The self-trapped state (STS) of the interlayer exciton (IX) has aroused enormous interest owing to its significant impact on the fundamental properties of the van der Waals heterostructures (vdWHs). Nevertheless, the microscopic mechanisms of STS are still controversial. Herein, we study the corrections of the binding energies of the IXs stemming from the exciton−interface optical phonon coupling in four kinds of vdWHs and find that these IXs are in the STS for the appropriate ratio of the electron and hole effective masses. We show that these self-trapped IXs could be classified into type  with the increasing binding energy in the tens of millielectronvolts range, which are very agreement with the red-shift of the IX spectra in experiments, and type  with the decreasing binding energy, which provides a possible explanation for the blue-shift and broad line width of the IX's spectra at low temperatures. Moreover, these two types of exciton states could be transformed into each other by adjusting the structural parameters of vdWHs. These results not only provide an in-depth understanding for the self-trapped mechanism but also shed light on the modulations of IXs in vdWHs.

No abstract

Metal halide perovskites quantum dots (MHPQDs) have aroused enormous interest in the photovoltaic and photoelectric disciplines because of their marvelous properties and size characteristics. However, one of the key problems of how to systematically analyze charge carriers trapped by defects is still a challenging task. Here, we study multiphonon processes of the charge carrier trapping by various defects in MHPQDs based on the well-known Huang–Rhys model, in which a method of a full-configuration defect, including different defect species with variable depth and lattice relaxation strength, is developed by introducing a localization parameter in the quantum defect model. With the help of this method, these fast trapping channels for charge carriers transferring from the quantum dot ground state to different defects are found. Furthermore, the dependence of the trapping time on the radius of quantum dot, the defect depth, and temperature is given. These results not only enrich the knowledge of charge carrier trapping processes by defects, but also bring light to the designs of MHPQDs-based photovoltaic and photoelectric devices.

The formation of Fr$\ddot{o}$hlich polaron in metal halide perovskites, arising from the charge carrier-longitudinal optical (LO) phonon coupling, has been proposed to explain their exceptional properties, but the effective identification of polaron in these materials is still a challenge task. Herein, we theoretically present the infrared optical absorption of Fr$\ddot{o}$hlich polaron based on Huang-Rhys model. We find that multiphonon overtones are appeared as the energy of incident photon matches the multiple LO phonons, wherein the average phonon numbers of a polaron can be directly evaluated by the order of the strongest overtone. These multiphonon structures sensitively depend on the scale of electronic distribution in the ground state and the dimensionality of the perovskite materials, which gives the enlightenment for the effective modulation of competing processes between the polaron formation and carrier cooling. Moreover, the order of the strongest overtone shifts to the higher ones with temperature, providing a potential proof of the carriers mobility affected by LO phonons scattering. The present model not only suggests a direct way to verify Fr$\ddot{o}$hlich polaron, but also enriches the understanding of the polaron properties in metal halide perovskites.

The self-trapped state (STS) of interlayer exciton (IX) has been aroused enormous interesting owing to their significant impact on the fundamental properties of the van der Waals heterostructures (vdWHs). Nevertheless, the microscopic mechanisms of STS are still controversial. Herein, we study the corrections of the binding energies of the IXs due to the exciton-interface optical phonon coupling in four kinds of vdWHs and find that these IXs are in the STS for the appropriate ratio of the electron and hole effective masses. We show that these STSs could be classified into the type I with the increasing binding energy in the tens of meV range, which are very agreement with the red-shift of the IXs spectra in experiments, and the type II with the decreasing binding energy, which provides a possible explanation for the blue-shift and broad linewidth of the IX's spectra in the low temperature. Moreover, these two types of self-trapped IXs could be transformed into each other by adjusting the structural parameters of vdWHs. These results not only provide an in-depth understanding for the self-trapped mechanism of IX, but also shed light on the modulations of IXs in vdWHs.