RESUMEN
The systematical analysis for varieties of defects with different depths and lattice relaxation strengths in metal halide perovskites (MHPs) is a challenging task. Here, we study the energy shifts of the full-configuration defects due to the polaron effect based on the all-coupling variational method in MHPs, where these polaron states are formed stemming from different defect species coupling with the longitudinal optical phonon modes via Fro¨hlich mechanism. We find that the polaron effect results in defect levels varying from tens to several hundreds of meV, which are very close to the correction of defect levels due to the defect-polaron effect, especially for these defects migration proved in the recent experiments in MHPs. These results provide the significant enlightenment not only for analyzing the radiation and non-radiation processes of carriers mediated by defects, but also for optimizing defect effect in the photovoltaic and photoelectric devices based on MHPs materials.
RESUMEN
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 I 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 II 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.
RESUMEN
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.
RESUMEN
Quantum defects are essential to understand the non-radiative recombination processes in metal halide perovskites-based photovoltaic devices, in which Huang-Rhys factor, reflecting the coupling strength between the charge carrier and optical phonons, plays a key role in determining the non-radiative recombination via multiphonon processes. Herein, we theoretically present multiphonon Raman scattering intermediated by defects arising from the charge carrier of defect coupled with the longitudinal optical (LO) phonon in the deformation potential and Fröhlich mechanisms, respectively. We find that the Raman scattering shows multiple LO phonon overtones at equal interval LO phonons, where Huang-Rhys factor could be evaluated by the order of the strongest overtone. Meanwhile, we give the combinational multiphonon scattering between two mechanisms. Different types of the combinational modes with the weak scattering intensities provide a possible explanation for the long non-radiative charges-carrier lifetimes in metal halide perovskites.
RESUMEN
Quantum defects have been shown to play an essential role in nonradiative recombination in metal halide perovskites (MHPs). Nonetheless, the processes of charge transfer assisted by defects are still ambiguous. Herein, we theoretically study the nonradiative multiphonon processes among different types of quantum defects in MHPs using Markvart's model for the induced mechanisms of electron-electron and electron-phonon interactions. We find that the charge carrier can transfer between the neighboring levels of the same type of shallow defects by multiphonon processes, but it will be distinctly suppressed with an increase in the defect depth. For the nonradiation multiphonon transitions between donor- and acceptor-like defects, the processes are very fast and not sensitive to the defect depth, which provides a possible explanation for the phenomenon of blinking of photoluminescence spectra. We also discuss the temperature dependence of these multiphonon processes and find that their variational trends depend on the comparison of the Huang-Rhys factor with the emitted phonon number. These theoretical results not only fill some of the gaps in defect-assisted nonradiative processes in the perovskite materials but also provide deeper physical insights into producing higher-performance perovskite-based devices.
RESUMEN
We propose a theoretical model for studying the effective velocities of polaron spin states in monolayer transition metal dichalcogenides (TMDS) on the substrate. It is found that the effective velocity of polaron shows the splitting with different magnitudes due to the Rashba spin-orbit coupling, which results in the reversed distribution of the effective velocities of polaron spin states. Moreover, the reversed points depend on the truncated wave-vector of optical phonon and can be modulated by the polarity of substrate and the internal distance between monolayer TMDS and substrate. These theoretical results enlighten some simple ways to distinguish and modulate the polaron spin states in two-dimensional heterostructures.