AI 中文总结
该研究将时间分辨太赫兹斯塔克光谱学（TRTSS）扩展到室温水中溶解的分子，以孔雀绿和甲基橙为模型，证实其可在高极性氢键环境中观测斯塔克响应，且信号与TD-DFT计算相符，还发现构象效应会影响斯塔克参数。
AI 中文摘要
斯塔克光谱学是一种强大的方法，用于探测外加电场下的分子偶极矩变化、电荷转移动力学和极化率。时间分辨太赫兹斯塔克光谱学（TRTSS）利用强单周期太赫兹（THz）脉冲诱导瞬态斯塔克位移，克服了传统方法的关键局限。与静态或低频场不同，THz脉冲的振荡速度远快于典型分子转动时间，能有效阻止偶极重取向，可在常温下对溶液进行测量。在此，我们将TRTSS扩展到溶解在水中的分子——水是化学和生物系统中最重要的极性溶剂，并首次展示了室温下水中的斯塔克光谱学。以孔雀绿和甲基橙为模型体系，我们观测到清晰的THz诱导光谱调制，表明TRTSS甚至能在高极性、氢键环境中成功揭示THz斯塔克响应。两个体系的测量信号同时呈现线性（偶极驱动）和二次（极化率驱动）斯塔克效应，与时间依赖密度泛函理论（TD-DFT）计算结果一致。与TD-DFT的进一步比较表明，构象效应会影响溶剂化分子中提取的斯塔克参数。
英文摘要
Stark spectroscopy is a powerful method for probing molecular dipole moment changes, charge transfer dynamics, and polarizability under applied electric fields. Time-Resolved Terahertz Stark Spectroscopy (TRTSS), which employs intense single-cycle terahertz (THz) pulses to induce transient Stark shifts, overcomes key limitations of conventional approaches. Unlike static or low-frequency fields, THz pulses oscillate much faster than typical molecular rotation times, effectively preventing dipole reorientation and enabling measurements in solutions at ambient conditions. Here, we extend TRTSS to molecules dissolved in water, the most important polar solvent for chemical and biological systems and report the first demonstration of Stark spectroscopy in water at room temperature. Using Malachite Green and Methyl Orange as model systems, we observe clear THz-induced spectral modulations, demonstrating that TRTSS can successfully reveal THz Stark responses even in highly polar, hydrogen-bonded environments. Measured signals exhibit a combination of linear (dipole-driven) and quadratic (polarizability-driven) Stark effects in both systems, consistent with time-dependent density functional theory (TD-DFT) calculations. Comparison with TD-DFT further suggests that conformational effects can influence the extracted Stark parameters in solvated molecules.
