Improved Mass Calibration in MALDI MSI Using Neural Network-Based Recalibration.

Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI MSI) is a powerful imaging method for generating molecular maps of biological samples and has numerous applications in biomedical research. A key challenge in MALDI MSI is to reliably map observed mass peaks to theoretical masses, which can be difficult due to mass shifts that occur during the measurement process. In this paper, we propose MassShiftNet, a novel self-supervised learning framework for mass recalibration. We train a neural network on a data dependent and specifically augmented training data set to directly estimate and correct the mass shift in the observed spectra. In our evaluation, we show that this method is both able to reduce the absolute mass error and to increase the relative mass alignment between peptide MSI spectra acquired from FFPE-fixated tissue using a MALDI time-of-flight (TOF) instrument.