The Journal of Physical Chemistry Letters最新文献_第2页

Synergistic SERS Enhancement in Ag NW/WSe2 Heterostructures: Interfacial Charge Transfer and Layer-Dependent Sensitivity Ag NW/WSe2异质结构的协同SERS增强：界面电荷转移和层相关灵敏度

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-09 DOI: 10.1021/acs.jpclett.6c03177

Liu Lu,Shibo Yan,Xuelian Wu,Zongbao Shen,Yunkun Wu,Xifeng Ren

引用次数: 0

Single-Ion Hydration Through the Lens of Data-Driven Many-Body Potentials 数据驱动多体电位透镜下的单离子水合作用

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-09 DOI: 10.1021/acs.jpclett.6c02987

Francesco Paesani,Suman Saha,Richa Rashmi,Henry Agnew,Xuanyu Zhu,Olivia Zhou

引用次数: 0

Curvature Rebuilt d-Orbital Energy Levels of TM@g-C6N6 Nanotubes for Water-Splitting Enhancement 曲率重建的d轨道能级TM@g-C6N6纳米管的水分裂增强

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-09 DOI: 10.1021/acs.jpclett.6c03181

Jian Yang,Lintao Xu,Jiacai Nie,Yu Yang,Xiumei Wei,Ruifen Dou

{"title":"Curvature Rebuilt d-Orbital Energy Levels of TM@g-C6N6 Nanotubes for Water-Splitting Enhancement","authors":"Jian Yang,Lintao Xu,Jiacai Nie,Yu Yang,Xiumei Wei,Ruifen Dou","doi":"10.1021/acs.jpclett.6c03181","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c03181","url":null,"abstract":"Precisely constructing transition metal (TM) active sites in two-dimensional materials can enhance water splitting, whereas the role of geometric factors such as interfacial curvature remains poorly understood. Nanotubes (NTs) provide a well-defined curved architecture that can modulate electron interactions and reactivity. Here, we rationally design a series of TM@g-C6N6 NTs and use first-principles calculations assisted by machine learning to elucidate how dimensional reduction and curvature govern water-splitting activity. We find that reduced curvature radius systematically promotes water splitting. Notably, the Ir/Rh-decorated g-C6N6 NTs show remarkable electrocatalytic performance with calculated overpotentials of 0.05 eV for the hydrogen evolution reaction and 0.20 eV for the oxygen evolution reaction. Curvature-induced confinement drives reconstruction and reoccupation of the d-orbital states near the Fermi level upon transitioning from a flat plane to a tubular geometry. More importantly, for different reaction intermediates, we identify a curvature-dependent inversion of the dominant adsorption orbital transition from the dz2 to the dx2–y2, which directly correlates with enhanced catalytic activity. Our results establish interfacial curvature as a key manipulator for tuning electronic structure and water-splitting reactivity in TM@g-C6N6 NT single-atom catalysts and provide a new perspective on modulating electronic and catalytic properties in TM@g-C6N6 NT-like structures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"78 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368351","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

Acid-Etched Lead Telluride with Defect-Regulated Surfaces Enables Efficient Mechanical-Energy-Driven Nitrogen Fixation 酸蚀碲化铅与缺陷调节表面使高效的机械能驱动的固氮

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-09 DOI: 10.1021/acs.jpclett.6c03171

Hongda Zhu,Zheng Wu,Luohong Zhang,Siqi Hong,Huijuan Li,Huilin You,Shuangzhe Lu,Zixuan Cheng,Gangqiang Zhu,Qingping Wang,Zhenxiang Cheng,Yanmin Jia

{"title":"Acid-Etched Lead Telluride with Defect-Regulated Surfaces Enables Efficient Mechanical-Energy-Driven Nitrogen Fixation","authors":"Hongda Zhu,Zheng Wu,Luohong Zhang,Siqi Hong,Huijuan Li,Huilin You,Shuangzhe Lu,Zixuan Cheng,Gangqiang Zhu,Qingping Wang,Zhenxiang Cheng,Yanmin Jia","doi":"10.1021/acs.jpclett.6c03171","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c03171","url":null,"abstract":"Ambient ammonia synthesis is important for carbon neutrality. Tribo-electro-catalysis, which converts mechanical friction into chemical driving force through contact electrification and charge transfer, offers a route for nitrogen (N2) fixation. However, inefficient utilization of friction-induced charges and insufficient N2 activation remain major challenges. Herein, acid-etching defect engineering regulates the surface and electronic structures of lead telluride (PbTe) for N2 fixation. The catalyst etched for 90 min exhibits the enhanced activity under dark ambient conditions, delivering ammonium (NH4+) production rates of 258.98 and 329.60 μmol L–1·g–1·h–1 without and with 10 vol % methanol, respectively. Analyses reveal that etching reconstructs the surface, generates defect sites, facilitates N2 adsorption and activation, and promotes friction-induced charge utilization. Excessive etching decreases activity. Charge-trapping and electron paramagnetic resonance measurements support the role of friction-induced negative charges, establishing defect-mediated charge regulation as an effective strategy for sustainable ammonia synthesis.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"17 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368345","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

Influence of Crystal Structure and Shape Anisotropies on Valence-Band States of InP Colloidal Nanocrystals: Application of the xyz Algorithm 晶体结构和形状各向异性对InP胶体纳米晶体价带态的影响：xyz算法的应用

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-09 DOI: 10.1021/acs.jpclett.6c03306

Mikhail O. Nestoklon,Serguei V. Goupalov

引用次数: 0

In Situ EPR Spectroscopy to Track Gas Exchange Kinetics in Porous Liquids under Variable Gas Pressure 原位EPR光谱法跟踪可变气体压力下多孔液体中的气体交换动力学

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-09 DOI: 10.1021/acs.jpclett.6c03098

Ramis Zhitkeyev,Artem S. Poryvaev,Konstantin V. Zaitsev,Dmitry V. Alimov,Anton Yu. Shabalin,Sergey A. Prikhod’ko,Nicolay Yu. Adonin,Renad Z. Sagdeev,Matvey V. Fedin

{"title":"In Situ EPR Spectroscopy to Track Gas Exchange Kinetics in Porous Liquids under Variable Gas Pressure","authors":"Ramis Zhitkeyev,Artem S. Poryvaev,Konstantin V. Zaitsev,Dmitry V. Alimov,Anton Yu. Shabalin,Sergey A. Prikhod’ko,Nicolay Yu. Adonin,Renad Z. Sagdeev,Matvey V. Fedin","doi":"10.1021/acs.jpclett.6c03098","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c03098","url":null,"abstract":"Porous liquids (PLs) are novel promising materials, which demand development of informative spectroscopic tools to track their functioning in situ and operando. In this work we demonstrate in situ electron paramagnetic resonance (EPR) spectroscopy as a versatile method to investigate variable-pressure gas exchange in PLs of the third type based on metal–organic frameworks (MOFs) and sterically excluded solvents. The use of permanently encapsulated in-MOF spin probes (stable nitroxide radicals) allows tracking evolution of EPR spectral shapes under applied gas pressure, and following theoretical analysis reveals contributions of gas exchange kinetics in MOF particles, gas diffusion through the bulk sample and gas dissolution in PL. We exemplify this approach with two PLs based on MOF ZIF-8 dispersed in dibutyl phthalate or ionic liquid [Bmim]BF4. In both PL examples EPR provides unique information on gas exchange kinetics (air-to-CO2 and CO2-to-air) vs pressure in situ, which is indispensable for adjusting target functioning of PLs and their applications in future.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"25 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368350","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

Distinct Plasmonic and Electronically Mediated Pathways for Vibrational Excitation 振动激发的不同等离子体和电子介导途径

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-07 DOI: 10.1021/acs.jpclett.6c02827

Bing Gao,Jameel Damoah,Wassie M. Takele,Terefe G. Habteyes

{"title":"Distinct Plasmonic and Electronically Mediated Pathways for Vibrational Excitation","authors":"Bing Gao,Jameel Damoah,Wassie M. Takele,Terefe G. Habteyes","doi":"10.1021/acs.jpclett.6c02827","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02827","url":null,"abstract":"Understanding how plasmonic energy is transferred into molecular vibrations at metal–molecule interfaces is essential for controlling plasmon-driven chemistry and surface-enhanced spectroscopies. However, distinguishing vibrational excitation mediated by electronic transitions and vibronic coupling (VC) from plasmon-enhanced Raman vibrational pumping (PERVP) remains challenging because both mechanisms generate nonequilibrium vibrational populations. Here, we combine cryogenic surface-enhanced Raman scattering with controlled surface chemistry to investigate these competing excitation pathways using thionine adsorbed on gold nanostructures. Citrate-stabilized gold nanoparticles exhibit two distinct excitation regimes. The first is characterized by unusually intense anti-Stokes scattering despite weak Stokes emission, with laser-power dependences inconsistent with conventional vibrational pumping. This behavior is attributed to VC facilitated by molecular adsorption geometries that favor metal–molecule electronic coupling and transient charge transfer. The second regime exhibits strong Stokes scattering and superlinear anti-Stokes intensity, consistent with PERVP and molecular optomechanics. In contrast, bromide-containing gold nanorods exhibit a single excitation regime with laser-power dependences closely matching theoretical predictions for PERVP, suggesting preferential molecular dipole alignment with the localized plasmonic field. At cryogenic temperatures, pronounced anti-Stokes blinking and the transient activation of weak or Raman-inactive vibrational modes further reveal dynamic interfacial restructuring associated with bromide adsorption. These findings demonstrate how molecular orientation, interfacial electronic coupling, and surface chemistry influence the dominant vibrational excitation pathway, providing a framework for controlling plasmonic energy transfer at metal–molecule interfaces.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360286","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

Divergent Ultrafast Carrier-Density and Photoconductivity Dynamics in Antimony-Doped Halide Perovskite Thin Films 掺锑卤化物钙钛矿薄膜的发散超快载流子密度和光电导率动力学

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-07 DOI: 10.1021/acs.jpclett.6c02812

Yujie Wo,Folusho Helen Balogun,Marcin Giza,Jack Woolley,Edward Butler-Caddle,Nathaniel P. Gallop,Pablo Docampo,Rebecca L. Milot

{"title":"Divergent Ultrafast Carrier-Density and Photoconductivity Dynamics in Antimony-Doped Halide Perovskite Thin Films","authors":"Yujie Wo,Folusho Helen Balogun,Marcin Giza,Jack Woolley,Edward Butler-Caddle,Nathaniel P. Gallop,Pablo Docampo,Rebecca L. Milot","doi":"10.1021/acs.jpclett.6c02812","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02812","url":null,"abstract":"Heterovalent ion substitution can tune the optoelectronic properties of metal halide perovskites, but its impact on charge-carrier recombination and transport remain poorly understood. Here, we investigate antimony incorporation in methylammonium lead iodide (MAPI) thin films using complementary ultrafast spectroscopy techniques. Optical absorption shows that the bandgap remains approximately 1.61 eV across substitution levels up to 10%, whereas photoluminescence and transient absorption (TA) spectroscopy reveal increasing nonradiative recombination rates with increasing antimony content. Optical pump–terahertz probe (OPTP) spectroscopy further uncovers fluence-dependent dynamics distinct from TA that are absent in pristine MAPI. After considering alternative mechanisms, we interpret this behavior as consistent with partially heterogeneous transport, in which Sb3+ incorporation may introduce low-mobility, defect-rich regions within a higher-mobility crystalline network. Thus, heterovalent substitution can introduce hidden transport losses without changing optical bandgap, highlighting the importance of mobility-sensitive measurements to probe doped perovskite films.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"13 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360289","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

Controlled Growth and Disorder Mitigation of GaAs1–xSbx/InAs Core–Shell Quantum Wires GaAs1-xSbx /InAs核壳量子线的受控生长和无序缓解

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-06 DOI: 10.1021/acs.jpclett.6c02953

Ran Zhuo,Huading Song,Yanlin Wu,Wenlong Yang,Haiyan Shi,Xiyu Hou,Sijun Chen,Zhichuan Wang,Donghai Li,Jinjin Bai,Runan Shang,Hao Zhang,Dong Pan

{"title":"Controlled Growth and Disorder Mitigation of GaAs1–xSbx/InAs Core–Shell Quantum Wires","authors":"Ran Zhuo,Huading Song,Yanlin Wu,Wenlong Yang,Haiyan Shi,Xiyu Hou,Sijun Chen,Zhichuan Wang,Donghai Li,Jinjin Bai,Runan Shang,Hao Zhang,Dong Pan","doi":"10.1021/acs.jpclett.6c02953","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02953","url":null,"abstract":"We report the growth and transport properties of GaAs1–xSbx/InAs core–shell nanowires. Compared with the well-studied GaAs-InAs system, incorporating Sb substantially reduces the lattice mismatch between the core and shell. Accordingly, both the nanowire crystal quality and device performance improved significantly. Increasing x from 0.15 to 0.35, the density of crystalline defects, such as stacking faults in the InAs shell, decreases by half. Moreover, the field-effect mobility increases from 3850 cm2/(V s) to 4800 cm2/(V s), consistent with the reduction of the lattice mismatch. The incorporation of Sb makes the nanowire easier to pinch off via the gate voltage, enhancing the electric field tunability over the nanowire. Magneto-conductance measurements reveal Aharonov-Bohm-like oscillations, suggesting a phase-coherent tubular InAs shell. Our results identify lattice mismatch as a critical disorder source in core–shell nanowires and provide a practical route toward low-disorder core–shell quantum devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360287","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

Optical Absorption and Exciton Dispersion of Bulk Corrugated g-C3N4 块状波纹g-C3N4的光吸收和激子色散

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-11-06 DOI: 10.1021/acs.jpclett.6c03327

Francesca Martini,Pierluigi Cudazzo,Matteo Calandra

引用次数: 0