Dynamic Variation of Excitonic Coupling in Excited Bilayer Graphene Quantum Dots

The intermolecular interaction determines the photophysical properties of the organic aggregates,which are critical to the performance of organic photovoltaics.Here,excitonic coupling,an important intermolecular interaction in organic aggregates,between theπ-stacking graphene quantum dots is studied by using transient absorption spectroscopy.We find that the spectral evolution of the ground state bleach arises from the dynamic variation of the excitonic coupling in the excitedπ-stacks.According to the spectral simulations,we demonstrate that the kinetics of the vibronic peak can be exploited as a probe to measure the dynamics of excitonic coupling in the excitedπ-stacks.

Probing angle-resolved reflection signatures of intralayer and interlayer excitons in monolayer and bilayer MoS_(2)

Strongly bound excitons in atomically thin transition metal dichalcogenides offer many opportunities to reveal the underlying physics of basic quasiparticles and many-body effects in the two-dimensional(2D)limit.Comprehensive reflection investigation on band-edge exciton transitions is essential to exploring wealthy light–matter interactions in the emerging 2D semiconductors,whereas angle-resolved reflection(ARR)characteristics of intralayer and interlayer excitons in 2D MoS_(2)layers remain unclear.Herein,we report ARR spectroscopic features of A,B,interlayer excitons in monolayer(ML)and bilayer(BL)MoS_(2)on three kinds of photonic substrates,involving distinct exciton–photon interactions.In a BL MoS_(2)on a protected silver mirror,the interlayer exciton with one-third amplitude of A exciton appears at 0.05 eV above the A exciton energy,exhibiting an angleinsensitive energy dispersion.When ML and BL MoS_(2)lie on a SiO_(2)-covered silicon,the broad trapped-photon mode weakly couples with the reflection bands of A and B excitons by the Fano resonance effect,causing the asymmetric lineshapes and the redshifted energies.After transferring MoS_(2)layers onto a one-dimensional photonic crystal,two high-lying branches of B-exciton polaritons are formed by the interactions between B excitons and Bragg photons,beyond the weak-coupling regime.This work provides ARR spectral benchmarks of A,B,interlayer excitons in ML and BL MoS_(2),gaining insights into the interpretation of light–matter interactions in 2D semiconductors and the design of their devices for practical photonic applications.

Switching on/off phosphorescent or non-radiative channels by aggregation-induced quantum interference

Pure organic materials with persistent and efficient room-temperature phosphorescence have recently aroused great research interest due to their vast potential in applications.One crucial design principle for such materials is to suppress as much as possible the non-radiative decay of the triplet exciton while maintaining a moderate phosphorescent radiative rate.However,molecular engineering often exhibits similar regulation trends for the two processes.Here,we propose that the quantum interference caused by aggregation can be utilized to control the phosphorescent and non-radiative decay channels.We systematically analyze various constructive and destructive transition pathways in aggregates with different molecular packing types and establish clear relationships between the luminescence characters and the signs of the singlet and triplet excitonic couplings.It is shown that the decay channels can be flexibly switched on or off by regulating the packing type and excitonic couplings.Most importantly,an enhanced phosphorescent decay and a completely suppressed non-radiative decay can be simultaneously realized in the aggregate packed with inversion symmetry.This work lays the theoretical foundation for future experimental realization of quantum interference effects in phosphorescence.