Evidence for a large phononic band gap leading to slow hot carrier thermalisation

Abstract

It has been proposed that the rate of hot carrier thermalisation can be slowed down if there is a sufficiently large gap in the phonon dispersion for a bulk material. This phenomenon is critical for the development of high efficiency hot carrier solar cells to minimise energy loss to thermalisation. A gap where the minimum of the optical branches is at least twice that of the maximum of the acoustic branches can prevent the primary pathway where optical phonons loses energy, the Klemens' decay mechanism. The large gap in the phonon dispersion eliminates the Klemens' decay pathway due to energy and momentum conservation laws. This enables the electron population to remain hot by allowing sufficient time for optical phonons to re-scatter its energy to electrons. Binary compounds with a large mass difference between the two constituent atoms and high level of crystal symmetry such as zirconium nitride and hafnium nitride (HfN) have such a gap in their phonon dispersion. HfN thin films have been sputtered on silicon and quartz substrates. Characterisation of hot electron lifetimes in HfN films have been performed using ultrafast transient absorption spectroscopy. Preliminary analysis of transient absorption data, both spectra and time evolution has indicated high carrier temperatures with a nanosecond long decay time. It is postulated the long hot carrier lifetime is due to the large phononic gap.