 太阳能电池退化建模中获得的启示。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-15 DOI: 10.1021/acs.jpclett.4c02343

Will Clarke, Petra Cameron, Giles Richardson

引用次数: 0

Revealing Dynamics and Competitive Mechanism of Gas-Induced Surface Segregation of PdFe_0.08 Dilute Alloy by Multi-Dimensional Imaging. 通过多维成像揭示 PdFe0.08 稀合金气体诱导表面偏析的动力学和竞争机制

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-15 DOI: 10.1021/acs.jpclett.4c02903

Yafeng Zhang, Hong Li, Fang Liu, Mengwei Li, Yong Zhang, Jinming Cai, Yangsheng Li, Fan Yang, Feng Yin, Junling Lu, Tao Zhang, Bing Yang

{"title":"Revealing Dynamics and Competitive Mechanism of Gas-Induced Surface Segregation of PdFe0.08 Dilute Alloy by Multi-Dimensional Imaging.","authors":"Yafeng Zhang, Hong Li, Fang Liu, Mengwei Li, Yong Zhang, Jinming Cai, Yangsheng Li, Fan Yang, Feng Yin, Junling Lu, Tao Zhang, Bing Yang","doi":"10.1021/acs.jpclett.4c02903","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02903","url":null,"abstract":"The restructuring of dilute alloys under gas environments has shown a great impact on their catalytic performance due to intriguing structural sensitivity, but the structural dynamics and underlying mechanism remains elusive. Herein, we directly resolved the distinct dynamic behaviors of PdFe0.08 dilute alloys under CO or O2 environment by multidimensional imaging. The stronger binding of gaseous CO with Fe atoms stimulates Fe segregation out of the PdFe0.08, resulting in 3D growth of Fe islands, whereas the dissociative adsorption of O2 results in 2D layer-by-layer growth of segregated FeO as encapsulation overlayers that bind strongly with the Pd surface underneath. Such varied structures remarkably tune the catalytic activity for CO oxidation, showing a considerably high activity for a CO-treated sample. Our results reveal the competitive mechanism between adsorbate-metal and metal-metal interaction for gas-induced surface segregation, which should be highly considered for the rational design of dilute alloys with dynamically tuned structure and reactivity.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11737-11744"},"PeriodicalIF":4.8,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637933","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