Identification of surface and volume hot-carrier thermalization mechanisms in ultrathin GaAs layers

Hot-carrier solar cells offer the opportunity to harvest more energy than the limit set by the Shockley-Queisser model by reducing the losses due to the thermalization of photo-generated carriers. Previous reports have shown lower thermalization rates in thinner absorbers, but the origin of this phenomenon is not precisely understood. In this work, we investigate a series of ultrathin GaAs absorber layers sandwiched between AlGaAs barriers and transferred on host substrates with a gold back mirror. We perform power-dependent photoluminescence characterizations at different laser wavelengths from which we determine the carrier temperature in four absorber thicknesses between 20 and 200nm. We observe a linear relationship between the absorbed power and the carrier temperature increase. By relating the absorbed and thermalized power, we extract a thermalization coefficient for all samples. It shows an affine dependence with the thickness, leading to the identification of distinct volume and surface contributions to thermalization. We confirm that volume thermalization is linked to LO phonon decay. We discuss the origin of the interface-related thermalization, showing that the effect of LO phonon transport is negligible. Overall, this work sheds new light on thermalization processes in ultrathin semiconductor layers and introduces a method to compare the performance of hot-carrier absorbers.