Identifying incoherent mixing effects in the coherent two-dimensional photocurrent excitation spectra of semiconductors
Identifying incoherent mixing effects in the coherent two-dimensional photocurrent excitation spectra of semiconductors
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DOI：
10.1063/5.0121635
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发表时间：
2022-11-28
影响因子：
4.4
通讯作者：
Silva, Carlos
中科院分区：
文献类型：
--
作者：
Bargigia, Ilaria;Gutierrez-Meza, Elizabeth;Silva, Carlos
我们之前已经证明，在通过相位调制和相敏检测测量的二维（2D）相干电子光谱学的背景下，由于通过线性激发途径产生的光激发对而产生的非相干非线性响应作为意外背景对测量信号做出贡献[Gregoire等人，J. Chem.Phys.147，114201（2017）]。在这里，我们模拟的效果，这种不相干的人口混合收集的光电流信号从GaAs太阳能电池通过外部作用于用于相敏检测的跨谐放大器电路，我们确定了一个有效的策略，以识别存在的不相干的人口混合在2D数据。虽然我们发现，非相干混合反映了在四脉冲激励序列中的两个时间延迟变量的线性振幅之间的串扰，我们没有观察到任何严格的相干和非相干的贡献之间的相位相关性，从一个简单的系统建模预期。
We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an incoherent nonlinear response due to pairs of photoexcitations produced via linear excitation pathways contributes to the measured signal as an unexpected background [Gregoire et al., J. Chem. Phys. 147, 114201 (2017)]. Here, we simulate the effect of such incoherent population mixing in the photocurrent signal collected from a GaAs solar cell by acting externally on the transimpedance amplifier circuit used for phase-sensitive detection, and we identify an effective strategy to recognize the presence of incoherent population mixing in 2D data. While we find that incoherent mixing is reflected by the crosstalk between the linear amplitudes at the two time-delay variables in the four-pulse excitation sequence, we do not observe any strict phase correlations between the coherent and incoherent contributions, as expected from modeling of a simple system.