Direct observation of excitons and a continuum of one-dimensional Mott insulators: a reflection-type...

The third-harmonic-generation (THG) spectrum was measured for a NiBr-chain compound, which is a one-dimensional Mott insulator, in a reflection configuration. A sharp peak and a shoulder structure in the THG spectrum are attributed to three-photon resonance to an exciton and a continuum, respectively. The band-edge energy, the exciton binding energy, and the spectral weights for the exciton and the continuum were determined from comparative studies of linear absorption, THG, and electroreflectance spectra. The excitonic effect is more pronounced in the NiCl chain than in the NiBr chain.