Mapping structures and dynamics with frequency-correlated diffusion exchange

Understanding molecular motion in diffusion-driven complex environments is critical for designing sustainable materials and improving chemical processes. Here, we introduce a multidimensional nuclear magnetic resonance (NMR) method that captures how molecular populations exchange across different dynamic regimes. By extending the modulated gradient spin-echo (MGSE) technique to include frequency–frequency correlations, our approach reveals diffusion pathways that are otherwise obscured in heterogeneous systems. Implemented on a unilateral NMR magnet, the method eliminates gradient pulsing constraints and accesses dynamics in the kilohertz regime. We apply this technique to swelling and acid-catalyzed deconstruction of crosslinked and linear polymers to observe how structural heterogeneity evolves over time. By linking molecular motion to topology and chemical state, we extract physical metrics such as fractal surface dimensionality and reaction wavefront velocity–properties inaccessible..., , # Mapping structures and dynamics with frequency-correlated diffusion exchange

Dataset DOI: [10.5061/dryad.wm37pvn00](10.5061/dryad.wm37pvn00)

## Description of the data and file structure

Raw multidimensional NMR MGSE-MGSE data output from Prospa v3.62 corresponding to the descriptions in the paper \"Mapping structures and dynamics with frequency-correlated diffusion exchange.\" Zipped folder names indicate sample identity (listed below). Each sample folder contains 20 subfolders named N150, N1000, N1150, N1200, N1250, ... N11000. These folders are numbered to indicate the number of echoes recorded within the first 55-ms MGSE block; the number string following \"N1\" is the number of echoes incremented in that block. This can be converted to the modulation frequency of the indirect dimension of the MGSE correlation. Each of these folders contains subfolders named by number of echoes recorded within the second (readout dimension) MGSE block, also 55-ms here. The number of echoes in the r...,