LUT School of Engineering Science, LUT University, 53851 Lappeenranta, Finland.
Leibniz Institute of Photonic Technology, Albert-Einstein-Strasse 9, 07745 Jena, Germany.
Phys Chem Chem Phys. 2023 Jun 21;25(24):16340-16353. doi: 10.1039/d3cp01618h.
The nonresonant background (NRB) contribution to the coherent anti-Stokes Raman scattering (CARS) signal distorts the spectral line shapes and thus degrades the chemical information. Hence, finding an effective approach for removing NRB and extracting resonant vibrational signals is a challenging task. In this work, a bidirectional LSTM (Bi-LSTM) neural network is explored for the first time to remove the NRB in the CARS spectra automatically, and the results are compared with those of three DL models reported in the literature, namely, convolutional neural network (CNN), long short-term memory (LSTM) neural network, and very deep convolutional autoencoders (VECTOR). The results of the synthetic test data have shown that the Bi-LSTM model accurately extracts the spectral lines throughout the range. In contrast, the other three models' efficiency deteriorated while predicting the peaks on either end of the spectra, which resulted in a 60 times higher mean square error than that of the Bi-LSTM model. The Pearson correlation analysis demonstrated that Bi-LSTM model performance stands out from the rest, where 94% of the test spectra have correlation coefficients of more than 0.99. Finally, these four models were evaluated on four complex experimental CARS spectra, namely, protein, yeast, DMPC, and ADP, where the Bi-LSTM model has shown superior performance, followed by CNN, VECTOR, and LSTM. This comprehensive study provides a giant leap toward simplifying the analysis of complex CARS spectroscopy and microscopy.
非共振背景(NRB)对相干反斯托克斯拉曼散射(CARS)信号的贡献会扭曲光谱线形状,从而降低化学信息的质量。因此,找到一种有效去除 NRB 并提取共振振动信号的方法是一项具有挑战性的任务。在这项工作中,首次探索了双向长短时记忆(Bi-LSTM)神经网络,以自动去除 CARS 光谱中的 NRB,并将结果与文献中报道的三种深度学习(DL)模型的结果进行比较,即卷积神经网络(CNN)、长短时记忆(LSTM)神经网络和非常深的卷积自动编码器(VECTOR)。合成测试数据的结果表明,Bi-LSTM 模型准确地提取了整个范围内的光谱线。相比之下,其他三种模型在预测光谱两端的峰值时效率降低,导致均方误差比 Bi-LSTM 模型高 60 倍。Pearson 相关分析表明,Bi-LSTM 模型的性能优于其他模型,其中 94%的测试光谱的相关系数都高于 0.99。最后,将这四种模型应用于四种复杂的实验 CARS 光谱,即蛋白质、酵母、DMPC 和 ADP,Bi-LSTM 模型表现出了优异的性能,其次是 CNN、VECTOR 和 LSTM。这项全面的研究为简化复杂 CARS 光谱学和显微镜分析提供了巨大的飞跃。