Department of Mechanical Engineering , Boston University , Boston , Massachusetts 02215 , United States.
Division of Materials Science & Engineering , Boston University , Boston , Massachusetts 02215 , United States.
Nano Lett. 2019 Aug 14;19(8):5762-5768. doi: 10.1021/acs.nanolett.9b02402. Epub 2019 Jul 22.
Using a novel method developed to quantify the polarizability of photoluminescent nanoparticles in water, we present experimental observations of the extraordinary polarizability exhibited by nanoparticles of commensurate size with the Debye screening length, confirming previously reported theory. Semiconductor quantum dots (QDs) are ideal model nanoparticles to demonstrate this assay, due to their tunable size and bright photoluminescence. This assay is based upon microfluidic chambers with microelectrodes that generate trapping potentials that are weaker than thermal energy. By comparing the local electric field strength and variations in QD concentration, their polarizability was computed and found to agree with estimates based upon the hydrodynamic diameter found using light scattering. Strikingly, the polarizability of the nanoparticles increased 30-fold in low salt conditions compared to high salt conditions due to the increased thickness of the Debye layer relative to the particle radius. In addition to providing evidence that corroborates theoretical work studying direct solutions to the Poisson-Nernst-Planck equations, these observations provide an explanation for the previously observed conductivity dependence of biomolecule polarizability. As the polarizability of nanoparticles is of high importance to the electrically directed assembly of particles, as well as their interactions with other materials in complex environments, we anticipate that these results will be highly relevant to ongoing efforts in materials by design and nanomedicine.
利用一种新开发的方法来量化水中光致发光纳米粒子的极化率,我们展示了与德拜屏蔽长度相匹配的纳米粒子表现出的非凡极化率的实验观察结果,证实了之前报道的理论。半导体量子点 (QD) 是展示这种测定法的理想模型纳米粒子,因为它们的尺寸可调且光致发光强。该测定法基于具有微电极的微流控室,这些微电极产生的捕获势比热能弱。通过比较局部电场强度和 QD 浓度的变化,计算了它们的极化率,并发现其与使用光散射发现的基于流体力学直径的估计值一致。引人注目的是,由于 Debye 层相对于粒子半径的厚度增加,与高盐条件相比,在低盐条件下纳米粒子的极化率增加了 30 倍。这些观察结果除了提供证据证明了直接求解泊松-纳恩斯-普朗克方程的理论工作外,还为先前观察到的生物分子极化率与电导率的依赖性提供了解释。由于纳米粒子的极化率对粒子的电导向组装以及它们在复杂环境中与其他材料的相互作用非常重要,因此我们预计这些结果将与设计材料和纳米医学领域的当前努力高度相关。