Hybrid organic-inorganic lead halide perovskite materials show great promise in a number of optoelectronic applications, including solar cells, light emitting diodes, and photodetectors. Understanding their intrinsic material properties is critical to enhancing device performance and enabling innovative material and device designs. Here, we study lattice dynamics using far-infrared (FIR) reflectance and photogenerated carrier dynamics using surface photovoltage (SPV) measurements on high-quality methylammonium lead bromide (MAPbBr₃) single crystals. FIR reflectance shows three coherent infrared-active phonon modes between 40 and 200 cm⁻¹ that result in reststrahlen bands with much higher peak reflectance than has been previously reported. The phonon mode strength and damping are comparable to classical oxide perovskite single crystals. However, the effects of defects on photogenerated carrier recombination are still evident in SPV measurements. By performing SPV over different spectral ranges, we are able to separate the effects of surface and bulk defects on the recombination dynamics of photogenerated charge carriers. We further apply SPV measurements to obtain the minority carrier (electron) diffusion length for the MAPbBr₃ crystal. This study demonstrates that both FIR reflectance and SPV measurements provide useful information on the electromagnetic response properties of halide perovskite single crystals.

Dilute donor organic solar cells (OSCs) are a promising technology to circumvent the trade‐off between open‐circuit voltage (V_oc) and short‐circuit current density (J_sc). The origin of hole transport in OSCs with donor concentrations below the percolation threshold is diversely discussed in the community. Herein, both hole back transfer and long‐range hopping (tunneling) are analyzed as possible mechanisms of photocurrent in small molecule dilute donor OSCs using kinetic Monte Carlo (kMC) simulations. In contrast to previous kMC studies, the driving force for exciton dissociation is accounted for. As a study system, nitrogen‐bridged terthiophene (NBTT) molecules in a [6,6]‐phenyl‐C70‐butyric acid methyl ester (PC₇₁BM) matrix are investigated. The simulations show that hole back transfer from the small molecule donor to the fullerene matrix explains the measured concentration dependences of the photocurrents as well as the J_sc dependence on the light intensity for donor concentrations below 5 wt%. For 5 wt%, distances between NBTT molecules decrease to reasonable ranges that long‐range hopping or tunneling cannot be discounted. Compared with polymer donors, larger hole localization is observed. The results emphasize that the barrier for hole back transfer is not only due to the highest occupied molecular orbital (HOMO) offset, but also by hole localization.