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Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-09-22 , DOI: 10.1002/aenm.202001828 Ardalan Armin 1 , Nasim Zarrabi 1 , Oskar J. Sandberg 1 , Christina Kaiser 1 , Stefan Zeiske 1 , Wei Li 1 , Paul Meredith 1
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-09-22 , DOI: 10.1002/aenm.202001828 Ardalan Armin 1 , Nasim Zarrabi 1 , Oskar J. Sandberg 1 , Christina Kaiser 1 , Stefan Zeiske 1 , Wei Li 1 , Paul Meredith 1
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Free carrier photogeneration in bulk‐heterojunction solar cells composed of blends of acceptor and donor organic semiconductors proceeds via intermolecular charge transfer (CT) states. Non‐adiabatic Marcus theory has proven valid to explain the absorption and emission of these sub‐gap states which have extremely weak emission probabilities and absorption cross sections making them difficult to probe directly using optical spectroscopy. Therefore, the CT state parameters involved in the Marcus model are often extracted from fittings on the photovoltaic external quantum efficiency (EQEPV) and electroluminescence. These two spectra are (ideally) interrelated via the so‐called reciprocity principle. In this paper, the limitations of such an approach are demonstrated, in particular the impact of simple low finesse cavity interference effects acting as an uneven spectral filter for emission and absorption. This can produce almost spurious CT state parameterization with, for example, relative errors as large as 90% in absorption coefficients obtained from EQEPV. It is shown how these limitations can be partially lifted using an iterative transfer matrix approach applied to the EQEPV.
中文翻译：
使用光伏外部量子效率的电荷转移状态参数化的局限性
由受体和施主有机半导体的混合物组成的体-异质结太阳能电池中的自由载流子光生通过分子间电荷转移（CT）状态进行。事实证明，非绝热马库斯理论可有效解释这些亚隙态的吸收和发射，这些子隙态具有极弱的发射概率和吸收截面，这使它们很难直接用光谱法探测。因此，通常从光伏外部量子效率（EQE PV）的拟合中提取Marcus模型中涉及的CT状态参数。）和电致发光。这两个光谱通过所谓的互惠原理相互关联（理想）。在本文中，证明了这种方法的局限性，特别是简单的低精细腔干涉效应的影响，该效应充当发射和吸收的不均匀光谱滤波器。这可能会产生几乎是虚假的CT状态参数化，例如，从EQE PV获得的吸收系数中的相对误差高达90％。它显示了如何使用应用于EQE PV的迭代转移矩阵方法来部分解除这些限制。
更新日期：2020-11-03
中文翻译：
使用光伏外部量子效率的电荷转移状态参数化的局限性
由受体和施主有机半导体的混合物组成的体-异质结太阳能电池中的自由载流子光生通过分子间电荷转移（CT）状态进行。事实证明，非绝热马库斯理论可有效解释这些亚隙态的吸收和发射，这些子隙态具有极弱的发射概率和吸收截面，这使它们很难直接用光谱法探测。因此，通常从光伏外部量子效率（EQE PV）的拟合中提取Marcus模型中涉及的CT状态参数。）和电致发光。这两个光谱通过所谓的互惠原理相互关联（理想）。在本文中，证明了这种方法的局限性，特别是简单的低精细腔干涉效应的影响，该效应充当发射和吸收的不均匀光谱滤波器。这可能会产生几乎是虚假的CT状态参数化，例如，从EQE PV获得的吸收系数中的相对误差高达90％。它显示了如何使用应用于EQE PV的迭代转移矩阵方法来部分解除这些限制。
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