Photoinduced complete melting of spin-Peierls phase in Na-tetracyanoquinodimethane revealed by frequency doubling of coherent molecular oscillations

Photoinduced melting of the spin-Peierls phase was investigated in Na-tetracyanoquinodimethane by pump-probe reflection spectroscopy with a time resolution of 49 fs. Photoirradiation generates coherent molecular oscillation, which indicates that the spin-Peierls dimerization decreased. Increasing the excitation photon density to > 0.02 photon/molecule doubles the oscillation frequency attributable to recovery of the original symmetry, that is, complete melting of the spin-Peierls phase. We observed a complete photoinduced transition with symmetry recovery revealed by frequency doubling of coherent oscillations.