Electrochemical control of emission enhancement in solid-state nitrogen-doped carbon quantum dots

Because of their excellent optical and electrical properties, doped carbon quantum dots (CQDs) are expected to be used in novel film optoelectronic devices such as light-emitting diodes and solar cells. However, these device advancements are currently hindered by the elusive photophysical process of doped CQDs in solid-state films. Here, the optical properties of nitrogen-doped CQD (N-CQD) films are studied using spectro-electrochemical (SEC) methods. A distinctive photoluminescence (PL) enhancement phenomenon is observed, in which the PL intensity of the N-CQD film can be increased in both positive and negative electrochemical potential sweeps. The effect of positive potential on PL enhancement is greater (∼340% at +1.4 V), while that of negative potential is slightly weaker (∼10% at -1.4 V). To the best of our knowledge, no similar brightening process has been reported in all previous SEC studies on a variety of QDs, wherein the emission intensity can only exhibit enhancement under positive or negative potential at most. We propose that the above PL brightening is related to the weakened π-π stacking effect after electrochemical charge injection and nitrogen doping plays a crucial role in it. Finally, a low hysteresis reversible electrochemistry regulation of the PL spectrum can be achieved by increasing electrolyte fluidity with argon gas bubbling to reduce local charge aggregation.