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首页> 外文期刊>RSC Advances >Luminescence and photoelectrochemical properties of size-selected aqueous copper-doped Ag–In–S quantum dots
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Luminescence and photoelectrochemical properties of size-selected aqueous copper-doped Ag–In–S quantum dots

机译：尺寸选择的铜掺杂Ag-In-S水溶液量子点的发光和光电化学性质

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Ternary luminescent copper and silver indium sulfide quantum dots (QDs) can be an attractive alternative to cadmium and lead chalcogenide QDs. The optical properties of Cu–In–S and Ag–In–S (AIS) QDs vary over a broad range depending on the QD composition and size. The implementation of ternary QDs as emitters in bio-sensing applications can be boosted by the development of mild and reproducible syntheses directly in aqueous solutions as well as the methods of shifting the photoluminescence (PL) bands of such QDs as far as possible into the near IR spectral range. In the present work, the copper-doping of aqueous non-stoichiometric AIS QDs was found to result in a red shift of the PL band maximum from around 630 nm to ～780 nm and PL quenching. The deposition of a ZnS shell results in PL intensity recovery with the highest quantum yield of 15%, with almost not change in the PL band position, opposite to the undoped AIS QDs. Size-selective precipitation using 2-propanol as a non-solvent allows discrimination of up to 9 fractions of Cu-doped AIS/ZnS QDs with the average sizes in the fractions varying from around 3 to 2 nm and smaller and with reasonably the same composition irrespective of the QD size. The decrease of the average QD size results in a blue PL shift yielding a series of bright luminophors with the emission color varies from deep-red to bluish-green and the PL efficiency increases from 11% for the first fraction to up to 58% for the smallest Cu-doped AIS/ZnS QDs. The rate constant of the radiative recombination of the size-selected Cu-doped AIS/ZnS QDs revealed a steady growth with the QD size decrease as a result of the size-dependent enhancement of the spatial exciton confinement. The copper doping was found to result in an enhancement of the photoelectrochemical activity of CAIS/ZnS QDs introduced as spectral sensitizers of mesoporous titania photoanodes of liquid-junction solar cells.
机译：三元发光的铜和银铟硫化物量子点（QD）可能是镉和硫属元素化物QD的诱人替代品。 Cu-In-S和Ag-In-S（AIS）量子点的光学特性在很大的范围内变化，这取决于量子点的成分和大小。通过在水溶液中直接开发温和且可重现的合成物以及将此类QD的光致发光（PL）谱带尽可能移近的方法，可以促进三元QD在生物传感应用中作为发射体的实现。红外光谱范围。在目前的工作中，发现非化学计量AIS QD水溶液中的铜掺杂会导致最大PL带从约630 nm到约780 nm发生红移，并导致PL猝灭。 ZnS壳的沉积导致PL强度恢复，最高量子产率为15％，与未掺杂的AIS QD相反，PL谱带位置几乎没有变化。使用2-丙醇作为非溶剂进行尺寸选择沉淀可区分多达9个Cu掺杂AIS / ZnS QD组分，其平均粒径在3至2 nm之间，更小且组成合理与QD大小无关。平均QD尺寸的减小导致蓝色PL偏移，产生一系列明亮的发光体，其发光颜色从深红色变为蓝绿色，并且PL效率从第一个分数的11％增加到最大的58％。最小的铜掺杂AIS / ZnS QD。尺寸选择的掺杂铜的AIS / ZnS量子点的辐射复合速率常数显示，随着空间激子约束的尺寸依赖性增强，量子点尺寸减小，其稳定增长。发现铜掺杂导致作为液体结太阳能电池的介孔二氧化钛光阳极的光谱敏化剂引入的CAIS / ZnS QD的光电化学活性增强。

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