Chemistry and Biochemistry Department and ‡Physics Department UCSB , Santa Barbara, California 93117, United States.
ACS Nano. 2013 Nov 26;7(11):9798-807. doi: 10.1021/nn4033097. Epub 2013 Oct 8.
We develop approaches to hold fluorescent silver clusters composed of only 10-20 atoms in nanoscale proximity, while retaining the individual structure of each cluster. This is accomplished using DNA clamp assemblies that incorporate a 10 atom silver cluster and a 15 or 16 atom silver cluster. Thermally modulated fluorescence resonance energy transfer (FRET) verifies assembly formation. Comparison to Förster theory, using measured spectral overlaps, indicates that the DNA clamps hold clusters within roughly 5 to 6 nm separations, in the range of the finest resolutions achievable on DNA scaffolds. The absence of spectral shifts in dual-cluster FRET pairs, relative to the individual clusters, shows that select few-atom silver clusters of different sizes are sufficiently stable to retain structural integrity within a single nanoscale DNA construct. The spectral stability of the cluster persists in a FRET pair with an organic dye molecule, in contrast to the blue-shifted emission of the dye.
我们开发了一种方法,可以将仅由 10-20 个原子组成的荧光银团簇保持在纳米级接近的位置,同时保留每个团簇的个体结构。这是通过使用包含 10 个原子银团簇和 15 或 16 个原子银团簇的 DNA 夹组装来实现的。热调制荧光共振能量转移 (FRET) 验证了组装的形成。与Förster 理论相比,使用测量的光谱重叠表明 DNA 夹将团簇保持在大约 5 到 6nm 的分离距离内,这是在 DNA 支架上可实现的最精细分辨率范围内。与单个团簇相比,双团簇 FRET 对中没有光谱位移表明,不同大小的少数几个原子银团簇足够稳定,可以在单个纳米级 DNA 结构中保持结构完整性。与染料分子的蓝移发射相比,簇的光谱稳定性在 FRET 对中得以保留。