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

Data-Driven Exploration of Critical Factors for Single-Phase High-Entropy Oxide Anode Materials 数据驱动的单相高熵氧化阳极材料关键因素探索

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02225

Moriyuki Kanno*, Toshiaki Taniike and Itaru Honma,

{"title":"Data-Driven Exploration of Critical Factors for Single-Phase High-Entropy Oxide Anode Materials","authors":"Moriyuki Kanno*, Toshiaki Taniike and Itaru Honma, ","doi":"10.1021/acs.jpclett.5c02225","DOIUrl":"10.1021/acs.jpclett.5c02225","url":null,"abstract":"High-entropy oxides (HEOs) are attracting significant attention owing to their compositional tunability and structural robustness. However, the identification of specific compositional combinations that yield a single-phase structure in HEOs remains unclear owing to the immense combinatorial complexity inherent in multielement systems. This study adopts a materials informatics approach that integrates experimental synthesis data with machine learning to identify key compositional factors enabling single-phase HEO formation via solid-state synthesis. This approach extracts compositional rules and constraints favoring the formation of homogeneous rock-salt or spinel phases. Applying these insights allowed the compositional space to be efficiently explored, leading to the successful synthesis of a single-phase cobalt-free HEO exhibiting high reversible capacity and outstanding cycling stability as a lithium-ion battery anode. These findings demonstrate the effectiveness of data-driven methodologies in rational material design and highlight the potential of HEOs as sustainable materials for next-generation energy storage technologies.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9824–9829"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c02225","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026203","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

Tuning the Electrical Property and Electronic Band Structures of Organic Semiconductors via Surface Tension 利用表面张力调谐有机半导体的电学性质和电子能带结构。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c01757

Zonghan Guo, Yunfei Tian, Kai Chen, Xianrong Yuan, Zhonglin Zhang, Qijing Wang*, Yi Shi and Yun Li*,

{"title":"Tuning the Electrical Property and Electronic Band Structures of Organic Semiconductors via Surface Tension","authors":"Zonghan Guo, Yunfei Tian, Kai Chen, Xianrong Yuan, Zhonglin Zhang, Qijing Wang*, Yi Shi and Yun Li*, ","doi":"10.1021/acs.jpclett.5c01757","DOIUrl":"10.1021/acs.jpclett.5c01757","url":null,"abstract":"Stress engineering is an effective way to tune the performance of semiconductors, which has been verified in the work of inorganic and organic single-crystal semiconductors. However, due to the limitations of the vapor-phase growth preparation conditions, the deposited polycrystalline organic semiconductors are more susceptible to residual stress. Therefore, it is of great research significance to develop a low-cost stress engineering applicable to vapor-deposited semiconductors. In this work, we utilized the nonwetting state between water and semiconductors to provide compressive strain to the semiconductors and offset the tensile strain generated during thermal annealing. XRD and UPS measurements revealed that the water-treated films exhibited better crystal quality, lower work function (WF), and higher HOMO levels. These results highlighted the critical role of strain in modulating WF, demonstrating that compressive strain alleviates dynamic disorder and enhances intermolecular coupling. The transistors with water treatment achieved an improved mobility of 6.11 cm2 V–1 s–1 and a better stability. This work provides a feasible, low-cost approach to introduce compressive strain, facilitating the building of high-performance organic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9800–9805"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025718","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

Dissecting the Large Stokes Shift Fluorescence of Graphene-Sheet-Based Carbon Dots by Excitation-Dependent Ultrafast Spectroscopy 用激发相关超快光谱分析石墨烯基碳点的大斯托克斯位移荧光。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02377

Chieh-Hsi Kuan, Xueqiao Zhang, Taylor D. Krueger, Logan S. Lancaster, Cheng Chen, Sanjida Yeasmin, Ahasan Ullah, Li-Jing Cheng and Chong Fang*,

{"title":"Dissecting the Large Stokes Shift Fluorescence of Graphene-Sheet-Based Carbon Dots by Excitation-Dependent Ultrafast Spectroscopy","authors":"Chieh-Hsi Kuan, Xueqiao Zhang, Taylor D. Krueger, Logan S. Lancaster, Cheng Chen, Sanjida Yeasmin, Ahasan Ullah, Li-Jing Cheng and Chong Fang*, ","doi":"10.1021/acs.jpclett.5c02377","DOIUrl":"10.1021/acs.jpclett.5c02377","url":null,"abstract":"Carbon dots (CDs) represent a new class of nontoxic and sustainable nanomaterials with increasing applications. Among them, bright and large Stokes-shift CDs are highly desirable for display and imaging, yet the emission mechanisms remain unclear. We obtained structural signatures for the recently engineered green and red CDs by ground-state femtosecond stimulated Raman spectroscopy (FSRS), then synthesized orange CDs with similar size but much higher nitrogen dopants than red CDs. We implemented femtosecond transient absorption (fs-TA) spectroscopy to capture charge transfer (CT) from the core/edge to surface states on the ∼450 fs time scale via an ultrafast excited-state absorption (ESA) band shift, confirmed by solvent-dependent studies. Subsequently, optical and acoustic phonons contribute to edge-state dynamics after 400 nm excitation, whereas optical phonons become prominent after 500 and 267 nm excitations, unveiling an interplay among the excitation region, exciton–phonon coupling, and energy dissipation. Global analysis and probe-dependent fits corroborate key excited-state dynamics for large-Stokes-shift emissions, revealing a characteristic relaxation pathway toward an excitation-independent single emissive state at surface. These insights enable a bottom-up approach to rationally design and optimize nitrogen-doped CDs for redder and brighter emissions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9806–9814"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025720","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

Tunable Ferroelectricity, Valley Polarization, Layer Polarization, and Magnetism Via Stacking in 2D van der Waals Bilayers 可调谐铁电性、谷极化、层极化和磁性通过在二维范德华双层层中堆叠。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02418

Xiangjie Chen, Mengran Qin, Yonghu Xu, Jifan Wan, Yao He* and Kai Xiong,

引用次数: 0

Van der Waals Epitaxy of CsPbI3/MoS2 Heterojunction Phototransistors for Neuromorphic Computing 神经形态计算用CsPbI3/MoS2异质结光电晶体管的Van der Waals外延

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02548

Rong Lu, Chang Lu, Yanran Li, Honglin Song, Kaiyun Gou, Xiaoming Yuan* and Jie Jiang*,

{"title":"Van der Waals Epitaxy of CsPbI3/MoS2 Heterojunction Phototransistors for Neuromorphic Computing","authors":"Rong Lu, Chang Lu, Yanran Li, Honglin Song, Kaiyun Gou, Xiaoming Yuan* and Jie Jiang*, ","doi":"10.1021/acs.jpclett.5c02548","DOIUrl":"10.1021/acs.jpclett.5c02548","url":null,"abstract":"The optoelectronic properties of perovskite/two-dimensional (2D) material van der Waals heterojunctions provide greater potential for innovative neuromorphic devices. However, the traditional growth of heterojunctions still relies on strict lattice matching and high-temperature processes, which hinder high-quality interface construction and efficient carrier transport. Here, the 2D CsPbI3/MoS2 heterojunction is realized via the van der Waals epitaxy process, overcoming lattice matching limitations. Based on this, a novel neuromorphic 2D/2D CsPbI3/MoS2 heterojunction phototransistor is demonstrated. Its superiority lies in the high-quality stacked heterojunction structure constructed by the van der Waals epitaxy process, which promotes the effective separation of photogenerated carriers. More importantly, the different spiking Boolean logics and Hebbian synaptic learning rules can be modulated by the photoelectrically synergistic strategy. These results indicate that they can not only facilitate neuromorphic electronics but also enable light-tuned spatiotemporal logic dynamics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9830–9838"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026222","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

Efficient Fully-Solution-Processed Inverted Red Quantum Dot Light-Emitting Diodes Enabled by Charge-Exciton Regulation 利用电荷激子调节实现高效全溶液处理的倒红色量子点发光二极管。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02394

Tong Zhang, Zongming Chang, Yixian Wu, Mingming Zhou, Boyu Zhou, Yuhan Jiang and Yanping Wang*,

{"title":"Efficient Fully-Solution-Processed Inverted Red Quantum Dot Light-Emitting Diodes Enabled by Charge-Exciton Regulation","authors":"Tong Zhang, Zongming Chang, Yixian Wu, Mingming Zhou, Boyu Zhou, Yuhan Jiang and Yanping Wang*, ","doi":"10.1021/acs.jpclett.5c02394","DOIUrl":"10.1021/acs.jpclett.5c02394","url":null,"abstract":"Inverted quantum dot light-emitting diodes (QLEDs) show great promise for next-generation displays due to their compatibility with integrated circuit architectures. However, their development has been hindered by inefficient exciton utilization and charge transport imbalance. Here, we present a strategy for regulating charge-exciton dynamics through the rational design of a multifunctional hole transport layer (HTL), incorporating polyethylenimine ethoxylated (PEIE) as a protective interlayer in fully-solution-processed inverted red QLEDs. This HTL comprises poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-(4,4′-(N-(4-butylphenyl)] (TFB) doped with iridium(III) bis(2-methyldibenzo[f,h]quinoxaline) acetylacetonate (Ir(MDQ)2(acac)) and performs three critical functions: facilitating Förster resonance energy transfer to quantum dots, enabling Coulomb-assisted hole injection, and suppressing nonradiative recombination. The optimized inverted red QLEDs at a 5 wt % Ir(MDQ)2(acac) doping concentration achieved a record external quantum efficiency (EQE) of approximately 24.5% and an operational lifetime (T50) exceeding 24,600 h at 100 cd m–2. This work establishes fundamental design principles for high-performance inverted QLEDs, highlighting the crucial role of charge-exciton management in advancing optoelectronic device performance.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9785–9790"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025719","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

Pressure-Driven Structural and Optoelectronic Tuning of Cl-Substituted 2D Lead Halide Perovskite (ClPMA)2PbI4 cl取代2D卤化铅钙钛矿（ClPMA）2PbI4的压力驱动结构和光电子调谐。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02337

Muhammad Azeem, Jinhyuk Choi, Yeonhak Jung and Yongjae Lee*,

{"title":"Pressure-Driven Structural and Optoelectronic Tuning of Cl-Substituted 2D Lead Halide Perovskite (ClPMA)2PbI4","authors":"Muhammad Azeem, Jinhyuk Choi, Yeonhak Jung and Yongjae Lee*, ","doi":"10.1021/acs.jpclett.5c02337","DOIUrl":"10.1021/acs.jpclett.5c02337","url":null,"abstract":"We present a systematic high-pressure investigation of the chlorine-functionalized two-dimensional hybrid perovskite (ClPMA)2PbI4, integrating in situ high-pressure synchrotron powder X-ray diffraction (HP-PXRD), photoluminescence spectroscopy (HP-PL), and first-principles density functional theory (DFT) calculations. Under hydrostatic compression up to 6.18 (±0.42) GPa, HP-PXRD reveals anisotropic lattice contraction (Δa/a0 = 4.06%, Δb/b0 = 3.00%, Δc/c0 = 8.66%) with a bulk modulus of 16.8 (±1.5) GPa (K0 = 34.1 TPa–1) and the onset of amorphization near 6.18 (±0.42) GPa. DFT-optimized structures corroborate progressive PbI6 octahedral flattening leading to reduced interlayer spacing and enhanced Cl···I, Cl···H, and I···H interactions. The full elastic tensor indicates moderate anisotropy (AE = 2.1, AG = 2.63) yet large Poisson’s ratios (−0.196 to 0.67), unveiling coexisting auxetic and elastic deformation pathways. HP-PL spectra exhibit a continuous red shift from 525.2 nm to ∼630.5 nm and intensity quenching, attributable to bond-contraction-induced bandgap narrowing and pressure-enhanced nonradiative recombination in the partially amorphous matrix. DFT band-structure calculations confirmed the pressure-dependent direct-gap evolution and maintaining k-space valence-band maximum and conduction-band minimum alignment. These findings elucidate the structural, mechanical, and optoelectronic tunability of (ClPMA)2PbI4, underscoring its promise for strain-engineered optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9791–9799"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025898","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

Ultra-High Zinc Utilization Enabled by MXene Anode for Flexible Dual-Plating Zn–Br2 Microbatteries MXene阳极用于柔性双镀Zn-Br2微电池的超高锌利用率

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02342

Bin Wang, Guoliang Ma, Le Yu, Jiangqi Zhao* and Zifeng Lin*,

{"title":"Ultra-High Zinc Utilization Enabled by MXene Anode for Flexible Dual-Plating Zn–Br2 Microbatteries","authors":"Bin Wang, Guoliang Ma, Le Yu, Jiangqi Zhao* and Zifeng Lin*, ","doi":"10.1021/acs.jpclett.5c02342","DOIUrl":"10.1021/acs.jpclett.5c02342","url":null,"abstract":"Aqueous zinc-ion microbatteries exhibit promising prospects for wearable devices due to their high safety and cost-effectiveness but face challenges such as low energy density and short cycle life. To address these challenges, a dual-plating flexible Zn–Br2 microbattery was developed using freestanding MXene films as a zinc metal free anode. The MXene anode retains no redundant Zn, as Zn2+ from the electrolyte undergoes deposition/stripping reactions on its substrate, thereby eliminating the necessity for excess zinc. Compared to Zn anode, it exhibits significantly reduced mass while achieving enhanced depth of discharge and markedly ultrahigh zinc utilization efficiency. The MXene anode can in situ form a ZnF2-rich layer and exhibits low solvation energy, excellent hydrophilicity, and mechanical properties. Leveraging these properties, the MXene anode demonstrates low nucleation overpotential (2.8 mV) and remarkable cycling stability (970 h). More importantly, assembled Zn–Br2 microbatteries show 6000-cycle stability, flexibility, high energy density, and advance wearable energy storage.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9839–9848"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026201","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 into the Regulation of Ag NPs/ZnO NRs/GaN Heterostructure SERS Substrate via Pyroelectric Effects Ag NPs/ZnO NRs/GaN异质结构SERS衬底的热释电调控研究

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02332

Wanning Dou, Mingrui Shao, Chang Ji, Yang Wu, Shaoqi Deng, Zhen Li, Jing Yu, Chao Zhang, Shouzhen Jiang*, Xiaofei Zhao* and Yingying Ren*,

{"title":"Investigation into the Regulation of Ag NPs/ZnO NRs/GaN Heterostructure SERS Substrate via Pyroelectric Effects","authors":"Wanning Dou, Mingrui Shao, Chang Ji, Yang Wu, Shaoqi Deng, Zhen Li, Jing Yu, Chao Zhang, Shouzhen Jiang*, Xiaofei Zhao* and Yingying Ren*, ","doi":"10.1021/acs.jpclett.5c02332","DOIUrl":"10.1021/acs.jpclett.5c02332","url":null,"abstract":"Heterostructures have emerged as promising contenders for surface-enhanced Raman scattering (SERS) applications. Nevertheless, the construction of a composite SERS substrate with well-matched energy levels persists as a challenge, primarily due to the restricted selection of SERS-active materials. In this study, we successfully synthesized a Ag nanoparticles (NPs)/ZnO nanorods (NRs)/GaN heterojunction featuring type II staggered energy bands, which provides an outstanding platform for efficient SERS detection. Moreover, considering that both ZnO and GaN are pyroelectric semiconductor materials, the pyroelectric potential generated at the ZnO and GaN heterojunctions improves energy level matching. This, in turn, promotes charge transfer within the composite structure and substantially enhances the chemical enhancement of SERS. Under the modulation of pyroelectricity, the SERS signal intensity of rhodamine 6G (R6G) increased by approximately 15-fold, and the detection limit decreased by at least 2 orders of magnitude. Additionally, the substrate exhibited the capability to detect pollutants, such as 20 nm nanoplastics and thiram, indicating its significant potential for environmental monitoring.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 37","pages":"9856–9863"},"PeriodicalIF":4.6,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026204","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

Protonation Enables Durable and Efficient Water Oxidation on Commercial TiO2/IrO2 质子化使商业TiO2/IrO2持久有效的水氧化。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-10 DOI: 10.1021/acs.jpclett.5c02227

Da Huang, Yu Du, Haoyang Hu, Shicheng Yan* and Zhigang Zou,

引用次数: 0