标题： 分子形状到振动弗什巴赫共振的共振隧道观测及其随后的模式特异性裂解 显示英文标题

标题： Observation of Resonant Tunneling from Molecular Shape into Vibronic Feshbach Resonances Followed by Mode-Specific Fragmentation

摘要： 我们展示了一项关于线性OCS分子中解离电子附着（DEA）的运动学完整研究，重点探讨了电子如何共振地附着并触发解离。在弗兰克-康登区域附近，DEA主要由分子形状共振主导，在这些共振中，瞬态的OCS$^-$态以高振动振幅形成，光谱上表现为DEA截面中的宽特征。随着电子束能量从5.5 eV增加到6.0 eV，S$^-$的群体从低能高度密集的弯曲振动状态转移到高能状态，这强化了我们在偶极禁戒振动强度借用方面的发现。 我们使用方程运动耦合簇单双方法（EA-EOMCCSD）进行的先进的势能曲线计算揭示，在形状共振之外，非绝热共振隧穿控制着避免交叉现象，在动态过程中生成三种模式特定的振动Feshbach共振，随后完全解离成三种不同的动能带S$^-$。我们的理论结果定量和定性地解释了大部分实验观察结果。 这些见解加深了我们对共振介导的电子-分子共振散射中解离的基本理解，具有更广泛的量子力学、等离子物理、振动恢复、 astrochemistry（天体化学）和辐射损伤研究的含义。 显示英文摘要

摘要： We present a kinematically complete study of dissociative electron attachment (DEA) in linear OCS molecules, focusing on how electrons resonantly attach and trigger dissociation. Near the Franck-Condon regime, DEA is dominated by molecular shape resonances, where transient OCS$^-$ states form with high vibrational amplitudes, spectroscopically evident as broad features in DEA cross-sections. As the electron beam energy increases from 5.5 to 6.0 eV, S$^-$ population shifts from lower to higher-energy highly dense bending vibrational states, reinforcing our findings on dipole-forbidden vibronic intensity borrowing. Our advanced potential energy curve calculations, employing the Equation-of-motion coupled cluster singles and doubles for electron attachment (EA-EOMCCSD) method, reveal that beyond the shape resonance, non-adiabatic resonant tunneling governs the avoided crossings, dynamically generating three mode-specific vibronic Feshbach resonances before complete dissociation into three distinct kinetic energy bands of S$^-$. Our theoretical results probe most of the experimental observations quantitatively and qualitatively. These insights deepen our fundamental understanding of resonance-mediated dissociation in electron-molecule resonant scattering, with broader implications for quantum mechanics, plasma physics, vibrational revival, astrochemistry, and radiation damage research.