Raman and fluorescence contributions to the resonant inelastic soft x-ray scattering on LaAlO 3 / SrTiO 3 heterostructures

We present a detailed study of the Ti $3d$ carriers at the interface of ${\mathrm{LaAlO}}_{3}/{\mathrm{SrTiO}}_{3}$ heterostructures by high-resolution resonant inelastic soft x-ray scattering (RIXS), with special focus on the roles of overlayer thickness and oxygen vacancies. Our measurements show the existence of interfacial Ti $3d$ electrons already below the critical thickness for conductivity. The (total) interface charge carrier density increases up to a ${\mathrm{LaAlO}}_{3}$ overlayer thickness of 6 unit cells before it levels out. Furthermore, we observe strong Ti $3d$ charge carrier doping by oxygen vacancies. The RIXS data combined with photoelectron spectroscopy and transport measurements indicate the simultaneous presence of localized and itinerant charge carriers. At variance with previous interpretations, we show that in our excitation energy dependent RIXS measurements the amounts of localized and itinerant Ti $3d$ electrons in the ground state do not scale with the intensities of the Raman and fluorescence peaks, respectively. Rather, we attribute the observation of either Raman components or fluorescence signal to the specific nature of the intermediate state reached in the RIXS excitation process.