The Narrow Pulse Approximation and long length scale determination in xenon gas diffusion NMR studies of model porous media

TL;DR

This study investigates xenon gas diffusion NMR in model porous media, focusing on the breakdown of the narrow pulse approximation, long-length scale structural insights, and finite sample size effects, revealing pressure-dependent diffusion behavior and a consistent Pade length.

Contribution

It introduces a systematic analysis of xenon gas diffusion NMR in porous media, highlighting the effects of pulse duration, pressure, and sample size on diffusion measurements and proposing a Pade-based method to determine characteristic length scales.

Findings

Smaller deviations in D(t) at higher gas pressures.

Long-time diffusion limit proportional to inverse tortuosity.

Pade length approximately 0.13 times bead diameter.

Abstract

We report a systematic study of xenon gas diffusion NMR in simple model porous media: random packs of mono-sized glass beads, and focus on three specific areas peculiar to gas-phase diffusion. These topics are: (i) diffusion of spins on the order of the pore dimensions during the application of the diffusion encoding gradient pulses in a PGSE experiment (breakdown of the 'narrow pulse approximation' and imperfect background gradient cancellation), (ii) the ability to derive long-length scale structural information, and (iii) effects of finite sample size. We find that the time-dependent diffusion coefficient, D(t), of the imbibed xenon gas at short diffusion times in small beads is significantly affected by the gas pressure. In particular, as expected, we find smaller deviations between measured D(t) and theoretical predictions as the gas pressure is increased, resulting from reduced diffusion during the application of the gradient pulse. The deviations are then completely removed when water D(t) is observed in the same samples. The use of gas also allows us to probe D(t) over a wide range of length scales, and observe the long-time asymptotic limit which is proportional to the inverse tortuosity of the sample, as well as the diffusion distance where this limit takes effect (~ 1 - 1.5 bead diameters). The Pade approximation can be used as a reference for expected xenon D(t) data between the short and long time limits, allowing us to explore deviations from the expected behaviour at intermediate times as a result of finite sample size effects. Finally, the application of the Pade interpolation between the long and short time asymptotic limits yields a fitted length scale (the "Pade length"), which is found to be ~ 0.13b for all bead packs, where b is the bead diameter.