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Time-resolved non-linear dielectric responses in molecular systems

机译:分子系统中时间分辨的非线性介电响应

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摘要

Impedance measurements in the 0.1 Hz to 50 kHz range are performed beyond the linear response regime, using a technique where peak fields as high as 450 kV/cm are possible. The main focus is on the effects of the energy that is transferred irreversibly from the external field to a molecular glass-forming liquid. Because the slow degrees of freedom absorb this energy, their heterogeneous configurational temperatures are increased before the heat is transferred to the phonons on the time scale of structural relaxation. We also discuss a time-resolved variant of high-field impedance spectroscopy, where the harmonic field is applied for a number of cycles at a low field, followed by the same signal at a much higher field. Fourier analysis of the resulting voltage and current traces provides a period-by-period time-resolved picture for the response of the configurational temperature with a 5 mK resolution, resulting from a sensitivity on the 5 x 10(-5) level for tan delta. It turns out that this energy absorption is responsible for an extremely pronounced non-linearity in the electric field, where the dielectric relaxation can be accelerated by a factor of 2 prior to changing the temperature.
机译:在超过线性响应范围的范围内,使用可能高达450 kV / cm的峰值场的技术,在0.1 Hz至50 kHz范围内进行阻抗测量。主要焦点是能量的影响,这些能量不可逆地从外部场传递到形成分子玻璃的液体。由于缓慢的自由度会吸收此能量,因此在结构松弛的时间尺度上,热量传给声子之前,它们的异质构型温度会升高。我们还讨论了高场阻抗谱的时间分辨变体,其中谐波场在低场施加多个循环,然后在更高的场施加相同的信号。所得电压和电流迹线的傅立叶分析提供了一个周期性的时间分辨图像,用于以5 mK分辨率对配置温度的响应,这是由于tanδ的灵敏度为5 x 10(-5) 。事实证明,这种能量吸收是导致电场中非常明显的非线性的原因,其中在改变温度之前,介电弛豫可以被加速2倍。

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