†Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, Colorado 80309, United States.
‡National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
J Am Chem Soc. 2015 May 27;137(20):6452-5. doi: 10.1021/jacs.5b02077. Epub 2015 May 15.
(Ga(1-x)Zn(x))(N(1-x)O(x)) is a visible absorber of interest for solar fuel generation. We present a first report of soluble (Ga(1-x)Zn(x))(N(1-x)O(x)) nanocrystals (NCs) and their excited-state dynamics over the time window of 10(-13)-10(-4) s. Using transient absorption spectroscopy, we find that excited-state decay in (Ga0.27Zn0.73)(N0.27O0.73) NCs has both a short (<100 ps) and a long-lived component, with a long overall average lifetime of ∼30 μs. We also find that the strength of the visible absorption is comparable to that of direct band gap semiconductors such as GaAs. We discuss how these results may relate to the origin of visible absorption in (Ga(1-x)Zn(x))(N(1-x)O(x)) and its use in solar fuel generation.
(Ga1-xZnx)(N1-xOx) 是一种用于太阳能燃料生成的可见光吸收体。我们首次报道了可溶性 (Ga1-xZnx)(N1-xOx) 纳米晶体 (NCs) 及其在 10-13 到 10-4 s 的时间窗口内的激发态动力学。通过瞬态吸收光谱,我们发现 (Ga0.27Zn0.73)(N0.27O0.73) NCs 中的激发态衰减既有短(<100 ps)又有长寿命成分,平均总寿命约为 30 μs。我们还发现,可见光吸收的强度与直接带隙半导体(如 GaAs)相当。我们讨论了这些结果如何与 (Ga1-xZnx)(N1-xOx) 中可见光吸收的起源及其在太阳能燃料生成中的应用有关。