History-dependent Nano-Photoisomerization by Optical Near-Field in Photochromic Single Crystals

The history dependence of physical systems is promising for solving complex problems. To exploit spontaneous nanometre-scale optical memory for computation, the history dependence must be elucidated. Here, we demonstrate history-dependent or dynamic nano-photoisomerization through the sequential formation of multiple memory pathways in photochromic crystals via optical near-field interactions. Incident photons passing through photoisomerization memory pathways are observed using a double-probe optical near-field microscope, with one probe located on the front surface for local excitation and the other on the rear surface for near-field observations. By performing localised near-field excitation twice but at spatially different positions, negatively correlated near-field output patterns are observed between the first and second memory pathways. We also confirm that the first memory pathway is preserved after the formation of the second memory pathway. This result indicates that photoisomerization using an optical near field in diarylethene crystals has a history dependence, leading to brain-like dynamic information memorisation.