Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
Phys Chem Chem Phys. 2012 May 21;14(19):6974-80. doi: 10.1039/c2cp24044k. Epub 2012 Mar 22.
Quantum cutting (QC) of one visible photon into two infrared ones has been reported for the lanthanide ion couple (Tm(3+), Yb(3+)) in a variety of host lattices. The mechanism responsible for QC was assumed to be a cooperative energy transfer (ET) process from Tm(3+) to two Yb(3+) ions, however, no solid evidence was presented. Herein we report visible-to-infrared QC for (Tm(3+), Yb(3+)) in YPO4 phosphors. The ET process from the excited (1)G4 level of Tm(3+) to Yb(3+) was investigated in detail by means of optical spectroscopy. By monitoring the steady-state photoluminescence (PL) and PL decay of the intermediate (3)F4 level of Tm(3+) as a function of the Yb(3+) concentration, we demonstrated the QC of one incident blue photon into one near-infrared emitting photon at 1004 nm from Yb(3+) and simultaneously into one mid-infrared emitting photon at 1791 nm from Tm(3+), rather than two emitting photons from Yb(3+). It was revealed that such visible-to-infrared QC was induced by phonon-assisted ET instead of cooperative ET as previously reported. This kind of QC phosphors may have potential as solar spectral converters to enhance the external quantum efficiency in multi-junction solar cells based on narrow band-gap semiconductors such as Ge, PbS or In1-xGaxN.
已报道将一个可见光子量子切割(QC)成两个红外光子的现象,这发生在一系列基质晶格中的镧系离子对(Tm(3+),Yb(3+))中。负责 QC 的机制被假定为 Tm(3+)到两个 Yb(3+)离子的协同能量转移(ET)过程,然而,并没有提出确凿的证据。在此,我们报告了 YPO4 荧光粉中(Tm(3+),Yb(3+))的可见到红外 QC。通过光学光谱详细研究了 Tm(3+)的激发(1)G4 能级到 Yb(3+)的 ET 过程。通过监测 Tm(3+)的中间(3)F4 能级的稳态光致发光(PL)和 PL 衰减随 Yb(3+)浓度的变化,我们证明了一个入射蓝光光子可以量子切割成一个来自 Yb(3+)的近红外发射光子,波长为 1004nm,同时也可以量子切割成一个来自 Tm(3+)的中红外发射光子,波长为 1791nm,而不是来自 Yb(3+)的两个发射光子。结果表明,这种可见到红外 QC 是由声子辅助 ET 引起的,而不是之前报道的协同 ET。这种 QC 荧光粉可能有潜力作为太阳能光谱转换器,以提高基于窄带隙半导体(如 Ge、PbS 或 In1-xGaxN)的多结太阳能电池的外量子效率。