The Journal of Physical Chemistry Letters最新文献

英文中文

Persistent Orbital Magnetism from Light-Induced Attosecond Charge Migration in Linear Molecules. 线性分子中光诱导的阿秒电荷迁移的持续轨道磁性。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-20 DOI: 10.1021/acs.jpclett.6c00139

Jean Christophe Tremblay,Gopal Dixit

Laser-driven coherent charge migration is a fundamental process occurring on the attosecond time scale, and it plays a central role in a wide range of chemical and biological phenomena. In this work, we show that linear polyatomic molecules can exhibit light-induced magnetic behavior through the selective excitation of low-lying, optically accessible charge-transfer states that can bear ring currents. Using ultrashort circularly polarized laser pulses, we demonstrate that oriented lithium cyanide undergoes a screw-like helical charge migration, which generates intense, rapidly oscillating magnetic fields on subfemtosecond time scales. Time-resolved electronic current-density maps are employed to visualize the evolving charge flow and to link the helical currents to the underlying π → σ charge-transfer character of the excitation. These results reveal a chemically intuitive mechanism for inducing ultrafast circulating currents in linear polyatomic molecules and establish a route toward engineering molecular magnetism. The present findings open new opportunities for controlling electronic currents and magnetic responses in molecules, with promising implications for light-driven molecular functionality.

激光驱动的相干电荷迁移是发生在阿秒时间尺度上的一个基本过程，它在广泛的化学和生物现象中起着核心作用。在这项工作中，我们证明了线性多原子分子可以通过选择性激发低洼、光学可及的、可以承受环电流的电荷转移态来表现出光诱导磁行为。利用超短圆偏振激光脉冲，我们证明了取向氰化锂经历了螺旋状的螺旋电荷迁移，在亚飞秒时间尺度上产生了强烈的、快速振荡的磁场。时间分辨的电子电流密度图用于显示电荷流的演变，并将螺旋电流与激发的π→σ电荷转移特征联系起来。这些结果揭示了在线性多原子分子中产生超快循环电流的化学直观机制，并为工程分子磁学开辟了一条途径。目前的发现为控制分子中的电流和磁响应开辟了新的机会，对光驱动分子功能有很好的意义。

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引用次数: 0

Nuclear Quantum Effects Sustain Cooperative Hydride Ion Migration and Restore Arrhenius Behavior in Pnma LaH3-x. 核量子效应维持氢化物离子协同迁移并恢复Pnma LaH3-x中的Arrhenius行为。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-20 DOI: 10.1021/acs.jpclett.6c00094

Ziqi Wang,Hujun Cao,Yong Pei

Hydride ion (H-) conduction materials have attracted significant attention for their potential in advanced clean energy storage and conversion. Moreover, understanding H- migration mechanisms is essential for controlling ionic transport in these materials and advancing next-generation energy technologies, given the quantum mechanical nature of hydrogen. Here, we investigate the role of nuclear quantum effects (NQEs) by comparing results obtained from thermostated ring polymer molecular dynamics (TRPMD) simulations with those from classical molecular dynamics (MD) simulations using a trained deep potential (DP) model. Our results show that the main manifestation of NQEs is not the conventional quantum tunneling often intuitively expected. Instead, they facilitate the cooperative H- migration mechanism at low temperatures. This is reflected in the increased mean square displacements (MSDs) and diffusion coefficients observed under these conditions. Notably, the temperature dependence of diffusion coefficients from TRPMD follows Arrhenius behavior, whereas that of classical MD deviates significantly at low temperatures. This work highlights the crucial role of NQEs in governing low-temperature transport and provides fundamental insights for the design of advanced H- conductors.

氢化物离子（H-）传导材料因其在先进清洁能源储存和转换方面的潜力而受到广泛关注。此外，考虑到氢的量子力学性质，理解氢迁移机制对于控制这些材料中的离子传输和推进下一代能源技术至关重要。在这里，我们研究了核量子效应（NQEs）的作用，通过比较热稳态环聚合物分子动力学（TRPMD）模拟结果和经典分子动力学（MD）模拟结果，使用训练深势（DP）模型。我们的研究结果表明，NQEs的主要表现不是人们通常直观地期望的传统量子隧道效应。相反，它们促进了低温下氢离子的协同迁移机制。这反映在这些条件下观察到的均方位移（MSDs）和扩散系数的增加上。值得注意的是，TRPMD的扩散系数的温度依赖关系遵循Arrhenius行为，而经典MD的扩散系数在低温下明显偏离。这项工作强调了NQEs在控制低温输运中的关键作用，并为设计先进的氢导体提供了基本的见解。

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引用次数: 0

Catalytic NO Reduction by Single Au-Doped Aluminum Oxide Cluster Anions: Structural Role of Au. 单Au掺杂氧化铝簇阴离子催化NO还原：Au的结构作用。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-20 DOI: 10.1021/acs.jpclett.6c00383

Hui-Ru Jia,Yu-Zhe Hu,Jiao-Jiao Chen,Jun Ma,Xun-Lei Ding,Sheng-Gui He

Supported gold (Au) catalysts have attracted sustained interest, owing to their remarkable reactivity in a wide range of catalytic reactions, where Au is generally regarded as the active site or an electron buffer. Herein, through a combination of state-of-the-art mass-spectrometric experiments and quantum-chemical calculations, we demonstrate that single Au-doped aluminum oxide cluster anions AuAl3O4,5- can catalyze NO reduction by CO. The catalytic cycle proceeds via a single-electron mechanism driven exclusively by the electron-rich Al site, while the Au atom remains redox-inactive and acts as a spectator throughout the reaction pathway. Detailed analyses reveal that Al actively participates in the electron-transfer processes, whereas Au forms persistent Au-Al bonds that stabilize the cluster framework and maintain a favorable energetic landscape for catalysis. These results uncover an unconventional catalytic scenario in which Au functions primarily as a structural stabilizer rather than an active center, offering molecular-level insight into metal-support interactions and deepening the mechanistic understanding of CO-mediated NO reduction in Au-based catalytic systems.

负载金（Au）催化剂吸引了持续的兴趣，因为它们在广泛的催化反应中具有显著的反应性，其中Au通常被认为是活性位点或电子缓冲。本文中，通过最先进的质谱实验和量子化学计算相结合，我们证明了单个Au掺杂的氧化铝簇阴离子aual3o4,5 -可以催化CO还原NO。催化循环通过单电子机制进行，该机制完全由富电子Al位驱动，而Au原子在整个反应过程中保持不氧化还原活性，并充当旁观者。详细分析表明，Al积极参与电子转移过程，而Au形成持久的Au-Al键，稳定团簇框架并保持有利的催化能量景观。这些结果揭示了一种非常规的催化情景，其中Au主要作为结构稳定剂而不是活性中心，提供了分子水平上对金属支持相互作用的见解，并加深了对Au基催化体系中co介导的NO还原机制的理解。

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引用次数: 0

Ultrafast Optical Probing of Hypersonic Phonons in Nanoscale GeTe Films. 纳米GeTe薄膜中高超声子的超快光学探测。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-20 DOI: 10.1021/acs.jpclett.6c00461

Margherita Vittucci,Alessandro Casto,Jessy Paterson,Martina Tomelleri,Nicholas Blanchard,Aurélien Crut,Stéphane Pailhès,Francesco Banfi,Natalia Del Fatti,Pierre Noé,Valentina M Giordano,Paolo Maioli

Using time-resolved optical spectroscopy, we investigate the acoustic dynamics of polycrystalline germanium telluride (GeTe) nanoscale thin films, a multifunctional material combining phase-change behavior for nonvolatile memory and reconfigurable photonics with promising thermoelectric performance. We probe the generation and propagation of longitudinal acoustic waves with submicrometer wavelengths and frequencies in the range of tens of gigahertz. Our experimental approach integrates phonon echo measurements in thicker layers (∼360 nm) with the analysis of fundamental thickness-breathing modes in thinner layers (∼80 nm), enabling separation of intrinsic and interface contributions to attenuation. This allows the direct extraction of both intrinsic acoustic attenuation and longitudinal sound velocity in polycrystalline GeTe thin films. We determine mean free paths of approximately 0.7-7 μm for 10-20 GHz acoustic waves. These findings clarify hypersonic phonon dynamics in GeTe, establish a benchmark for high-frequency acoustic dissipation in chalcogenide thin films, and support the development of devices ranging from phase-change memory to thermoelectrics.

利用时间分辨光谱学，我们研究了多晶碲化锗（GeTe）纳米薄膜的声动力学。多晶碲化锗是一种结合相变行为的多功能材料，具有非易失性存储器和可重构光子学，具有很好的热电性能。我们探测了亚微米波长和频率在几十千兆赫兹范围内的纵向声波的产生和传播。我们的实验方法将较厚层（~ 360 nm）中的声子回波测量与较薄层（~ 80 nm）中的基本厚度呼吸模式分析相结合，实现了对衰减的本征和界面贡献的分离。这允许直接提取多晶GeTe薄膜的固有声衰减和纵向声速。我们确定了10-20 GHz声波的平均自由程约为0.7-7 μm。这些发现阐明了GeTe中的高超声子动力学，为硫系薄膜中的高频声耗散建立了基准，并支持了从相变存储器到热电器件的开发。

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引用次数: 0

Amyloid-β “Co-assembles” with Coatomer Subunit Delta (δ-COP) 淀粉样蛋白-β与涂层亚基δ (δ-COP)“共组装”

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-19 DOI: 10.1021/acs.jpclett.5c03565

Anastasia Vlachou, Om Shanker Tiwari, Ehud Gazit, Phanourios Tamamis

Previous studies showed that δ-COP interacts with APP and regulates its intracellular trafficking, while an important reduction in the level of Aβ plaques was observed in AD/δ-COP I422T mice. Here, we show that δ-COP interacts directly with Aβ assemblies according to experiments and simulations. Experiments suggest a two-binding site model, one with high affinity and one with lower affinity. Simulations comply with experiments and provide mechanistic biophysical insights into the high-affinity interactions, comprising a “co-assembly-like” β-sheet interaction within nearly identical domains ₄₂₆DGEYRHDS₄₃₃ of δ-COP and ₁DAEFRHDS₈ of Aβ, complemented by interactions between ₄₁₆GVGAPVIGEI₄₂₅ of δ-COP and ₁₃HHQKLVFFAED₂₃ of Aβ, with a β-bridge between δ-COP I422 and Aβ D23. As such, our simulations highlight the role of I422, which is also investigated in comparison to T422. Our studies can provide impetus for the future investigation of the interaction between δ-COP and Aβ, particularly in its involvement in intracellular trafficking in Alzheimer’s disease.

先前的研究表明，δ-COP与APP相互作用并调节其细胞内运输，同时在AD/δ-COP I422T小鼠中观察到Aβ斑块水平的重要降低。通过实验和模拟，我们发现δ-COP直接与Aβ组装体相互作用。实验提出了一个高亲和力和低亲和力的双结合位点模型。模拟结果符合实验结果，并提供了高亲和相互作用的机制生物物理见解，包括δ-COP的426DGEYRHDS433和a β的1DAEFRHDS8几乎相同的结构域内的“共组装样”β-sheet相互作用，δ-COP的416GVGAPVIGEI425和a β的13HHQKLVFFAED23之间的相互作用，δ-COP I422和a β D23之间的β-桥接。因此，我们的模拟突出了I422的作用，并将其与T422进行了比较研究。我们的研究可以为未来研究δ-COP和Aβ之间的相互作用提供动力，特别是其参与阿尔茨海默病的细胞内运输。

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引用次数: 0

Intrinsic Altermagnetic–Ferroelectric Multiferroicity and Magnetoelectric Coupling in Reversed Transition-Metal Bromides 反过渡金属溴化物的本征交变铁电多铁性和磁电耦合

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-19 DOI: 10.1021/acs.jpclett.6c00283

Chunlin Pan, Jie Wang, Hong Zhang, Tingting Zhong, Qing Yang, Sheng Meng

Multiferroic materials, which exhibit the coexistence of magnetic and ferroelectric orders, offer opportunities for the exploration of new physical phenomena. A recent study proposed that van der Waals altermagnetism can combine with sliding ferroelectricity within the same crystal, constituting a novel type of multiferroic material [Wu et al., Sci. China-Phys. Mech.Astron. 2025, 68, 297511]. This represents significant advancement in the research of novel multiferroics, Nevertheless, the diverse magnetoelectric couplings and their underlying mechanisms warrant further investigation. Here, through targeted interlayer engineering informed by first-principles calculations and spin space group analysis, we identify NiBr₂ and MnBr₂ as compounds simultaneously hosting robust altermagnetism and sliding ferroelectricity. Crucially, altermagnetism of MnBr₂ becomes spontaneously locked to the ferroelectric state at maximal polarization via symmetry constraints, enabling deterministic magnetoelectric coupling and nonvolatile electric control of magnetization. This breakthrough not only presents the first material realization of such a coupled phenomenon but also establishes a generic symmetry-engineering paradigm for developing advanced multiferroics in transition metal bromides.

多铁性材料表现出磁性和铁电序的共存，为探索新的物理现象提供了机会。最近的一项研究提出，范德华变磁可以与滑动铁电在同一晶体内结合，构成一种新型的多铁性材料[Wu et al., Sci.]。China-Phys。Mech.Astron。[j].农业机械学报，1998,29(5):951 - 951。这代表了新型多铁性材料研究的重大进展，然而，不同的磁电耦合及其潜在机制有待进一步研究。在这里，通过第一性原理计算和自旋空间群分析，我们确定NiBr2和MnBr2是同时具有强磁场和滑动铁电性的化合物。至关重要的是，通过对称约束，MnBr2的交变磁性在最大极化时自发锁定为铁电态，从而实现了确定性磁电耦合和磁化的非易失性电控制。这一突破不仅首次在材料上实现了这种耦合现象，而且为开发过渡金属溴化物中的先进多铁性材料建立了一个通用的对称工程范式。

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引用次数: 0

Periodic Hirshfeld Atom Refinement. 周期性赫斯菲尔德原子精化。

IF 4.6 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-19 Epub Date: 2026-02-27 DOI: 10.1021/acs.jpclett.5c03918

Kanghyun Chu, Dylan Jayatilaka, Lorraine A Malaspina, Alessandro Genoni, Georgia Cametti, Stefan Mebs, Dieter Lentz, Hans-Beat Bürgi, Sergey V Churakov, Simon Grabowsky

Hirshfeld Atom Refinement (HAR) is a quantum crystallographic method for analyzing single-crystal X-ray diffraction data, providing accurate and precise structural parameters. Despite its success in predicting hydrogen-atom parameters, the application of HAR is fundamentally limited to molecular crystals. Inspired by two recently developed HAR versions that employ periodic-boundary conditions, here we introduce a new variant of periodic HAR (pHAR) that is applicable to any periodic-network structure while remaining compatible with conventional HAR by using atom-centered Gaussian orbitals with a Bloch wave formalism. pHAR was tested against high-quality single-crystal diffraction data for boranes and borates comprising N-H and B-H bonds in different chemical environments. The results demonstrate a close agreement of X-H bond lengths with reference data from neutron-diffraction experiments with improved precision. Using pHAR, this study has nearly doubled the previously available body of reliable experimental structural data on B-H bonds.

Hirshfeld原子精化（HAR）是一种用于分析单晶x射线衍射数据的量子晶体学方法，可提供精确的结构参数。尽管HAR在预测氢原子参数方面取得了成功，但它的应用基本上仅限于分子晶体。受最近开发的两种采用周期性边界条件的HAR版本的启发，我们在这里引入了一种新的周期性HAR （pHAR）变体，该变体适用于任何周期性网络结构，同时通过使用具有Bloch波形式的原子中心高斯轨道与传统HAR保持兼容。利用高质量的单晶衍射数据对不同化学环境下含有N-H和B-H键的硼烷和硼酸盐进行了pHAR测试。结果表明，x -氢键长度与中子衍射实验的参考数据非常吻合，精度提高了。利用pHAR，本研究几乎将先前可用的关于B-H键的可靠实验结构数据增加了一倍。

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引用次数: 0

Pressure-Induced Discovery of a Topological Phase of Bi4Br4 with AA''-Stacking. 压力诱导发现具有AA " -堆叠的Bi4Br4拓扑相。

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-19 DOI: 10.1021/acs.jpclett.6c00232

Honglin Li,Fuyi Wang,Zhenyu Wang,Lu Li,Wencheng Lu,Qing Tian,Hongjian Zhao,Wei Zhang,Jian Lv,Haijun Zhang,Pengyue Gao,Yanchao Wang

Bismuth halides Bi4X4 (X = Br, I) consist of quasi-one-dimensional van der Waals chains whose interchain stacking can be reshaped by pressure, potentially reprogramming topology. Using CALYPSO structure searches with first-principles enthalpy ranking, we uncover a previously unreported C2/m phase of Bi4Br4 featuring a novel AA″ stacking that becomes stable above ∼4 GPa and persists to at least 15 GPa. We map the transformation from known β-Bi4Br4 (AA stacking): under compression β develops an imaginary phonon mode, appears as a first-order saddle point in the crystal-solution landscape, and relaxes into the C2/m-AA″ structure with an estimated barrier of ∼40 meV/atom, explaining pressure-driven stacking rearrangement. With spin-orbit coupling, a band gap opens at symmetry crossings and a nontrivial inversion yields Z2 = (001; 0), identifying the AA″ phase as a weak topological insulator with gapless (100)/(010) surface states.

卤化铋Bi4X4 （X = Br， I）由准一维范德华链组成，其链间的堆叠可以通过压力重塑，可能会重新编程拓扑结构。使用CALYPSO结构搜索和第一原理焓排序，我们发现了以前未报道的Bi4Br4的C2/m相，具有新颖的AA″堆叠，在~ 4 GPa以上变得稳定，并持续到至少15 GPa。我们绘制了从已知的β- bi4br4 （AA堆叠）的转变：在压缩下β发展出一个假想的声子模式，在晶体溶液中作为一阶鞍点出现，并以估计约40 meV/原子的势垒弛豫成C2/m-AA″结构，解释了压力驱动的堆叠重排。通过自旋-轨道耦合，带隙在对称交叉处打开，非单调反转产生Z2 =(001; 0)，确定AA″相为具有无间隙(100)/(010)表面态的弱拓扑绝缘体。

引用次数: 0

Comprehensive Structural Descriptors Enable Machine Learning Prediction of Perovskite Band Characteristics 综合结构描述符实现钙钛矿带特性的机器学习预测

IF 6.475 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-18 DOI: 10.1021/acs.jpclett.6c00030

Zixuan Ni, Zhirui Zhang, Yiming Chen, Daye Zheng, Jian Xu

Organic–inorganic hybrid and all-inorganic perovskites are promising candidates for next-generation optoelectronics. Accurate prediction of band characteristics is essential for guiding the rational design of high-performance perovskite devices. Although machine learning (ML) has been applied in this field, the soft lattices of halide perovskites exhibit significant structural distortions that are often difficult for conventional ML descriptors to capture. Here, we introduce a set of physically meaningful structural descriptors that directly quantify key distortion modes: octahedral distortion, cation displacement, and segregation index. The resulting model achieves high accuracy for prediction of bandgap, VBM, and CBM positions of two representative Br-alloyed lead halide perovskite systems (Cs_0.25FA_0.75PbI_xBr_3–x and CsPbI_xBr_3–x), underscoring the importance of structural information in ML-driven electronic-property prediction. Notably, we identified an unexpected inverse correlation between the standard deviation of Pb–X–Pb bond angles and the bandgap, which is associated with an enhanced contribution of Br to the VBM under higher structural order.

有机-无机杂化钙钛矿和全无机钙钛矿是下一代光电子学的有前途的候选者。准确预测能带特性对于指导高性能钙钛矿器件的合理设计至关重要。尽管机器学习（ML）已应用于该领域，但卤化物钙钛矿的软晶格表现出明显的结构扭曲，这通常是传统ML描述符难以捕获的。在这里，我们引入了一组物理上有意义的结构描述符，可以直接量化关键的畸变模式：八面体畸变、阳离子位移和偏析指数。所得到的模型在预测两种具有代表性的br合金卤化铅钙钛矿体系（Cs0.25FA0.75PbIxBr3-x和CsPbIxBr3-x）的带隙、VBM和CBM位置方面达到了很高的精度，强调了结构信息在机器学习驱动的电子性质预测中的重要性。值得注意的是，我们发现了Pb-X-Pb键角的标准差与带隙之间出乎意料的负相关，这与Br在更高结构阶下对VBM的贡献增强有关。

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引用次数: 0

Exploring Molecular Orbital Pseudospins as All-Optical Quantum Sensors. 探索分子轨道伪自旋作为全光量子传感器。

IF 4.6 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters

Pub Date : 2026-03-18 DOI: 10.1021/acs.jpclett.6c00406

Yong Rui Poh, Joel Yuen-Zhou

Recent developments in molecular qubits have focused on transitions among electron spin states interfaced with optical electronic transitions for better sensing resolutions. However, molecular electronic states can also form pseudospins, and using them as qubits would bypass the additional step of spin-optical interfacing. In this work, we discuss whether precessions of molecular orbital pseudospins under environmental influence can allow for all-optical quantum sensing via optical pump-probe spectroscopy. We find that these oscillations can survive rotational averaging and can be detected in isotropic environments. Unfortunately, fast electronic decoherence is likely to constrain measurements to environmental quantities that strongly influence orbital pseudospins, which are uncommon. This pitfall may be mitigated by further molecular engineering, which can be faster than spin-based qubits, given the high ab initio predictability of molecular electronic states.

分子量子比特的最新发展主要集中在电子自旋态与光学电子跃迁之间的转变上，以获得更好的传感分辨率。然而，分子电子态也可以形成假自旋，使用它们作为量子比特将绕过自旋光学界面的额外步骤。在这项工作中，我们讨论了分子轨道假自旋在环境影响下的进动是否可以通过光泵浦探测光谱实现全光量子传感。我们发现这些振荡可以经受住旋转平均，并且可以在各向同性环境中被检测到。不幸的是，快速电子退相干可能会限制测量到强烈影响轨道伪自旋的环境量，这是不常见的。考虑到分子电子状态的高从头算可预测性，进一步的分子工程可以比基于自旋的量子位更快地缓解这个陷阱。

引用次数: 0

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