The PL spectra of 3-LnLnʹ were recorded with a range of excitation wavelengths targeting the absorptions of the different ligands (hfac, Ex = 317 nm; pd •-, Ex = 474, 526 nm). Note that from the absorption spectra of 1-Ln, pd also exhibits some absorbance near 317 nm, albeit at lower intensity (see Figure , 1-Yb vs. 2-Eu). As a control, 2-Ln afforded typical Ln 3+ emission spectra upon excitation of the hfac ligands (2-Eu, Figure ; 2-Yb, ESI Figure ). As shown in Figure , excitation via the hfac ligand in 3-YbEu resulted in emission from Eu 3+ ( = 575-700 nm) and to a lesser extent Yb 3+ ( = 975-1050 nm). Contrastingly, direct excitation of pd •-in the visible region produced NIR emission from Yb 3+ only. In 3-DyYb, (see ESI, Figure ) excitation of the hfac ligand resulted predominantly in Yb 3+ emission, along with somewhat lower levels of emission from Dy 3+ ( = 475-750 nm). Excitation of pd •-however resulted only in emission from Yb 3+ , in line with our observations of 1-Dy. As in the case of 1-Ln, excitation of Thermal ellipsoids drawn at 50% probability. Bond metrics can be found in the ESI Table .