Temperature dependence of radiative and non-radiative decay in the luminescence of one-dimensional pyridinium lead halide hybrids
Temperature dependence of radiative and non-radiative decay in the luminescence of one-dimensional pyridinium lead halide hybrids
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一维吡啶鎓卤化铅杂化物发光中辐射和非辐射衰变的温度依赖性
DOI：
10.1039/d3cp02186f
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发表时间：
2023
影响因子：
3.3
通讯作者：
Djurovich, Peter I.
中科院分区：
文献类型：
--
作者：
Alfaraidi, Abdulrahman M.;Schaab, Jonas;McClure, Eric T.;Kellogg, Michael;Hodgkins, Taylor L.;Idris, Muazzam;Bradforth, Stephen E.;Melot, Brent C.;Thompson, Mark E.;Djurovich, Peter I.
研究了有机-无机吡啶溴化铅[（pyH）PbBr 3]和碘化铅[（pyH）PbI 3]化合物的光致发光特性随温度的变化。无机亚结构由PbX 6八面体的面共享链组成。化合物的漫反射光谱显示出低能量吸收特征，与从PbX 3链到吡啶阳离子的电荷转移跃迁一致。这两种化合物在室温下显示出极弱的发光，在冷却至77 K时变得强烈增强。在两种化合物中，宽的、无特征的低能发射（λem > 600 nm）具有大的斯托克斯位移[（pyH）PbBr 3为1.1 eV，（pyH）PbI 3为0.46 eV]，并且被分配为从无机链上的自陷激子的跃迁，而在（pyH）PbBr 3中，在较高能量下的发射（λem = 450 nm）被分配为从自由激子态的发光。从随温度变化的发光强度测量的数据的分析给出了激活能（Ea）的非辐射衰减的自陷激子在（pyH）PbBr 3和（pyH）PbI 3，（Ea = 0.077 eV和0.103 eV，分别）和自由激子在（pyH）PbBr 3（Ea = 0.010 eV）。温度依赖的发光寿命数据的分析表明，另一个非辐射衰减过程中（pyH）PbI 3在较高的温度（Ea = 0.17 eV）。在低于80 K的（PyH）PbI 3的发光寿命的大幅增加是一致的三重态子能级之间的热化。分析的发光功率依赖性（PyH）PbI 3显示超线性响应，提示淬火静态陷阱。
The photoluminescence properties of organic–inorganic pyridinium lead bromide [(pyH)PbBr3] and iodide [(pyH)PbI3] compounds were investigated as a function of temperature. The inorganic substructure consists of face-sharing chains of PbX6 octahedra. Diffuse reflectance spectra of the compounds show low energy absorption features consistent with charge transfer transitions from the PbX3 chains to the pyridinium cations. Both compounds display extremely weak luminescence at room temperature that becomes strongly enhanced upon cooling to 77 K. Broad, featureless low energy emission (λem > 600 nm) in both compounds have large Stokes shifts [1.1 eV for (pyH)PbBr3 and 0.46 eV for (pyH)PbI3] and are assigned to transitions from self-trapped excitons on the inorganic chains whereas emission at higher energy in (pyH)PbBr3 (λem = 450 nm) is assigned to luminescence from a free exciton state. Analysis of data from temperature-dependent luminescence intensity measurements gives activation energies (Ea) for non-radiative decay of the self-trapped excitons in (pyH)PbBr3 and (pyH)PbI3, (Ea = 0.077 eV and 0.103 eV, respectively) and for the free exciton in (pyH)PbBr3 (Ea = 0.010 eV). Analysis of temperature dependent luminescence lifetime data indicates another non-radiative decay process in (pyH)PbI3 at higher temperatures (Ea = 0.17 eV). A large increase in the luminescence lifetime of (pyH)PbI3 below 80 K is consistent with thermalization between triplet sublevels. Analysis of the luminescence power dependence for (pyH)PbI3 shows superlinear response suggestive of quenching by static traps.