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We demonstrate history-dependent or dynamic nano-photoisomerization bysequential formation of multiple memory pathways in photochromic crystals viaoptical near-field interactions. We observed the incident photons passingthrough the photoisomerization memory pathways by a double-probe opticalnear-field microscope, with one probe located on the front surface for localexcitation and the other on the rear surface for near-field observation. Bycarrying out localized near-field excitation twice but at spatially differentpositions, we observed negatively correlated near-field output patterns betweenthe first memory pathway and the second memory pathway. That is, the addedmemory pathway was formed exclusively to the previously formed memory pathway.We also confirmed that the first memory pathway was preserved after the secondmemory pathway was formed. This result indicates that photoisomerization by anoptical near-field in diarylethene crystals has a history dependence, leadingto brain-like dynamic information memorization using light-matter interactionson the nanometer-scale.

History-dependent nano-photoisomerization by optical near-field in photochromic single crystals