Rudolf Peierls Centre for Theoretical Physics, Oxford University , Oxford, OX13NP, United Kingdom.
Nano Lett. 2016 Apr 13;16(4):2205-12. doi: 10.1021/acs.nanolett.5b04372. Epub 2016 Mar 15.
We calculate the power spectrum of electric-field-driven ion transport through nanometer-scale membrane pores using both linearized mean-field theory and Langevin dynamics simulations. Remarkably, the linearized mean-field theory predicts a plateau in the power spectral density at low frequency ω, which is confirmed by the simulations at low ion concentration. At high ion concentration, however, the power spectral density follows a power law that is reminiscent of the 1/ω(α) dependence found experimentally at low frequency. On the basis of simulations with and without ion-ion interactions, we attribute the low-frequency power-law dependence to ion-ion correlations. We show that neither a static surface charge density, nor an increased pore length, nor an increased ion valency have a significant effect on the shape of the power spectral density at low frequency.
我们使用线性化平均场理论和朗之万动力学模拟计算了电场驱动的离子通过纳米尺度膜孔的输运的功率谱。值得注意的是,线性化平均场理论预测在低频ω处功率谱密度会出现一个平台,这一预测在低离子浓度的模拟中得到了验证。然而,在高离子浓度下,功率谱密度遵循幂律,这让人联想到在低频下实验中发现的 1/ω(α)依赖性。基于有和没有离子-离子相互作用的模拟,我们将低频幂律依赖性归因于离子-离子相关性。我们表明,无论是静态表面电荷密度、增加的孔长度还是增加的离子价态,都不会对低频功率谱密度的形状产生显著影响。