Enhancing the Throughput of FT Mass Spectrometry Imaging Using Joint Compressed Sensing and Subspace Modeling.

Mass spectrometry imaging (MSI) allows for untargeted mapping of the chemical compositions of tissues with attomole detection limits. MSI using Fourier transform-based mass spectrometers, such as FT-ion cyclotron resonance (FT-ICR), grants the ability to examine the chemical space with unmatched mass resolution and mass accuracy. However, direct imaging of large tissue samples on FT-ICR is restrictively slow. In this work, we present an approach that combines the subspace modeling of ICR temporal signals with compressed sensing to accelerate high-resolution FT-ICR MSI. A joint subspace and sparsity constrained reconstruction enables the creation of high-resolution imaging data from the sparsely sampled and short-time acquired transients. Simulation studies and experimental implementation of the proposed acquisition in investigation of brain tissues demonstrate a factor of 10 enhancement in throughput of FT-ICR MSI, without the need for instrumental or hardware modifications.

[1]  I. Amster,et al.  Fourier Transform Mass Spectrometry , 1996 .

[2]  Liang Gao,et al.  High-speed compressed-sensing fluorescence lifetime imaging microscopy of live cells , 2020, Proceedings of the National Academy of Sciences.

[3]  Zhi-Pei Liang,et al.  High‐resolution 1H‐MRSI of the brain using SPICE: Data acquisition and image reconstruction , 2016, Magnetic resonance in medicine.

[4]  Lydia Ng,et al.  Allen Brain Atlas: an integrated spatio-temporal portal for exploring the central nervous system , 2012, Nucleic Acids Res..

[5]  Bernhard Spengler,et al.  Atmospheric pressure MALDI mass spectrometry imaging of tissues and cells at 1.4-μm lateral resolution , 2016, Nature Methods.

[6]  A. Marshall,et al.  Fourier transform ion cyclotron resonance mass spectrometry: a primer. , 1998, Mass spectrometry reviews.

[7]  A. Marshall,et al.  High resolution mass spectrometry. , 2012, Analytical chemistry.

[8]  R. Caprioli,et al.  High-speed MALDI MS/MS imaging mass spectrometry using continuous raster sampling. , 2016, Journal of mass spectrometry : JMS.

[9]  Jamie L. Marshall,et al.  Compressed sensing for highly efficient imaging transcriptomics , 2021, Nature Biotechnology.

[10]  Daniel Coelho de Castro,et al.  Accelerating Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry Imaging Using a Subspace Approach. , 2020, Journal of the American Society for Mass Spectrometry.

[11]  Lei Zhu,et al.  Faster STORM using compressed sensing , 2012, Nature Methods.

[12]  D. Donoho,et al.  Sparse MRI: The application of compressed sensing for rapid MR imaging , 2007, Magnetic resonance in medicine.

[13]  R. Caprioli,et al.  High-Speed MALDI-TOF Imaging Mass Spectrometry: Rapid Ion Image Acquisition and Considerations for Next Generation Instrumentation , 2011, Journal of the American Society for Mass Spectrometry.

[14]  E. Moskovets,et al.  Rapid matrix-assisted laser desorption/ionization time-of-flight mass spectrometry imaging with scanning desorption laser beam. , 2014, Analytical chemistry.

[15]  Andrew P. Bowman,et al.  Ultra-High Mass Resolving Power, Mass Accuracy, and Dynamic Range MALDI Mass Spectrometry Imaging by 21-T FT-ICR MS , 2020, Analytical chemistry.