PbBr-based layered perovskite organic-inorganic superlattice having carbazole chromophore; Hole-mobility and quantum mechanical calculation

We have successfully evaluated hole mobility in a spin-coated film of a lead-bromide based layered perovskite having carbazole chromophore-linked ammonium molecules as organic layer by using FET measurement. The values of hole mobility, threshold voltage and on/off ratio at room temperature were evaluated to be 1.7 × 10^-6 cm² V^-1 s^-1 , 27 V and 28 V, respectively. However, the spin-coated films on Si substrates were not so uniform compared with those on fused quartz substrates. To improve the film uniformity, we examined the relationship between substrate temperature during spin-coating and film morphology in the layered perovskite spin-coated films. The mean roughness of the spin-coated films on Si substrates was dependent on the substrate temperature. At 353 K, the mean roughness was minimized and the carrier mobility was enhanced by one order of magnitude; the values of hole mobility and threshold voltage were estimated to be 3.4×10^-5 cm² V^-1 s^-1, and 22 V at room temperature in a preliminary FET evaluation, respectively. In addition, we determined a crystal structure of the layered perovskite by X-ray diffraction analysis. To gain a better understanding of the observed hole transports, we conducted quantum mechanical calculations using the obtained crystal structure information. The calculated band structure of the layered organic perovskite showed that the valence band is composed of the organic carbazole layer, which confirms that the measured hole mobility is mainly derived from the organic part of the layered perovskite. Band and hopping transport mechanisms were discussed by calculating the effective masses and transfer integrals for the 2D periodic system of the organic layer in isolation.