非均匀电场中液态水的非平衡热力学和集体振动模式
Non-equilibrium thermodynamics and collective vibrational modes of liquid water in an inhomogeneous electric field
摘要：
在该实验中，使用高压（20 kV）点-平面电极系统使液态水经受不均匀电场（${\nabla}^2 E_a {\approx} 10^{10} \frac{V}{m^2}$）。利用干涉测量法，发现对水施加强电场梯度会产生液体折射率的局部变化，使表面极化并产生向下移动的电对流射流。在点电极附近测得的最大温差为1 °C。水的拉曼光谱揭示了振动集体模式（3250 $cm^{-1}$）的增强以及局部模式（3490 $cm^{-1}$）能量的增加。这种双峰增强表明光谱变化不是由于温度。因此，强场梯度建立了远离热平衡的振动振子的激发子群。集体振动模式的离域在空间上扩展了这种激发的人口超过微观尺度。由于分子偶极子的电场钉扎而阻碍的旋转自由阻碍了热流并产生化学电势梯度。这些变化是导致观察到的折射率和温度变化的原因。它表明，极性液体，因此可以支持当地的非平衡热力学瞬态关键的生化和环境过程。
英文摘要：
In this experiment liquid water is subject to an inhomogeneous electric field (${\nabla}^2 E_a {\approx} 10^{10} \frac{V}{m^2}$ ) using a high voltage (20 kV) point-plane electrode system. With interferometry it was found that the application of a strong electric field gradient to water generates local changes in the refractive index of the liquid, polarizes the surface and creates a downward moving electro-convective jet. A maximum temperature difference of 1 °C is measured in the immediate vicinity of the point electrode. Raman spectroscopy on water reveals an enhancement of the vibrational collective modes (3250 $cm^{-1}$) as well as an increase in the local mode (3490 $cm^{-1}$) energy. This bimodal enhancement indicates the spectral changes are not due to temperature. The intense field gradient thus establishes an excited subpopulation of vibrational oscillators far from thermal equilibrium. Delocalization of the collective vibrational mode spatially expands this excited population beyond the microscale. Hindered rotational freedom due to electric field pinning of molecular dipoles retards heat flow and generates a chemical potential gradient. These changes are responsible for the observed changes in refractive index and temperature. It is demonstrated that polar liquids can thus support local non-equilibrium thermodynamic transient states critical to biochemical and environmental processes.
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