Abstract
Single-molecule (SM) optical spectroscopy and imaging approaches have proven transformative, allowing for deep insights into molecular dynamics and behaviour. Despite their intrinsically weaker signals, vibrational spectro-microscopies have advanced significantly within the past decade, allowing for far-field vibrational spectroscopy and imaging at the SM level under ambient conditions. In this Perspective, we first discuss the critical insights and advancements that allowed for SM vibrational spectroscopy and imaging to be realized, highlighting the technical developments that have allowed vibrational spectro-microscopies to break the SM barrier with far-field optics. We then discuss the unique and exciting opportunities of these SM vibrational methods.