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 R 2 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.