By measuring electron spin resonance (ESR) spectra at the X-band frequency and absorption spectra from the visible to ultraviolet region at room temperature, it was confirmed that perovskite single crystal LaAlO3 contains Cr and Fe as impurities. When LaAlO3 is exposed to photons with energies higher than 4.5 eV, the intensities of ESR signals due to Cr3+ and Fe3+ decrease, which indicates that electrons released by the photon irradiation are captured by Cr3+ and Fe3+. Concurrently with this, a broad optical absorption band at about 3.0 eV and two new broad and weak ESR signals appear. The former is attributable to a combination of a hole and a La3+ (or Al3+) vacancy, and the two weak ESR signals are assigned to the O− center and F+ center.

Photoluminescence (PL) spectra induced in LaAlO3 by ultraviolet (UV) photons were measured for two types of samples, i.e., single-crystal plates and thin films. The films, which were amorphous when deposited, became polycrystalline after being annealed at 800 °C or higher. When the excitation photon energy exceeded the band-gap energy of LaAlO3, three PL peaks appeared at approximately 1.60 eV in the single crystals and polycrystalline films deposited and annealed on a Si single-crystal substrate. When the films were deposited and annealed on a CaF2 single-crystal substrate, the in-plane lattice parameters became smaller and the energies of the three PL peaks shifted to higher values. This indicates that the three PL peaks are susceptible to a crystal field. Furthermore, the intensities of the three PL peaks did not depend on the measurement temperature. Taking these results together with their spectral shapes into consideration, the three PL peaks are due to the R-line luminescence resulting from Cr3+ impurities in LaAlO3. The detection of Cr3+ ions by inductively coupled plasma optical emission spectrometry failed, indicating that the Cr3+ content of the present samples is below 1 ppm. The fact that the PL peaks appeared in both the single-crystal plates and thin films obtained from different raw chemicals with different processes indicates that there is a strong possibility that the Cr3+ ions are present in Al ore. Another PL peak appearing at 2.8 eV in the single crystals was assumed to originate from oxygen vacancies.

Impurities present in LaAlO 3 , were identified by analyzing electron spin resonance spectra and optical absorption spectra. Especially, the effects of ultraviolet photon irradiation and thermal annealing on these spectra were studied in detail. The experimental results confirm that LaAlO 3 contains Cr and Fe as impurities. They also indicate that electrons and holes are released by the irradiation of UV photons with energies higher than 4.5 eV or by the annealing in an oxidizing atmosphere at temperatures above 500 o C. The released electrons are captured by trivalent impurity ions (Fe 3+ or Cr 3+ ), while the holes are captured by trivalent vacancies of La 3+ or Al 3+ . It is assumed that the opposite reaction is induced by the irradiation of visible light or by the annealing in a reducing atmosphere at temperatures above 500 o C.