In condensed matter physics the quasi two-dimensional electron gas at the interface of two different insulators, polar LaAlO3 on nonpolar SrTiO3 (LaAlO3/SrTiO3) is a spectacular and surprising observation. This phenomenon is LaAlO3 film thickness dependent and may be explained by the polarization catastrophe model, in which a charge transfer of 0.5e(-) from the LaAlO3 film into the LaAlO3/SrTiO3 interface is expected. Here we show that in conducting samples (≥ 4 unit cells of LaAlO3) there is indeed a ~0.5e(-) transfer from LaAlO3 into the LaAlO3/SrTiO3 interface by studying the optical conductivity in a broad energy range (0.5-35 eV). Surprisingly, in insulating samples (≤ 3 unit cells of LaAlO3) a redistribution of charges within the polar LaAlO3 sublayers (from AlO2 to LaO) as large as ~0.5e(-) is observed, with no charge transfer into the interface. Hence, our results reveal the different mechanisms for the polarization catastrophe compensation in insulating and conducting LaAlO3/SrTiO3 interfaces.
Plasmonics has attracted tremendous interests for its ability to confine light into subwavelength dimensions, creating novel devices with unprecedented functionalities. New plasmonic materials are actively being searched, especially those with tunable plasmons and low loss in the visible–ultraviolet range. Such plasmons commonly occur in metals, but many metals have high plasmonic loss in the optical range, a main issue in current plasmonic research. Here, we discover an anomalous form of tunable correlated plasmons in a Mott-like insulating oxide from the Sr1−xNb1−yO3+δ family. These correlated plasmons have multiple plasmon frequencies and low loss in the visible–ultraviolet range. Supported by theoretical calculations, these plasmons arise from the nanometre-spaced confinement of extra oxygen planes that enhances the unscreened Coulomb interactions among charges. The correlated plasmons are tunable: they diminish as extra oxygen plane density or film thickness decreases. Our results open a path for plasmonics research in previously untapped insulating and strongly-correlated materials.
Semiconductor compounds are widely used for photocatalytic hydrogen production applications, where photogenerated electron–hole pairs are exploited to induce catalysis. Recently, powders of a metallic oxide (Sr1−xNbO3, 0.03
Electron-electron (e-e) and electron-hole (e-h) interactions are often associated with many exotic phenomena in correlated electron systems. Here, we report an observation of anomalous excitons at 3.75 , 4.67 and 6.11 eV at 4.2 K in bulk -SrTiO3. Fully supported by ab initio GW Bethe-Salpeter equation calculations, these excitons are due to surprisingly strong e-h and e-e interactions with different characters: 4.67 and 6.11 eV are resonant excitons and 3.75 eV is a bound Wannier-like exciton with an unexpectedly higher level of delocalization. Measurements and calculations on SrTi1−xNbxO3 for 0.0001≤x ≤0.005 further show that energy and spectral-weight of the excitonic peaks vary as a function of electron doping (x ) and temperature, which are attributed to screening effects. Our results show the importance of e-h and e-e interactions yielding to anomalous excitons and thus bring out a new fundamental perspective in SrTiO3.
Interfaces of two dissimilar complex oxides exhibit exotic physical properties that are absent in their parent compounds. Of particular interest is insulating LaAlO3 films on an insulating SrTiO3 substrate, where transport measurements have shown a metal-insulator transition as a function of LaAlO3 thickness. Their origin has become the subject of intense research, yet a unifying consensus remains elusive. Here, we report evidence for the electronic reconstruction in both insulating and conducting LaAlO3/SrTiO3 heterointerfaces revealed by O K-edge X-ray absorption spectroscopy. For the insulating samples, the O K-edge XAS spectrum exhibits features characteristic of electronically active point defects identified as noninteger valence states of Ti. For conducting samples, a new shape-resonance at ∼540.5 eV, characteristic of molecular-like oxygen (empty O-2p band), is observed. This implies that the concentration of electronic defects has increased in proportion with LaAlO3 thickness. For larger defect concentrations, the electronic defect states are no longer localized at the Ti orbitals and exhibit pronounced O 2p-O 2p character. Our results demonstrate that, above a critical thickness, the delocalization of O 2p electronic states can be linked to the presence of oxygen vacancies and is responsible for the enhancement of conductivity at the oxide heterointerfaces.
Patterning of the two-dimensional electron gas formed at the interface of two band insulators such as LaAlO3/SrTiO3 is one of the key challenges in oxide electronics. The use of energetic ion beam exposure for engineering the interface conductivity has been investigated. We found that this method can be utilized to manipulate the conductivity at the LaAlO3/SrTiO3 interface by carrier localization, arising from the defects created by the ion beam exposure, eventually producing an insulating ground state. This process of ion-beam-induced defect creation results in structural changes in SrTiO3 as revealed by the appearance of first-order polar TO2 and TO4 vibrational modes which are associated with Ti-O bonds in the Raman spectra of the irradiated samples. Furthermore, significant observation drawn from the magnetotransport measurements is that the irradiated (unirradiated) samples showed a negative (positive) magnetoresistance along with simultaneous emergence of first-order (only second order) Raman modes. In spectroscopic ellipsometry measurements, the optical conductivity features of the irradiated interface are broadened because of the localization effects, along with a decrease of spectral weight from 4.2 to 5.4 eV. These experiments allow us to conclude that the interface ground state (metallic/insulating) at the LaAlO3/SrTiO3 can be controlled by tailoring the defect structure of the SrTiO3 with ion beam exposure. A resist-free, single-step direct patterning of a conducting LaAlO3/SrTiO3 interface has been demonstrated. Patterns with a spatial resolution of 5 μm have been fabricated using a stencil mask, while nanometer scale patterns may be possible with direct focused ion beam writing.
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