Temperature-Induced Self-Compensating Defect Traps and Gain Thresholds in Colloidal Quantum Dots.

Continuous-wave (CW) lasing was recently achieved in colloidal quantum dots (CQDs) by lowering the threshold through the introduction of biaxial strain. However, the CW laser threshold is still much higher than the femtosecond threshold. This must be addressed before electrically injected lasing can be realized. Here we investigate the relationship between threshold and temperature and find a subpicosecond recombination process that proceeds very efficiently at temperatures reached during CW excitation. We combine density functional theory and molecular dynamics simulations to explore potential candidates for such a process, and find that crystal defects having thermally vibrating energy levels can become electronic traps-i.e., they can protrude into the bandgap-when they are sufficiently distorted at higher temperatures. We find that biaxially strained CQDs, which have a lower femtosecond laser threshold than traditional CQDs, result in less heat for a given transparency/gain level and thus undergo this trapping to a lower extent. We also propose methods to tailor CQDs to avoid self-compensating defect traps.

Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy.

Colloidal quantum dots (CQDs) feature a low degeneracy of electronic states at the band edges compared with the corresponding bulk material, as well as a narrow emission linewidth. Unfortunately for potential laser applications, this degeneracy is incompletely lifted in the valence band, spreading the hole population among several states at room temperature. This leads to increased optical gain thresholds, demanding high photoexcitation levels to achieve population inversion (more electrons in excited states than in ground states-the condition for optical gain). This, in turn, increases Auger recombination losses, limiting the gain lifetime to sub-nanoseconds and preventing steady laser action. State degeneracy also broadens the photoluminescence linewidth at the single-particle level. Here we demonstrate a way to decrease the band-edge degeneracy and single-dot photoluminescence linewidth in CQDs by means of uniform biaxial strain. We have developed a synthetic strategy that we term facet-selective epitaxy: we first switch off, and then switch on, shell growth on the (0001) facet of wurtzite CdSe cores, producing asymmetric compressive shells that create built-in biaxial strain, while still maintaining excellent surface passivation (preventing defect formation, which otherwise would cause non-radiative recombination losses). Our synthesis spreads the excitonic fine structure uniformly and sufficiently broadly that it prevents valence-band-edge states from being thermally depopulated. We thereby reduce the optical gain threshold and demonstrate continuous-wave lasing from CQD solids, expanding the library of solution-processed materials that may be capable of continuous-wave lasing. The individual CQDs exhibit an ultra-narrow single-dot linewidth, and we successfully propagate this into the ensemble of CQDs.