Here we present an augmented form of two-dimensional correlation spectroscopy (2DCOS), that integrates in a single format data from spectroscopic and multiple non-spectroscopic sources for analysis. The integration is effected by augmenting every spectrum in a hyperspectral data set with relevant non-spectroscopic data to permit two-dimensional correlation analysis of the ensemble of augmented spectra. A k-means clustering is then applied to the results of the perturbation domain decomposition to determine which Raman peaks cluster with any of the non-spectroscopic data. We introduce and explain the method with the aid of synthetic spectra and synthetic non-spectroscopic data. We then demonstrate this approach with data using Raman spectra from human embryonic stem cell aggregates undergoing directed differentiation toward pancreatic endocrine cells and parallel bioassays of hormone mRNA expression and C-peptide levels in spent medium. These pancreatic endocrine cells generally contain insulin or glucagon. Insulin has disulfide bonds that produce Raman scattering near 513 cm-1, but no tryptophan. For insulin-positive cells, we found that the application of multisource correlation analysis revealed a high correlation between insulin mRNA and Raman scattering in the disulfide region. In contrast, glucagon has no disulfide bonds but does contain tryptophan. For glucagon-positive cells, we also observed a high correlation between glucagon mRNA and tryptophan Raman scattering (~757 cm-1). We conclude with a discussion of methods to enhance spectral resolution and its effects on the performance of multisource correlation analysis.

中文翻译：

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EXPRESS：用于联合分析光谱和不同来源的相关变化的增强二维相关光谱

在这里，我们提出了一种增强形式的二维相关光谱 (2DCOS)，它集成了来自光谱和多个非光谱源的单一格式数据进行分析。积分是通过用相关的非光谱数据增加高光谱数据集中的每个光谱来实现的，以允许对增强光谱的集合进行二维相关分析。然后将 k 均值聚类应用于扰动域分解的结果，以确定哪个拉曼峰与任何非光谱数据聚类。我们借助合成光谱和合成非光谱数据介绍和解释该方法。然后，我们使用来自人类胚胎干细胞聚集体的拉曼光谱的数据证明了这种方法，这些数据正在经历向胰腺内分泌细胞的定向分化，并对用过的培养基中的激素 mRNA 表达和 C 肽水平进行平行生物测定。这些胰腺内分泌细胞通常含有胰岛素或胰高血糖素。胰岛素具有二硫键，可在 513 cm-1 附近产生拉曼散射，但没有色氨酸。对于胰岛素阳性细胞，我们发现多源相关分析的应用揭示了胰岛素 mRNA 与二硫化物区域拉曼散射之间的高度相关性。相比之下，胰高血糖素没有二硫键，但含有色氨酸。对于胰高血糖素阳性细胞，我们还观察到胰高血糖素 mRNA 与色氨酸拉曼散射 (~757 cm-1) 之间的高度相关性。