Deciphering the Relaxation Mechanism of Red-Emitting Carbon Dots Using Ultrafast Spectroscopy and Global Target Analysis.

Red-emitting carbon dots (C-dots) have tremendous potential for bioimaging and optoelectronic applications. Here, we investigated the structural modification of red-emitting C-dots due to boron doping and their ultrafast relaxation dynamics. It is evident from the X-ray photoelectron spectroscopy study that the relative percentage of pyrridinic nitrogen is increased at the expense of amino nitrogen and graphitic nitrogen in B-doped C-dots. Transient absorption spectroscopy and global target analysis reveal the formation of an additional excited-state level that takes away a significant amount of the excited-state population after boron doping. This new excited state slows the initial relaxation process toward the emissive state from 317 to 750 fs and increases the overall lifetime from 1.03 to 1.45 ns in B-doped C-dots.