Mark D. Scafetta

Band structure and optical transitions in LaFeO3: theory and experiment

The optical absorption properties of LaFeO(3) (LFO) have been calculated using density functional theory and experimentally measured from several high quality epitaxial films using variable angle spectroscopic ellipsometry. We have analyzed the calculated absorption spectrum using different Tauc models and find the model based on a direct-forbidden transition gives the best agreement with the ab initio band gap energies and band dispersions. We have applied this model to the experimental data and determine the band gap of epitaxial LFO to be ∼2.34 eV, with a slight dependence on strain state. This approach has also been used to analyze the higher indirect transition at ∼3.4 eV. Temperature dependent ellipsometry measurements further confirm our theoretical analysis of the nature of the transitions. This works helps to provide a general approach for accurate determination of band gaps and transition energies in complex oxide materials.

Electronic phase diagram of epitaxial La1−xSrxFeO3 films

The electronic phase diagram of epitaxial La1−xSrxFeO3 films is presented. The films were grown on SrTiO3 using molecular beam epitaxy with post-growth annealing to minimize oxygen vacancies. Insulating behavior is observed from x = 0–0.9, with metallic conduction only present for x = 1.0. While the La-rich compounds exhibit polaron conduction over all temperatures measured, the Sr-rich films exhibit an electronic phase transition within the compositional window of x = 0.49–0.9 as revealed by temperature-dependent resistivity measurements. The transition temperatures are found to decrease with increasing Sr content. The constructed phase diagram is discussed in the context of other 3d eg perovskite systems including manganites and cobaltites.

Optical absorption in epitaxial La1−xSrxFeO3 thin films

We report the dependence of optical absorption on Sr concentration in La1−xSrxFeO3 (LSFO) (x≤0.4) perovskite thin films. Strained epitaxial films were deposited on SrTiO3 substrates using oxide molecular beam epitaxy. We find systematic changes in the optical absorption spectra with increasing x including a red-shift of transition energies and the increasing presence of a lower energy transition within the fundamental gap of pure LaFeO3. These results serve as a demonstration of the complex manner in which absorption spectra can be altered in complex oxides via heterovalent A-site substitution.

Ultrafast transient reflectance of epitaxial semiconducting perovskite thin films

Ultrafast pump-probe transient reflectance (TR) spectroscopy was used to study carrier dynamics in an epitaxial perovskite oxide thin film of LaFeO3 (LFO) with a thickness of 40 unit cells (16 nm) grown by molecular beam epitaxy on (LaAlO3)0.3(Sr2AlTaO6)0.7 (LSAT). TR spectroscopy shows two negative transients in reflectance with local maxima at ∼2.5 eV and ∼3.5 eV which correspond to two optical transitions in LFO as determined by ellipsometry. The kinetics at these transients were best fit with an exponential decay model with fast (5–40 ps), medium (∼200 ps), and slow (∼ 3 ns) components that we attribute mainly to recombination of photoexcited carriers. Moreover, these reflectance transients did not completely decay within the observable time window, indicating that ∼10% of photoexcited carriers exist for at least 3 ns. This work illustrates that TR spectroscopy can be performed on thin (<20 nm) epitaxial oxide films to provide a quantitative understanding of recombination lifetimes, which are importan...

Optical absorption in epitaxial thin films

We report the dependence of optical absorption on Sr concentration in La1−xSrxFeO3 (LSFO) (x≤0.4) perovskite thin films. Strained epitaxial films were deposited on SrTiO3 substrates using oxide molecular beam epitaxy. We find systematic changes in the optical absorption spectra with increasing x including a red-shift of transition energies and the increasing presence of a lower energy transition within the fundamental gap of pure LaFeO3. These results serve as a demonstration of the complex manner in which absorption spectra can be altered in complex oxides via heterovalent A-site substitution.

Optical absorption in epitaxial La{sub 1-x}Sr{sub x}FeO{sub 3} thin films

We report the dependence of optical absorption on Sr concentration in La1−xSrxFeO3 (LSFO) (x≤0.4) perovskite thin films. Strained epitaxial films were deposited on SrTiO3 substrates using oxide molecular beam epitaxy. We find systematic changes in the optical absorption spectra with increasing x including a red-shift of transition energies and the increasing presence of a lower energy transition within the fundamental gap of pure LaFeO3. These results serve as a demonstration of the complex manner in which absorption spectra can be altered in complex oxides via heterovalent A-site substitution.