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  • Open Access

Determining adsorbate diffusion coefficients on surfaces from helium-3 spin-echo measurements of atomistic dynamics

Min Lin (林旻)1,*, Sam M. Lambrick1,2, and Andrew P. Jardine1

  • *Contact author: ml976@cam.ac.uk
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Phys. Rev. B 113, 085418 – Published 12 February, 2026

DOI: https://doi.org/10.1103/rys7-5t69

Abstract

Surface diffusion is typically described using tracer diffusion coefficients Ds, which provides a bridge between atomistic dynamics and macroscopic modeling. Here we introduce a new framework to convert helium-3 spin-echo (HeSE) coherent scattering information into tracer diffusion coefficients Ds, systematically distinguishing and treating three different diffusion regimes—Brownian, hopping, and correlated—within a single HeSE analysis framework. HeSE resolves adsorbate motion on both Å length scales and picosecond timescales and yields highly accurate hopping rates and dephasing rates data across a broad range of systems, yet results are seldom reported directly as Ds because a standard conversion from the coherent intermediate scattering function has been lacking. By combining analytical models with molecular dynamics simulations where interadsorbate forces are explicitly included, we establish a unified workflow to extract Ds, and produce an initial benchmark library of HeSE-derived Ds for surface-diffusion studies, providing an experimentally derived tracer diffusion coefficients for a set of adsorbate-substrate systems.

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Phys. Rev. B 113, 085418– Published 12 February, 2026
  • Received 29 April 2025
  • Revised 8 December 2025
  • Accepted 15 January 2026
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