Assessment of false discovery rate control in tandem mass spectrometry analysis using entrapment

Nat Methods. 2025 Jul;22(7):1454-1463. doi: 10.1038/s41592-025-02719-x. Epub 2025 Jun 16.

Abstract

A critical challenge in mass spectrometry proteomics is accurately assessing error control, especially given that software tools employ distinct methods for reporting errors. Many tools are closed-source and poorly documented, leading to inconsistent validation strategies. Here we identify three prevalent methods for validating false discovery rate (FDR) control: one invalid, one providing only a lower bound, and one valid but under-powered. The result is that the proteomics community has limited insight into actual FDR control effectiveness, especially for data-independent acquisition (DIA) analyses. We propose a theoretical framework for entrapment experiments, allowing us to rigorously characterize different approaches. Moreover, we introduce a more powerful evaluation method and apply it alongside existing techniques to assess existing tools. We first validate our analysis in the better-understood data-dependent acquisition setup, and then, we analyze DIA data, where we find that no DIA search tool consistently controls the FDR, with particularly poor performance on single-cell datasets.

MeSH terms

  • Algorithms
  • Humans
  • Proteomics* / methods
  • Reproducibility of Results
  • Software
  • Tandem Mass Spectrometry* / methods