Fröhlich interaction dominated by a single phonon mode in CsPbBr3.

The excellent optoelectronic performance of lead halide perovskites has generated great interest in their fundamental properties. The polar nature of the perovskite lattice means that electron-lattice coupling is governed by the Fröhlich interaction. Still, considerable ambiguity exists regarding the phonon modes that participate in this crucial mechanism. Here, we use multiphonon Raman scattering and THz time-domain spectroscopy to investigate Fröhlich coupling in CsPbBr3. We identify a longitudinal optical phonon mode that dominates the interaction, and surmise that this mode effectively defines exciton-phonon scattering in CsPbBr3, and possibly similar materials. It is additionally revealed that the observed strength of the Fröhlich interaction is significantly higher than the expected intrinsic value for CsPbBr3, and is likely enhanced by carrier localization in the colloidal perovskite nanocrystals. Our experiments also unearthed a dipole-related dielectric relaxation mechanism which may impact transport properties.

Non-Lorentzian Local Density of States in Coupled Photonic Crystal Cavities Probed by Near- and Far-Field Emission.

Recent theories proposed a deep revision of the well-known expression for the Purcell factor, with counterintuitive effects, such as complex modal volumes and non-Lorentzian local density of states. We experimentally demonstrate these predictions in tailored coupled cavities on photonic crystal slabs with relatively low optical losses. Near-field hyperspectral imaging of quantum dot photoluminescence is proved to be a direct tool for measuring the line shape of the local density of states. The experimental results clearly evidence non-Lorentzian character, in perfect agreement with numerical and theoretical predictions. Spatial maps with deep subwavelength resolution of the real and imaginary parts of the complex mode volumes are presented. The generality of these results is confirmed by an additional set of far-field and time-resolved experiments in cavities with larger modal volume and higher quality factors.

Strong Carrier-Phonon Coupling in Lead Halide Perovskite Nanocrystals.

We highlight the importance of carrier-phonon coupling in inorganic lead halide perovskite nanocrystals. The low-temperature photoluminescence (PL) spectrum of CsPbBr3 has been investigated under a nonresonant and a nonstandard, quasi-resonant excitation scheme, and phonon replicas of the main PL band have been identified as due to the Fröhlich interaction. The energy of longitudinal optical (LO) phonons has been determined from the separation of the zero phonon band and phonon replicas. We reason that the observed LO phonon coupling can only be related to an orthorhombically distorted crystal structure of the perovskite nanocrystals. Additionally, the strength of carrier-phonon coupling has been characterized using the ratio between the intensities of the first phonon replica and the zero-phonon band. PL emission from localized versus delocalized carriers has been identified as the source of the observed discrepancies between the LO phonon energy and phonon coupling strength under quasi-resonant and nonresonant excitation conditions, respectively.

Controlling mode degeneracy in a photonic crystal nanocavity with infiltrated liquid crystal.

We demonstrate the control of the mode degeneracy when a liquid crystal (LC) is infiltrated into an InGaAsP membrane photonic crystal nanocavity with embedded InAs quantum dots. Mode splitting exists in the anisotropic nematic LC state, and not in the unfilled or isotropic LC state. The degeneracy lifting of the quadrupole mode is attributed to the different interactions of the two orthogonal basis modes of the degenerate mode with the two components of the refractive index of the LC. The interpretation is supported by the quantitative agreement between the experimental results and the three-dimensional finite-difference time-domain computations.