Encapsulating photoluminescent lanthanide ions like erbium (Er) into fullerene cages affords photoluminescent endohedral metallofullerenes (EMFs). Few reported photoluminescent Er-EMFs are all based on encapsulation of multiple (two to three) metal atoms, whereas mono-Er-EMFs exemplified by Er@C are not photoluminescent due to its narrow optical bandgap. Herein, by entrapping an Er-cyanide cluster into various C cages to form novel Er-monometallic cyanide clusterfullerenes (CYCFs), ErCN@C (C (5), C (6), and C (9)), the photoluminescent properties of CYCFs are investigated, and obvious near-infrared (NIR) photoluminescence only is observed for ErCN@C (5)-C . Combined with a comparative photoluminescence study of three medium-bandgap di-Er-EMFs, including Er @C (6)-C , Er O@C (6)-C , and Er C @C (6)-C , this study proposes that the optical bandgap can be used as a simple criterion for switching the photoluminescence of Er-EMFs, and the bandgap threshold is determined to be between 0.83 and 0.74 eV. Furthermore, the photoluminescent patterns of these three di-Er-EMFs differ dramatically. It is found that the location of the Er atom within the same C (6)-C cage is almost fixed and independent on the endo-unit; thus the previous statement on the key role of metal position in photoluminescence of di-Er-EMFs seems erroneous, and the geometric configuration of the endo-unit, especially the bridging mode of two Er ions, is decisive instead.
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