Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA.
J Am Chem Soc. 2012 Sep 5;134(35):14618-23. doi: 10.1021/ja3062425. Epub 2012 Aug 23.
We developed a system to reversibly encapsulate small numbers of molecules in an array of nanofabricated "dimples". This system enables highly parallel, long-term, and attachment-free studies of molecular dynamics via single-molecule fluorescence. In studies of bimolecular reactions of small numbers of confined molecules, we see phenomena that, while expected from basic statistical mechanics, are not observed in bulk chemistry. Statistical fluctuations in the occupancy of sealed reaction chambers lead to steady-state fluctuations in reaction equilibria and rates. These phenomena are likely to be important whenever reactions happen in confined geometries.
我们开发了一种系统，可以将少量分子可逆地包裹在纳米制造的“酒窝”阵列中。通过单分子荧光，该系统可以实现高度平行、长期和无附着的分子动力学研究。在对少量受限分子的双分子反应的研究中，我们观察到了一些现象，这些现象虽然可以从基本的统计力学中预测到，但在体相化学中却观察不到。密封反应室中占据数的统计波动导致反应平衡和速率的稳态波动。这些现象在反应发生在受限几何形状时很可能很重要。
