Equilibrium gigahertz acoustics reveals long-range confinement in liquids

Abstract

Understanding how the mechanical properties of liquids confined within nanometer-scale gaps differ from bulk behavior is central to biophysics, lubrication, catalysis, electrochemistry, and surface science. Yet the characterization of ultrathin confined liquids remains challenging, as many existing approaches rely on destructive or intrusive contact-based techniques, mostly measuring the liquid flow in the low frequency regime. Here, we present a non-invasive, all-optical technique based on ultrafast laser ultrasonics that probes confined liquids at equilibrium in the gigahertz frequency range. The method measures the phase and amplitude of time-domain Brillouin scattering signals transmitted through liquid layers whose thickness is varied step by step with subnanometer effective sampling. Supported by numerical modeling of acoustic propagation and optical detection, these signals allow us to extract the thickness-dependent acoustic velocity and attenuation of confined liquids. We show that nanometric confinement modifies the GHz acoustic response of glycerol, the liquid crystal 8CB, and a butyl-based ionic liquid over unexpectedly long spatial scales. These effects extend from a few nanometers to several tens of nanometers and reveal bound interfacial layers, acoustic stiffening, and enhanced solid-like behavior under confinement. Our results open a route to probing liquid confinement in a scarcely explored regime: dynamically measured at gigahertz frequencies, yet sufficiently weakly perturbative to preserve the equilibrium confined state.