Localized Photon Absorption in a Single-Crystalline Material

Abstract

The absorption of light is one of the most fundamental processes in condensed-matter physics and optics. Here we investigate under which conditions laser light is absorbed by a crystalline material as an electromagnetic wave with delocalized properties or rather as photons that cause discrete, localized, nanometer-sized consequences. We excite the first-order phase transition of vanadium dioxide with laser pulses of sufficient frequency to overcome the band gap but with insufficient pulse energy to overcome the latent heat. According to Maxwell's equations and Bloch theory, no transition should occur, because nowhere in the material is enough energy. Nevertheless, we observe with ultrafast electron diffraction a disordered crystal geometry with nanometer-sized spots of switched material that grow and diminish with time. The amount of localized spots matches approximately to the number of photons in the absorbed laser wave. Two optical experiments substantiate this phenomenon, and simulations reproduce all measurements results. We discuss whether crystals defects, temperature, or a genuine wavefunction collapse can explain the discovered phenomenon. Practically, the reported absorption mechanism enables local consequences at substantially higher energy than average and provides insight into symmetry breaks and non-thermal fluctuations within complex materials.