The Journal of Physical Chemistry Letters最新文献

英文中文

Intrinsic Chiroptical Evolution in Perovskite Nanocrystals. 钙钛矿纳米晶体的本征热带演化。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.jpclett.5c03687

Pengbo Ding,Dezhang Chen,Mohsen Tamtaji,GuanHua Chen,Liang Guo,Jonathan E Halpert

Here, we observed chiroptical evolution during the synthesis of perovskite nanocrystals (NCs). Using a steric-delayed nucleation strategy, we slowed the ripening of NCs and observed changes in the circular dichroism (CD) signal of perovskite NCs. Two chiroptical evolution events occurred during NC formation under different conditions, attributed to ligand displacement and NC self-assembly, respectively. Surface characterization and computational studies demonstrate that the ligands initially bind to the NC surface and dissociate during the ripening stage, offering the time window to observe and enhance the intrinsic chirality. Our findings provide a new strategy for studying and designing intrinsically chiral perovskite nanostructures.

在这里，我们观察了钙钛矿纳米晶体（NCs）合成过程中的热带演化。采用立体延迟成核策略，我们延缓了NCs的成熟，并观察了钙钛矿NCs的圆二色性（CD）信号的变化。在不同的条件下，NC形成过程中发生了两个不同的进化事件，分别归因于配体位移和NC自组装。表面表征和计算研究表明，配体最初与NC表面结合并在成熟阶段解离，为观察和增强本征手性提供了时间窗口。我们的发现为研究和设计内在手性钙钛矿纳米结构提供了一种新的策略。

引用次数: 0

Electrical Double Layer as a Voltage Divider: Suppressing Counterion Transport in Atomically Thin Nanopores. 作为分压器的双电层：抑制原子薄纳米孔中的反离子传输。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.jpclett.5c03986

Xiao-Yu Huang,Yu-Xi Liu,Long Gao,Jianguo Tian,Zhibo Liu

Surface charge in nanochannels is traditionally understood to enhance the ionic conductance. Particularly in the low-concentration regime, the electrical double layer (EDL) enriches counterions significantly above bulk levels, thereby sustaining high conductance. Experimental deviations from this behavior, such as anomalous conductance scaling, are typically attributed to surface physicochemical limitations or an insufficient ion supply. However, through finite element method simulations of ion transport in atomically thin nanopores, we reveal that the EDL itself acts as a potent voltage divider. This effect intensifies by up to an order of magnitude as the surface charge density increases or the bulk concentration decreases. Consequently, the local driving field within the pore is severely suppressed, rendering the enriched counterions ineffective for conduction despite their high local density. We derive a phenomenological model for this field attenuation and combine it with a refined, beyond-Donnan ion distribution profile to construct a conductance formulation that accurately reproduces the observed scaling behavior. Our findings unveil a dual nature of the EDL: while capable of recruiting conductive ions, the EDL can paradoxically function as a formidable barrier to transport via voltage division, challenging the classical view of surface-charge-governed conduction.

传统上认为纳米通道中的表面电荷可以增强离子电导率。特别是在低浓度状态下，双电层（EDL）显著富集了高于体水平的反离子，从而保持了高电导。实验偏离这种行为，如异常电导缩放，通常归因于表面物理化学限制或离子供应不足。然而，通过原子薄纳米孔中离子输运的有限元模拟，我们揭示了EDL本身作为一个有效的分压器。随着表面电荷密度的增加或体积浓度的降低，这种效应会增强一个数量级。因此，孔内的局部驱动场受到严重抑制，使得富集的反离子尽管局部密度很高，但仍无法传导。我们推导了该场衰减的现象学模型，并将其与精细的超越donnan离子分布剖面相结合，构建了一个准确再现所观察到的结垢行为的电导公式。我们的研究结果揭示了EDL的双重性质：虽然能够招募导电离子，但EDL可以矛盾地作为通过电压划分传输的强大屏障，挑战了表面电荷控制传导的经典观点。

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引用次数: 0

Probing Electrocatalytic Gas Evolution Reaction at Pt by Force Noise Measurements. Part 2. Oxygen 用力噪声测量法探测铂电催化释气反应。第2部分。氧气

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.jpclett.5c03776

Nataraju Bodappa, Gregory Jerkiewicz, Peter Grutter

Understanding O₂ bubble nucleation and growth during the oxygen evolution reaction (OER) is crucial to comprehend their influence on the location and distribution of catalytically active sites in the process. To achieve this goal, mapping the spatial variation of nanoscale dynamic individual steps at the electrocatalytic interfaces is vital, as it further enables a detailed understanding of the mechanism of the process. Here, we combine tapping mode AFM imaging with a Pt ultramicroelectrode to investigate oxygen bubble nucleation, growth, and detachment. Our AFM feedback error signal and topography data reveal that O₂ gas bubbles nucleate at step-edge sites and interact with catalytically active sites. This interaction between primary catalytic sites and bubble nucleation sites is the main reason for a decrease in the current density at a given high overpotential of the OER. Our findings advance the understanding of the complexity of phenomena involved in electrolytic gas evolution reactions on catalytic surfaces.

了解析氧反应（OER）过程中O2泡的成核和生长，对于理解它们对该过程中催化活性位点的位置和分布的影响至关重要。为了实现这一目标，绘制电催化界面上纳米尺度动态单个步骤的空间变化是至关重要的，因为它进一步使我们能够详细了解该过程的机制。在这里，我们将攻丝模式AFM成像与Pt超微电极相结合来研究氧泡的成核、生长和脱离。我们的AFM反馈误差信号和形貌数据显示，O2气泡在阶梯边缘位置成核，并与催化活性位点相互作用。初级催化位点和气泡成核位点之间的相互作用是在给定的高过电位OER下电流密度下降的主要原因。我们的发现促进了对催化表面上电解气体析出反应的复杂现象的理解。

引用次数: 0

Interface-Induced Symmetry-Breaking Processes Behind Intrinsic Chirality in Lead Halide Metal–Ligand Complexes and Perovskite Nanoclusters 卤化铅金属配体配合物和钙钛矿纳米团簇本征手性背后的界面诱导对称性破缺过程

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c03539

Celia Todd, Kai-Chun Chou, Mariam Khvichia, Xiao Wang, David Zeitz, Rayan Ali, Alyssa Yee, Jin Zhong Zhang

Here, we investigated the origin of chirality in PbBr₂–DMF metal–ligand complexes (MLCs) and their evolution into larger chiral nanoclusters. Utilizing a combination of UV–vis electronic absorption and circular dichroism (CD) spectroscopy, we identified chiral MLCs at 283 and 310 nm, which were assigned as [PbBr₂(DMF)₄] and [PbBr₃(DMF)₃]⁻¹. Upon the addition of methylammonium bromide (MABr) and injection into toluene with oleic acid/oleylamine ligands, new bands appeared at ∼370, 395, and 430 nm. These are assigned to multi-Pb MLCs, molecular clusters (MCs), and perovskite nanoclusters (PNCs), respectively. Raman spectra indicate PbBr₂ dissolution and Pb–DMF coordination based on the shift of PbBr₂ phonon modes alongside the appearance of new Pb–Br stretches and solvation-induced low-frequency modes associated with Pb–DMF bonding. Preliminary density functional theory (DFT) calculations also support both Pb–O and Pb–N binding, as the difference in relative energies between O- and N-bound MLC configurations is comparable to room-temperature thermal motion. Our findings demonstrate that chirality can originate directly from asymmetric solvation of Pb²⁺ at the solid–liquid interface and propagate through hierarchical growth into larger assemblies, providing a vital foundation for understanding the emergence of chirality in perovskite nanomaterials.

在这里，我们研究了PbBr2-DMF金属配体配合物（MLCs）的手性起源及其向更大的手性纳米团簇的演变。利用紫外-可见电子吸收和圆二色（CD）光谱相结合，我们在283和310 nm处鉴定了手性MLCs，它们被命名为[PbBr2(DMF)4]和[PbBr3(DMF)3]−1。在加入甲基溴铵（MABr）并将油酸/油胺配体注入甲苯后，在~ 370、395和430 nm处出现了新的谱带。它们分别被分配给多pb MLCs、分子簇（MCs）和钙钛矿纳米簇（pnc）。拉曼光谱表明，PbBr2的溶解和Pb-DMF的配位是基于PbBr2声子模式的转移，同时出现了新的Pb-Br延伸和与Pb-DMF键相关的溶剂化诱导的低频模式。初步的密度泛函数理论（DFT）计算也支持Pb-O和Pb-N结合，因为O和n结合的MLC构型之间的相对能量差异与室温热运动相当。我们的研究结果表明，手性可以直接源于Pb2+在固液界面的不对称溶剂化，并通过分层生长传播成更大的组装体，为理解钙钛矿纳米材料中手性的出现提供了重要的基础。

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引用次数: 0

Plasmon-Enhanced Photoluminescence of Interlayer Excitons Induced on WSe2/MoS2 Heterobilayers. 等离子体增强WSe2/MoS2异质层间激子的光致发光。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c03746

Keisuke Imaeda,Yusuke Takahashi,Shimba Ushikoshi,Takahiko Endo,Yasumitsu Miyata,Kosuke Nagashio,Sou Ryuzaki,Kosei Ueno

Excitonic light emission from transition-metal dichalcogenides (TMDs) heterobilayers has attracted considerable attention as a promising platform for atomically thin light sources. However, their emission efficiency is limited by the momentum mismatch between the valleys of the constituent TMD monolayers, and hence improving the emission quantum yield is highly desirable for their practical implementation in light-emitting devices. Here, we achieve a 10-fold enhancement of momentum-indirect emission by resonantly coupling plasmonic nanostructures with the WSe2/MoS2 heterobilayer. We observe a pronounced acceleration of the radiative recombination process of interlayer excitons in the plasmon-heterobilayer coupled system, demonstrating that the emission enhancement originates from the plasmonic Purcell effect. Our findings provide valuable insight into the influence of the plasmonic Purcell effect on momentum-indirect radiative transitions in TMD heterobilayers and offer compelling evidence that plasmonic nanostructures can effectively promote such transitions, paving the way for the development of highly efficient light-emitting devices based on TMD heterobilayers.

过渡金属二硫族化合物（TMDs）异质层的激子发光作为一种很有前途的原子薄光源平台引起了人们的广泛关注。然而，它们的发射效率受到组成TMD单层的谷之间的动量不匹配的限制，因此提高发射量子产率对于它们在发光器件中的实际实施是非常可取的。在这里，我们通过共振耦合等离子体纳米结构与WSe2/MoS2异质层实现了10倍的动量间接发射增强。我们观察到在等离子体-异质层耦合系统中，层间激子的辐射复合过程明显加速，表明发射增强是由等离子体珀塞尔效应引起的。我们的发现为等离子体Purcell效应对TMD异质层中动量间接辐射跃迁的影响提供了有价值的见解，并提供了令人信服的证据，证明等离子体纳米结构可以有效地促进这种跃迁，为开发基于TMD异质层的高效发光器件铺平了道路。

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引用次数: 0

Engineering Interfacial Donor-Acceptor Molecular Cocrystals. 工程界面供体-受体分子共晶。

IF 4.6 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c03865

Nikolai Severin, Neda Todorova, Tomáš Neveselý, Megan Davis, Martin Presselt, Filippo Giovanni Fabozzi, Stefan Hecht

Y6 is a high-performance non-fullerene acceptor widely used in organic solar cells. The assembly behavior of Y6 at interfaces, however, remains mostly unknown and respective in-depth investigations are missing. Here, we use room temperature scanning tunneling microscopy to investigate the self-assembly of Y6 at the solid-liquid interface. We show how coadsorption of polycyclic aromatic hydrocarbon donor molecules leads to the formation of a series of donor-acceptor interfacial cocrystals with tailored molecular structure and order on a graphite surface. The gained understanding of the intricate interplay of the underlying intermolecular interactions should facilitate the engineering of multicomponent interfacial nanostructures and help to potentially improve charge separation and transport in organic (opto)electronic devices.

Y6是一种高性能的非富勒烯受体，广泛应用于有机太阳能电池。然而，Y6在界面上的组装行为仍然是未知的，缺乏相应的深入研究。在这里，我们使用室温扫描隧道显微镜研究了Y6在固液界面的自组装。我们展示了多环芳烃供体分子的共吸附如何导致石墨表面形成一系列具有定制分子结构和顺序的供体-受体界面共晶。对潜在分子间相互作用的复杂相互作用的理解将有助于多组分界面纳米结构的工程设计，并有助于潜在地改善有机（光电）电子器件中的电荷分离和传输。

引用次数: 0

The Hidden Path to the Resonance-Stabilized Fulvenallenyl Radical (C7H5) via the Bimolecular Reaction of Tricarbon (C3, X1Σg+) with 1,3-Butadiene (C4H6; X1Ag) 三碳（C3, X1Σg+）与1,3-丁二烯（C4H6; X1Ag）双分子反应生成共振稳定的富尔venallenyl自由基（C7H5）的隐藏路径

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c03004

Iakov A. Medvedkov, Alexander M. Mebel, Anatoliy A. Nikolayev, Zhenghai Yang, Shane J. Goettl, Ralf I. Kaiser

We report a novel bimolecular reaction pathway forming the resonance-stabilized fulvenallenyl radical (C₇H₅) via the gas-phase reaction of tricarbon (C₃, X¹Σg⁺) with 1,3-butadiene (C₄H₆, X¹A_g). Crossed molecular beam experiments combined with high-level electronic structures and statistical calculations reveal a rich potential energy surface. The reaction proceeds via tricarbon addition to a double bond of 1,3-butadiene, overcoming a 30 kJ mol^–1 barrier, followed by ring closure, isomerizations (ring opening/closures, hydrogen shifts), and eventual hydrogen atom loss, yielding the fulvenallenyl radical (p1) almost exclusively via two dominant pathways. Considering the entrance barrier, this reaction may occur in high-temperature environments, like circumstellar envelopes of carbon stars, but is suppressed in colder regions such as molecular clouds and Titan’s atmosphere. These findings highlight the unexpected reactivity of small carbon clusters in shaping the molecular complexity of our universe, from the flicker of a flame to the death of a star.

我们报道了一种新的双分子反应途径，通过三碳（C3, X1Σg+）与1,3-丁二烯（C4H6, X1Ag）的气相反应形成共振稳定的fulvenallenyl自由基（C7H5）。交叉分子束实验结合高能级电子结构和统计计算揭示了一个丰富的势能面。反应通过三碳加成到1,3-丁二烯的双键上，克服30 kJ mol-1势垒进行，接着是环闭合，异构化（环开/闭，氢位移），最终氢原子损失，产生黄醛烯基自由基（p1），几乎完全通过两个主要途径。考虑到入口障碍，这种反应可能发生在高温环境中，比如碳星的星周包层，但在分子云和土卫六大气层等较冷的区域会受到抑制。这些发现强调了小碳团意想不到的反应性，在塑造我们宇宙的分子复杂性方面，从火焰的闪烁到恒星的死亡。

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引用次数: 0

Optical Anisotropy and Polarization Selectivity in WS2/CrSBr Heterostructure for Multifunctional All-Optical Logic Gates. 多功能全光逻辑门用WS2/CrSBr异质结构的光各向异性和偏振选择性

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c04006

Xinhui Yang,Mengya Li,Xiaojing Du,Chaochao Shen,Zhihui Chen,Jun He,Xiaoming Yuan

All-optical nanoscale logic components are regarded as fundamental building blocks of optical computing, enabling logic functions to be executed quickly and effectively avoiding thermal effects and signal crosstalk problems. Consequently, nanoscale all-optical computing is technologically forward-looking, but its realization necessitates the development of a multifunctional logic unit library. Here we construct a WS2/CrSBr heterostructure network to break the rotational symmetry of WS2, achieving a photoluminescence (PL) anisotropy ratio of 2.2. The twist angle of WS2/CrSBr has been further proven to be an effective method for modulating the PL anisotropy ratio and valley polarization degree. Taking advantage of the polarization-dependent emission characteristics of the WS2/CrSBr heterostructure networks, we demonstrate all-optical nanoscale switches. These networks can carry out diverse logical operations (including AND, OR, NAND, and NOR functions) and further implement all-optical binary arithmetic calculations, such as n-bit addition and subtraction. Our research highlights that assembling van der Waals heterostructure networks opens a new pathway for multifunctional optoelectronic devices and development of monolithic on-chip all-optical nanoprocessors.

全光纳米级逻辑元件被认为是光学计算的基本组成部分，使逻辑功能能够快速有效地执行，避免热效应和信号串扰问题。因此，纳米级全光计算在技术上具有前瞻性，但其实现需要开发多功能逻辑单元库。本文通过构建WS2/CrSBr异质结构网络打破WS2的旋转对称性，实现了WS2的光致发光（PL）各向异性比为2.2。进一步证明了WS2/CrSBr的扭转角是调制PL各向异性比和谷极化度的有效方法。利用WS2/CrSBr异质结构网络的偏振相关发射特性，我们展示了全光纳米级开关。这些网络可以进行多种逻辑运算（包括AND、OR、NAND和NOR功能），并进一步实现n位加减等全光二进制算术计算。我们的研究强调，组装范德华异质结构网络为多功能光电器件和单片全光纳米处理器的发展开辟了新的途径。

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引用次数: 0

Cooperative Effects of Active Sites in Single-Atom Catalysts. 单原子催化剂中活性位点的协同效应。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c03063

Min Hu,Yulan Han,Qin-Kun Li,Ke Ye,Guozhen Zhang

Single-atom catalysts (SACs) have come to the forefront of heterogeneous catalysis, largely built upon the success of an isolated active site model that maximizes metal atom utility and offers excellent catalytic activity. However, the drive toward industrial relevance has spurred synthetic advances that now routinely yield high loadings, pushing SACs into a new high-density regime, where the conventional "isolated site" assumption no longer holds. This Perspective posits that intersite synergy is a tunable emergent property in these systems, shaped by the spatial distance between adjacent active centers. The impacts of site cooperation on heterogeneous catalysis manifest in various forms, including modified linear scaling relationships, alternating reaction pathways, and tunable spin-dependent activities. We conclude by outlining the challenges and opportunities in operando characterization and theoretical modeling of these cooperative catalytic ensembles, charting a course for the next frontier in the study of single-atom catalysis.

单原子催化剂（SACs）已成为多相催化的前沿，主要建立在一个孤立的活性位点模型的成功，最大限度地发挥金属原子的效用，并提供优异的催化活性。然而，对工业相关性的驱动刺激了合成技术的进步，现在通常产生高负载，将sac推向新的高密度状态，传统的“孤立站点”假设不再成立。该观点认为，在这些系统中，场地间的协同作用是一种可调节的涌现特性，由相邻活动中心之间的空间距离形成。位点合作对多相催化的影响表现为多种形式，包括改变线性标度关系、改变反应途径和调节自旋依赖活性。最后，我们概述了这些协同催化体系的operando表征和理论建模方面的挑战和机遇，并为单原子催化研究的下一个前沿指明了方向。

引用次数: 0

Second Harmonic Generation Electric Field Triplet Interferometry for Absolute Phasing. 绝对相位的二次谐波产生电场三重态干涉测量。

IF 4.6 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.jpclett.5c03777

Raiden Speelman, Nicole M Gonzalez, Camille M Bridgewater, Franz M Geiger

We report second harmonic generation (SHG) electric field triplet interferometry performed using three mutually coherent ultrafast pulses in a common path with controllable relative phases, namely, the light fields of a sample signal (SI), a reference oscillator (RO), and a local oscillator (LO). The ROLO phase determined from the interference of the light fields produced by two quartz wafers is subtracted from the phase determined from the SIROLO interferogram to yield the signal phase, ϕ_SI. The new method also calibrates the measured SHG intensity from a given sample internally by sending the fundamental light field reflected from the sample into one of the quartz wafers in the ROLO element. The approach avoids having to exchange the sample against a reference material with a known χ⁽²⁾ value or known phase and accounts on-the-fly for situations where the reflected fundamental light field intensity changes with experimental conditions. The new method is successfully benchmarked against z-cut α-quartz, fused silica held at its point of zero charge, and hematite nanolayers in air, across three different interferometers. The approach should be applicable for other second-order nonlinear spectroscopies, such as vibrational or electronic sum-frequency generation.

我们报道了使用三个相互相干的超快脉冲在具有可控相对相位的共路径上进行的二次谐波产生（SHG）电场三重态干涉测量，即样品信号（SI），参考振荡器（RO）和本振（LO）的光场。从两个石英晶圆产生的光场的干涉中确定的ROLO相位从从SIROLO干涉图中确定的相位中减去，从而产生信号相位，si。新方法还通过将样品反射的基光场发送到ROLO元件中的一个石英晶圆中，在内部校准来自给定样品的测量SHG强度。该方法避免了将样品与已知χ(2)值或已知相位的参考物质交换，并在反射的基本光场强度随实验条件变化的情况下进行动态计算。新方法通过三种不同的干涉仪成功地对z形切割α-石英、保持在零电荷点的熔融二氧化硅和空气中的赤铁矿纳米层进行了基准测试。该方法应适用于其他二阶非线性光谱，如振动或电子和频产生。

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引用次数: 0

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