-Angle-resolved photoemission spectroscopy (ARPES) is a powerful technique for the study of electronic structure, but it lacks a direct ability to study buried interfaces between two materials. We address this limitation by combining ARPES with soft x-ray standing-wave (SW) excitation (SWARPES), in which the SW profile is scanned through the depth of the sample. We have studied the buried interface in a prototypical magnetic tunnel junction La 0.7 Sr 0.3 MnO 3 /SrTiO 3 . Depth-and momentum-resolved maps of Mn 3d e g and t 2g states from the central, bulk-like and interface-like regions of La 0.7 Sr 0.3 MnO 3 exhibit distinctly different behavior consistent with a change in the Mn bonding at the interface. We compare the experimental results to state-of-the-art density-functional and one-step photoemission theory, with encouraging agreement that suggests wide future applications of this technique.
The interfaces between two condensed phases often exhibit emergent physical properties that can lead to new physics and novel device applications and are the subject of intense study in many disciplines. We here apply experimental and theoretical techniques to the characterization of one such interesting interface system: the two-dimensional electron gas (2DEG) formed in multilayers consisting of SrTiO 3 (STO) and GdTiO 3 (GTO). This system has been the subject of multiple studies recently and shown to exhibit very high carrier charge densities and ferromagnetic effects, among other intriguing properties. We have studied a 2DEG-forming multilayer of the form [6 unit cells (u.c.) STO/3 u.c. of GTO] 20 using a unique array of photoemission techniques including soft and hard x-ray excitation, soft x-ray angle-resolved photoemission, core-level spectroscopy, resonant excitation, and standing-wave effects, as well as theoretical calculations of the electronic structure at several levels and of the actual photoemission process. Standing-wave measurements below and above a strong resonance have been exploited as a powerful method for studying the 2DEG depth distribution. We have thus characterized the spatial and momentum properties of this 2DEG in detail, determining via depth-distribution measurements that it is spread throughout the 6 u.c. layer of STO and measuring the momentum dispersion of its states. The experimental results are supported in several ways by theory, leading to a much more complete picture of the nature of this 2DEG and suggesting that oxygen vacancies are not the origin of it. Similar multitechnique photoemission studies of such states at buried interfaces, combined with comparable theory, will be a very fruitful future approach for exploring and modifying the fascinating world of buried-interface physics and chemistry.
The experimental determination of valence band offsets (VBOs) at interfaces in complex-oxide heterostructures using conventional soft x-ray photoelectron spectroscopy (SXPS, h 1500 eV) and reference core-level binding energies can present challenges because of surface charging when photoelectrons are emitted and insufficient probing depth to clearly resolve the interfaces. In this paper, we compare VBOs measured with SXPS and its multi-keV hard x-ray analogue (HXPS, h > 2000 eV). We demonstrate that the use of HXPS allows one to minimize charging effects and to probe more deeply buried interfaces in heterostructures such as SrTiO 3 /LaNiO 3 and SrTiO 3 / GdTiO 3. The VBO values obtained by HXPS for these interfaces are furthermore found to be close to those determined by first-principles calculations. V
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