Quantitative Mass Spectrometry Imaging Using Multivariate Curve Resolution and Deep Learning: A Case Study.

In the present contribution, a novel approach based on multivariate curve resolution and deep learning (DL) is proposed for quantitative mass spectrometry imaging (MSI) as a potent technique for identifying different compounds and creating their distribution maps in biological tissues without need for sample preparation. As a case study, chlordecone as a carcinogenic pesticide was quantitatively determined in mouse liver using matrix-assisted laser desorption ionization-MSI (MALDI-MSI). For this purpose, data from seven standard spots containing 0 to 20 picomoles of chlordecone and four unknown tissues from the mouse livers infected with chlordecone for 1, 5, and 10 days were analyzed using a convolutional neural network (CNN). To solve the lack of sufficient data for CNN model training, each pixel was considered as a sample, the designed CNN models were trained by pixels in training sets, and their corresponding amounts of chlordecone were obtained by multivariate curve resolution-alternating least-squares (MCR-ALS). The trained models were then externally evaluated using calibration pixels in test sets for 1, 5, and 10 days of exposure, respectively. Prediction R2 for all three data sets ranged from 0.93 to 0.96, which was superior to support vector machine (SVM) and partial least-squares (PLS). The trained CNN models were finally used to predict the amount of chlordecone in mouse liver tissues, and their results were compared with MALDI-MSI and GC-MS methods, which were comparable. Inspection of the results confirmed the validity of the proposed method.