Scaling and merging time-resolved pink-beam diffraction with variational inference
Time-resolved x-ray crystallography (TR-X) at synchrotrons and free electron lasers is a promising technique for recording dynamics of molecules at atomic resolution. While experimental methods for TR-X have proliferated and matured, data analysis is often difficult. Extracting small, time-dependent changes in signal is frequently a bottleneck for practitioners. Recent work demonstrated this challenge can be addressed when merging redundant observations by a statistical technique known as variational inference (VI). However, the variational approach to time-resolved data analysis requires identification of successful hyperparameters in order to optimally extract signal. In this case study, we present a successful application of VI to time-resolved changes in an enzyme, DJ-1, upon mixing with a substrate molecule, methylglyoxal. We present a strategy to extract high signal-to-noise changes in electron density from these data. Furthermore, we conduct an ablation study, in which we systematically remove one hyperparameter at a time to demonstrate the impact of each hyperparameter choice on the success of our model. We expect this case study will serve as a practical example for how others may deploy VI in order to analyze their time-resolved diffraction data.
Authors
- Kara A. Zielinski (ORCID: https://orcid.org/0000-0002-9907-5058)
- Lois Pollack (ORCID: https://orcid.org/0000-0002-9366-4396)
- Kevin M. Dalton (ORCID: https://orcid.org/0000-0001-9396-085X)
- Robert Henning (ORCID: https://orcid.org/0000-0003-4404-0189)
- Mark A. Wilson (ORCID: https://orcid.org/0000-0001-6317-900X)
- V. Šrajer (ORCID: https://orcid.org/0000-0003-0710-290X)
- Harrison K. Wang (ORCID: https://orcid.org/0000-0003-4275-9472)
- Doeke R. Hekstra (ORCID: https://orcid.org/0000-0003-2332-9223)
- Cole Dolamore (ORCID: https://orcid.org/0000-0002-7274-1014)
Institutions
- University of Nebraska–Lincoln (US)
- Harvard University (US)
- Cornell University (US)
- SLAC National Accelerator Laboratory (US)
- University of Chicago (US)
- Harvard Bioscience (United States) (US)
- Linac Coherent Light Source (US)
- New York University (US)
Publication Details
- Journal
- Structural Dynamics
- Published
- 2024-11-01
- DOI
- https://doi.org/10.1063/4.0000269
- Citations
- 4
- Primary Topic
- Enzyme Structure and Function
- Type
- article
- Field-Weighted Citation Impact
- 0.47
Funders
- National Science Foundation
- U.S. Department of Energy
- Burroughs Wellcome Fund
- National Institutes of Health
- Office of Science
- National Institute of General Medical Sciences
- Basic Energy Sciences
- SLAC National Accelerator Laboratory