Department of Chemistry, University of Waterloo, 200 University Avenue West, Waterloo, Ontario N2L 3G1, Canada.
J Am Chem Soc. 2010 Jul 14;132(27):9250-2. doi: 10.1021/ja101333h.
We report a colloidal synthesis of gallium oxide (Ga(2)O(3)) nanocrystals having metastable cubic crystal structure (gamma phase) and uniform size distribution. Using the synthesized nanocrystal size series we demonstrate for the first time a size-tunable photoluminescence in Ga(2)O(3) from ultraviolet to blue, with the emission shifting to lower energies with increasing nanocrystal size. The observed photoluminescence is dominated by defect-based donor-acceptor pair recombination and has a lifetime of several milliseconds. Importantly, the decay of this phosphorescence is also size dependent. The phosphorescence energy and the decay rate increase with decreasing nanocrystal size, owing to a reduced donor-acceptor separation. These results allow for a rational and predictable tuning of the optical properties of this technologically important material and demonstrate the possibility of manipulating the localized defect interactions via nanocrystal size. Furthermore, the same defect states, particularly donors, are also implicated in electrical conductivity rendering monodispersed Ga(2)O(3) nanocrystals a promising material for multifunctional optoelectronic structures and devices.
我们报告了一种胶体合成法,用于制备具有亚稳立方晶体结构(γ相)和均匀尺寸分布的氧化镓(Ga2O3)纳米晶体。利用合成的纳米晶尺寸系列,我们首次证明了 Ga2O3 的尺寸可调光致发光,从紫外光到蓝光,随着纳米晶尺寸的增加,发射向更低的能量移动。观察到的光致发光主要由基于缺陷的施主-受主对复合主导,具有几毫秒的寿命。重要的是,这种磷光的衰减也与尺寸有关。由于施主-受主分离减少,磷光能量和衰减率随纳米晶尺寸的减小而增加。这些结果允许对这种具有重要技术意义的材料的光学性质进行合理和可预测的调整,并证明了通过纳米晶尺寸来操纵局部缺陷相互作用的可能性。此外,相同的缺陷态,特别是施主,也与电导率有关,这使得单分散 Ga2O3 纳米晶体成为多功能光电结构和器件的有前途的材料。