Direct observation of water mediated single proton transport between hBN surface defects

TL;DR

This study visualizes single proton transport at the water/hBN interface using optical microscopy, revealing water-mediated proton mobility and providing insights into interfacial charge transport mechanisms.

Contribution

It introduces a novel optical method to directly observe single proton transport at room temperature in aqueous environments, overcoming limitations of traditional surface science techniques.

Findings

Protons move via jumps between surface defects facilitated by water.

Proton mobility is enhanced under illumination but limited by defect desorption.

Water acts as a preferred pathway for lateral proton transport.

Abstract

Aqueous proton transport at interfaces is ubiquitous and crucial for a number of fields, ranging from cellular transport and signaling, to catalysis and membrane science. However, due to their light mass, small size and high chemical reactivity, uncovering single proton surface transport at room temperature and in aqueous environment has so far remained out-of-reach of conventional atomic-scale surface science techniques, such as STM. Here, we use single-molecule localization microscopy techniques to resolve optically the transport of individual excess protons at the interface of hexagonal boron nitride crystals and aqueous solutions at room temperature. Our label-free approach relies on the successive protonation and activation of optically active defects at the surface of the crystal allowing us to resolve interfacial proton transport at the single molecule scale with nanometric resolution and over micrometer range. Proton trajectories are revealed as a succession of jumps between proton-binding defects, mediated by interfacial water. We demonstrate unexpected interfacial proton mobility under illumination, limited by proton desorption from individual defects. The proposed mechanism is supported by ab initio molecular dynamics simulations of defected and pristine hBN/water interface. Our observations provide direct experimental evidence at the single molecule scale that interfacial water provides a preferential pathway for lateral proton transport. Our findings have fundamental and general implications for water-mediated molecular charge transport at interfaces.