(Invited) Interlayer Excitons in Two-Dimensional Perovskite/Monolayer Transition Metal Dichalcogenide Heterostructures

Abstract

The emergence of two-dimensional (2D) materials has intrigued a great deal of research on novel physical phenomena and various functional applications due to their particular crystal structures and reduced dimensionality. Unlike 3D materials, bulks of 2D materials can be easily thinned to atomic thickness by mechanical exfoliation and atomically thin 2D materials can be arbitrarily stacked to form vertical van der Waals (vdW) heterostructures, which could inherit the unique characteristics of the constituent layers and even exhibit new properties not possessed by them. Particularly, when type-Ⅱ vdW heterostructures are excited, the positive and the negative charges would reside in the different layers after the charge transfer but be limited within a short distance due to the strong quantum confinement effect of 2D materials, leading to strong Coulomb interaction and the formation of interlayer excitons (IXs). IXs are generally equipped with orientated dipole moment and long lifetime, making them ideal media for the future interconnects between optical transmission and electronic computation. Currently, studies on IXs are mainly focused on the vdW heterostructures formed by monolayers of transition-metal dichalcogenides (TMDs). Here, I will first talk about vdW heterostructures formed by 2D perovskites and TMDs for studying IXs. Stacking different kinds of 2D perovskites and TMDs, formation of IXs is confirmed by excitation-power-, temperature-, electric-field-dependent and time-resolved photoluminescence (PL) studies. Notably, robust IX emission can be observed regardless of the stacking sequence and geometric alignment of the constituent layers, showing great advantages over the TMD/TMD vdW heterostructures, which require special twist-angle and thermal annealing. Then, I would like to give a brief introduction on widely tuning the IX emission energy by changing the layer number of the 2D perovskite or the TMD, which shed light on the application of 2D perovskite/TMD vdW heterostructures in broad-spectrum optoelectronics. Furthermore, I would like to next talk about how the selection of organic chains in 2D perovskites influences the properties of the IXs. By using chiral 2D perovskites, the IX emission shows substantial circular polarization and the polarization direction is only related to the chirality of the molecules regardless of the excitation scheme or any other external field, which could open up new passages for controlling valley- or spin-polarization of IXs. By introducing molecules with different dielectric constants, the dielectric screening strength in the vdW heterostructure is changed and hence the binding energy of the IXs is also modified, which offers great opportunities for exploiting tunable excitonic devices and studying exciton condensation. Finally, I will also introduce IX as a non-destructive tool for probing the local phase transition at the surface of the 2D perovskite (BA)2PbI4 flakes. By spatially PL mapping of the (BA)2PbI4/WSe2 heterostructure, two different IX species can be observed to distinguish the low-temperature and the high-temperature phase respectively.