Stroyuk Oleksandr, Raevskaya Alexandra, Spranger Felix, Gaponik Nikolai, Zahn Dietrich R T
Semiconductor Physics, Chemnitz University of Technology, 09107, Chemnitz, Germany.
L.V. Pysarzhevsky Institute of Physical Chemistry, National Academy of Sciences of Ukraine, Kyiv, 03028, Ukraine.
Chemphyschem. 2019 Jun 17;20(12):1640-1648. doi: 10.1002/cphc.201900088. Epub 2019 May 14.
The temperature dependence of the photoluminescence (PL) intensity of colloidal semiconductor nanocrystals (NCs) makes them an appealing option in bio-sensing applications. Here, we probed the temperature-dependent PL behavior of aqueous glutathione (GSH)-capped Ag-In-S (AIS) NCs and their core/shell AIS/ZnS heterostructures. We show that both core and core-shell materials reveal strong PL quenching upon heating from 10 to 80 °C, which is completely reversible upon cooling. The PL quenching is assigned to the thermally activated dissociation of complexes formed by ligands with the metal cations on the NC surface and the introduction of water into the NC coordination sphere. This unique mechanism of the thermal PL quenching results in a much higher temperature sensitivity of the aqueous colloidal AIS (AIS/ZnS) NCs as compared with previously reported analogs capped by covalently bound ligands. Our results are expected to stimulate further studies on aqueous ternary NCs as colloidal luminescent nano-thermometers applicable for ratiometric temperature sensing.
胶体半导体纳米晶体(NCs)的光致发光(PL)强度与温度的相关性使其在生物传感应用中成为一个有吸引力的选择。在此,我们探究了水相谷胱甘肽(GSH)包覆的Ag-In-S(AIS)纳米晶体及其核壳AIS/ZnS异质结构的温度依赖性PL行为。我们发现,从10℃加热到80℃时,核材料和核壳材料均显示出强烈的PL猝灭,冷却后完全可逆。PL猝灭归因于配体与NC表面金属阳离子形成的配合物的热激活解离以及水进入NC配位球。与先前报道的由共价键合配体包覆的类似物相比,这种独特的热PL猝灭机制导致水相胶体AIS(AIS/ZnS)纳米晶体具有更高的温度敏感性。我们的结果有望激发对水相三元纳米晶体作为适用于比率温度传感的胶体发光纳米温度计的进一步研究。