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Title: Direct Evidence of Exciton–Exciton Annihilation in Single-Crystalline Organic Metal Halide Nanotube Assemblies
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Award ID(s):
1709116 1664661
Publication Date:
Journal Name:
The Journal of Physical Chemistry Letters
Page Range or eLocation-ID:
2164 to 2169
Sponsoring Org:
National Science Foundation
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  1. Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS2), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS2 is still lacking. Here we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS2. We directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS2. We attribute this distinct feature in ReS2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.
  2. Aside from band gap reduction, little is understood about the effect of the tin-for-lead substitution on the fundamental optical and optoelectronic properties of metal halide perovskites (MHPs), especially when transitioning from 3D to lower dimensional structures. Herein, we take advantage of the spectroscopic isolation of excitons in 2D MHPs to study the intrinsic differences between lead and tin MHPs. The exciton's spectral fine structure indicates a larger polaron binding energy in tin MHPs. Additionally, the electroabsorption responses of the 2D MHPs demonstrates that tin MHPs have exciton binding energies 1.5–2× lower than that of their lead counterparts. Despite the lower binding energy, the excitons in tin MHPs are more Frenkel-like with small radii, small polarizabilities, and large dipole moments. These results are interpreted as consequences of small polaron formation and disorder-induced dipole moments. This work highlights the wide range of intrinsic differences between lead and tin MHPs as well as the complexity of excited states in these systems.