ABSTRACT
The fluorescent molecules utilizing hybridized local and charge-transfer (HLCT) state as potential organic light-emitting diodes materials attract extensive attention due to their high exciton utilization. In this work, we have performed the density functional theory method on three HLCT-state molecules to investigate their excited-state potential energy surface (PES). The calculated results indicate the T1 and T2 energy gap is quite large, and the T2 is very close to S1 in the energy level. The large gap is beneficial for inhibiting the internal conversion between T1 and T2, and quite closed S1 and T2 energies are favor for activating the T2 â S1 reverse intersystem crossing path. However, considering the singlet excited-state PES by twisting the triphenylamine (TPA) or diphenylamine (PA) group, it can be found that the TPA or PA group almost has no influence on T1 and T2 energy levels. However, the plots of S1 PES display two kinds of results that the S1 emissive state is dominated by charge-transfer (CT) or HLCT state. The CT emission state formation would decrease the S1 energy level, enlarge the S1 and T2 gap, and impair the triplet exciton utilization. Therefore, understanding the relationship between the S1 PES and molecular structures is important for designing high-performance luminescent materials utilizing HLCT state.
ABSTRACT
We realized a single-mode laser with an ultra-high quality factor in individual cesium lead bromide (CsPbBr3) perovskite micro-hemispheres fabricated by chemical vapor deposition. A series of lasing property analysis based on cavity size was reported under this material system. Due to good optical confinement capability of the whispering gallery resonant cavity and high optical gain of CsPbBr3 perovskite micro-hemispheres, single-mode lasing behavior was achieved with an ultra-high quality factor as large as 11,460 at room temperature. To study in detail the physical effects between lasing threshold and cavity, a set of cavity size dependence photoluminescence analyses were performed. We found that the lasing threshold increases while the cavity size decreases. Time-resolved PL analysis was conducted to confirm the relation between cavity size and lasing threshold. The larger cavity stands for longer PL lifetime and indicates easier-to-achieve carrier population inversion. Strong Purcell enhancement could be further investigated by the spontaneous emission coupling factor ß and internal quantum efficiency as a function of cavity size. A high ß-factor of 0.37 could be obtained from a 2.2 µm diameter hemisphere microcavity and a high Purcell factor of 14 in a 1.9 µm diameter hemisphere microcavity showing strong Purcell enhancement effect in our system.