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The photophysical properties of Bi82+ and Bi53+ polycations stabilized by[AlCl4]- have been studied experimentally and theoretically. The obtainedproduct was thoroughly evaluated by powder X-ray diffraction andphotoluminescence spectroscopy, making it clear that both Bi82+ and Bi53+contribute to the observed broad near-infrared emission. Furthermore, it wasrevealed that Bi82+ polycation mainly results in the emission peaking at ca.1180 nm, while Bi53+ the longer-wavelength emission. The following quantumchemistry calculation on Bi82+ polycation helps us attribute some observedexcitation bands in the visible spectral range to specific electronictransitions of bismuth polycations. It is believed that systematicalinvestigation of structural and luminescent properties as well as detailedquantum chemistry calculation of molecular crystals containing such kinds ofbismuth units allows us to obtain a clearer picture on bismuth-relatedphotophysical behaviors, which not only serve to solve the confusions on theluminescence origin of bismuth in other material systems such as bulk glasses,glass fibers and conventional crystals, but also is helpful to develop novelapplicable broadband tunable laser mediums.

Experimental and Theoretical Studies of Photoluminescence from Bi82+ and Bi53+ stabilized by [AlCl4]- in Molecular Crystals