Physics-Constrained Learning of Dose-Dependent Spectral Degradation in Metal--Organic Frameworks from In Situ Low-Loss EELS
Abstract
Electron-beam irradiation limits atomic-resolution characterization of beam-sensitive hybrid materials, yet quantitative models that connect \textit{in situ} spectroscopy to dose-dependent degradation remain scarce. Here we use a physics-informed neural network (PINN) to model beam-induced spectral evolution in MIL-101(Fe) from an in situ low-loss electron energy-loss spectroscopy (EELS) dose series. Each spectrum is reduced to fixed-window low-loss descriptors, ñeff,j(Φ)=∫𝒲jS(E,Φ) dE, evaluated over nominal π--π*, C--C, C--O, and M--O windows. These descriptors are relative window-integrated low-loss spectral areas, not absolute f-sum-rule effective electron numbers. For each spectral channel, a latent integrity variable Ci(Φ) obeys the same uncoupled power-law degradation equation in normalized dose space, dCi/dϕ=−ki Cipi, regularized by monotonicity, boundedness, and a single hierarchy prior kC−O≥ kC−C. Applied to nine dose frames spanning 152--1368~e-/Å2, the ensemble PINN identifies C--O and C--C as the most strongly dose-sensitive linker-associated channels, with half-integrity thresholds of approximately 1.0×103~e-/Å2. The 1--3~eV π--π*-labelled window increases with dose and is therefore interpreted as a mixed low-energy response, likely involving oscillator-strength redistribution rather than direct monotonic loss of a single bond population. The framework provides a dose-dependent, spectroscopy constrained description of MOF degradation while also defining the limits of what fixed-window low-loss EELS can assign without independent chemical-state validation.
Versions
Related
- Acquisition-calibrated degradation synthesis and dual-domain reconstruction for accelerated spectral-domain OCT
- Spectral Geometry and Dispersion-Constrained Projection of Diffusive Fields
- Wavelength-Dependent Photoluminescence Mapping of Depth-Dependent Degradation Under Thermal Stress in Phenethylammonium Tetrafluoroborate Treated Perovskite Solar Cells
- Topology-dependent relativistic degradation of multipartite entanglement
- Transport simulations with a constrained momentum-dependent chiral mean-field equation of state at various isospin fractions
BibTeX
@misc{santos2026physicsconstrained,
title = {{Physics-Constrained Learning of Dose-Dependent Spectral Degradation in Metal--Organic Frameworks from In Situ Low-Loss EELS}},
author = {Gabriel T. dos Santos and Roberto dos Reis and Vinayak P. Dravid},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2605.01697},
eprint = {2605.01697},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2605.01697},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Physics-Constrained Learning of Dose-Dependent Spectral Degradation in Metal--Organic Frameworks from In Situ Low-Loss EELS
AU - Gabriel T. dos Santos
AU - Roberto dos Reis
AU - Vinayak P. Dravid
PY - 2026
DA - 2026/09/30
PB - arXiv
DO - 10.48550/arxiv.2605.01697
UR - https://arxiv.org/abs/2605.01697
AB - Electron-beam irradiation limits atomic-resolution characterization of beam-sensitive hybrid materials, yet quantitative models that connect \textit{in situ} spectroscopy to dose-dependent degradation remain scarce. Here we use a physics-informed neural network (PINN) to model beam-induced spectral evolution in MIL-101(Fe) from an in situ low-loss electron energy-loss spectroscopy (EELS) dose series. Each spectrum is reduced to fixed-window low-loss descriptors, ñ_eff,j(Φ)=∫_𝒲_jS(E,Φ) dE, evaluated over nominal π--π^*, C--C, C--O, and M--O windows. These descriptors are relative window-integrated low-loss spectral areas, not absolute f-sum-rule effective electron numbers. For each spectral channel, a latent integrity variable C_i(Φ) obeys the same uncoupled power-law degradation equation in normalized dose space, dC_i/dϕ=−k_i C_i^p_i, regularized by monotonicity, boundedness, and a single hierarchy prior k_C−O≥ k_C−C. Applied to nine dose frames spanning 152--1368~e^-/Å^2, the ensemble PINN identifies C--O and C--C as the most strongly dose-sensitive linker-associated channels, with half-integrity thresholds of approximately 1.0×10^3~e^-/Å^2. The 1--3~eV π--π^*-labelled window increases with dose and is therefore interpreted as a mixed low-energy response, likely involving oscillator-strength redistribution rather than direct monotonic loss of a single bond population. The framework provides a dose-dependent, spectroscopy constrained description of MOF degradation while also defining the limits of what fixed-window low-loss EELS can assign without independent chemical-state validation.
ER -