Helium spin-echo as a surface-sensitive probe of vibrational energy dissipation

Abstract

Understanding vibrational lifetimes at surfaces is central to advancing our knowledge of thermal transport, energy dissipation, and nanoscale friction. While phonon lifetimes in the bulk are routinely accessed via inelastic neutron scattering or optical phonon modes via high-resolution Raman spectroscopy, the direct measurement of lifetimes for low-energy surface acoustic phonons, particularly at finite wavevector, remains a major experimental challenge. This is due to the extremely narrow linewidths involved, corresponding to picosecond lifetimes and requiring µeV energy resolution. Here, we demonstrate how helium spin-echo (HeSE) spectroscopy overcomes this limitation, enabling direct access to the intrinsic linewidths and lifetimes of surface vibrational modes. For Ag(001), we map the full dispersion of the Rayleigh wave. Temperature-dependent measurements at finite wavevector reveal its weak anharmonicity and allow extraction of its intrinsic linewidth from the associated broadening. This corresponds to a phonon lifetime of ≈29 ps at 0 K and a propagation length of ≈44 nm, indicating coherence over tens of nanometres despite electron–phonon and defect-induced scattering. In a complementary application, we explore the vibrational dynamics of organic adsorbates, using cobalt phthalocyanine (CoPc) on Ag(001) as a model system. Low-frequency frustrated translational modes of the adsorbed molecules illustrate HeSE’s capability to probe vibrational damping in complex adsorbate–surface systems. The observed linewidths reflect enhanced dissipation arising from intermolecular interactions and coupling to the substrate. These findings establish HeSE as a sensitive probe of vibrational energy dissipation at hybrid organic–metal interfaces. Taken together, these capabilities open new avenues for the quantitative study of phonon lifetimes and linewidths in complex and emergent material systems, including 2D heterostructures and unconventional superconductors, where vibrational dynamics and their coupling to other degrees of freedom play a decisive role.