论文标题

通过精确定量光子回收,揭示了钙钛矿膜的内部发光量子效率

Revealing the internal luminescence quantum efficiency of perovskite films via accurate quantification of photon recycling

论文作者

Fassl, Paul, Lami, Vincent, Berger, Felix J., Falk, Lukas M., Zaumseil, Jana, Richards, Bryce S., Howard, Ian A., Vaynzof, Yana, Paetzold, Ulrich W.

论文摘要

内部发光量子效率($ q_ \ mathrm {i}^\ mathrm {lum} $)提供了对半导体光电质量的出色​​评估。确定$ q_ \ mathrm {i}^\ mathrm {lum} $ perovskite膜上的薄膜来自实验可访问的外部发光量子效率($ q_ \ qudrm {e}^\ mathrm {lum {lum} $),这是必不可少的。 ($ p_ \ mathrm {e} $)。在这里,我们基于曲线拟合模型建立了一个分析程序,该过程准确地确定了来自光致发光(PL)光谱的p_ \ mathrm {e} $,该光谱是通过共聚焦显微镜和集成的球体设置测得的。我们表明,与早期假设相比,散射引起的最初捕获的PL解释了通常观察到的红移和扩大的PL光谱形状,并导致$ p_ \ mathrm {e} $在绝对方面高于10%以上。 Applying our model to CH$_3$NH$_3$PbI$_3$ films with exceptionally high $Q_\mathrm{e}^\mathrm{lum}$ up to 47.4% sets a real benchmark for $Q_\mathrm{i}^\mathrm{lum}$ at $78.0 \pm 0.5\%$, revealing there is比以前想象的要多于减少非辐射重组的两个范围。

The internal luminescence quantum efficiency ($Q_\mathrm{i}^\mathrm{lum}$) provides an excellent assessment of the optoelectronic quality of semiconductors. To determine $Q_\mathrm{i}^\mathrm{lum}$ of perovskite films from the experimentally accessible external luminescence quantum efficiency ($Q_\mathrm{e}^\mathrm{lum}$) it is essential to account for photon recycling, and this requires knowledge of the photon escape probability ($p_\mathrm{e}$). Here, we establish an analysis procedure based on a curve fitting model that accurately determines $p_\mathrm{e}$ of perovskite films from photoluminescence (PL) spectra measured with a confocal microscope and an integrating sphere setup. We show that scattering-induced outcoupling of initially-trapped PL explains commonly observed red-shifted and broadened PL spectral shapes and leads to $p_\mathrm{e}$ being more than 10% higher in absolute terms compared to earlier assumptions. Applying our model to CH$_3$NH$_3$PbI$_3$ films with exceptionally high $Q_\mathrm{e}^\mathrm{lum}$ up to 47.4% sets a real benchmark for $Q_\mathrm{i}^\mathrm{lum}$ at $78.0 \pm 0.5\%$, revealing there is beyond a factor of two more scope for reducing non-radiative recombination than previously thought.

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