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Register a new userARPES Studies of Two-Dimensional Electron Gases at Transition Metal Oxide Surfaces
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Added by
Siobhan McKeown Walker
Publication date
2016
fields
Physics
and research's language is
English
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High mobility two-dimensional electron gases (2DEGs) underpin todays silicon based devices and are of fundamental importance for the emerging field of oxide electronics. Such 2DEGs are usually created by engineering band offsets and charge transfer at heterointerfaces. However, in 2011 it was shown that highly itinerant 2DEGs can also be induced at bare surfaces of different transition metal oxides where they are far more accessible to high resolution angle resolved photoemission (ARPES) experiments. Here we review work from this nascent field which has led to a systematic understanding of the subband structure arising from quantum confinement of highly anisotropic transition metal d-states along different crystallographic directions. We further discuss the role of different surface preparations and the origin of surface 2DEGs, the understanding of which has permitted control over 2DEG carrier densities. Finally, we discuss signatures of strong many-body interactions and how spectroscopic data from surface 2DEGs may be related to the transport properties of interface 2DEGs in the same host materials.
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We report on the transport characterization in dark and under light irradiation of three different interfaces: LaAlO3/SrTiO3, LaGaO3/SrTiO3, and the novel NdGaO3/SrTiO3 heterostructure. All of them share a perovskite structure, an insulating nature of the single building blocks, a polar/non- polar character and a critical thickness of four unit cells for the onset of conductivity. The interface structure and charge confinement in NdGaO3/SrTiO3 are probed by atomic-scale- resolved electron energy loss spectroscopy showing that, similarly to LaAlO3/SrTiO3, extra electronic charge confined in a sheet of about 1.5 nm in thickness is present at the NdGaO3/SrTiO3 interface. Electric transport measurements performed in dark and under radiation show remarkable similarities and provide evidence that the persistent perturbation induced by light is an intrinsic peculiar property of the three investigated oxide-based polar/non-polar interfaces. Our work sets a framework for understanding the previous contrasting results found in literature about photoconductivity in LaAlO3/SrTiO3 and highlights the connection between the origin of persistent photoconductivity and the origin of conductivity itself. An improved understanding of the photo- induced metastable electron-hole pairs might allow to shed a direct light on the complex physics of this system and on the recently proposed perspectives of oxide interfaces for solar energy conversion.
The discovery of two-dimensional electron gases (2DEGs) at the interface between two insulating complex oxides, such as LaAlO3 (LAO) or gamma-Al2O3 (GAO) epitaxially grown on SrTiO3 (STO) 1,2, provides an opportunity for developing all-oxide electronic devices3,4. These 2DEGs at complex oxide interfaces involve many-body interactions and give rise to a rich set of phenomena5, for example, superconductivity6, magnetism7,8, tunable metal-insulator transitions9, and phase separation10. However, large enhancement of the interfacial electron mobility remains a major and long-standing challenge for fundamental as well as applied research of complex oxides11-15. Here, we inserted a single unit cell insulating layer of polar La1-xSrxMnO3 (x=0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 created at room temperature. We find that the electron mobility of the interfacial 2DEG is enhanced by more than two orders of magnitude. Our in-situ and resonant x-ray spectroscopic in addition to transmission electron microscopy results indicate that the manganite layer undergoes unambiguous electronic reconstruction and leads to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits clear Shubnikov-de Haas oscillations and the initial manifestation of the quantum Hall effect, demonstrating an unprecedented high-mobility and low electron density oxide 2DEG system. These findings open new avenues for oxide electronics.
We have performed systematic tight-binding (TB) analyses of the angle-resolved photoemission spectroscopy (ARPES) spectra of transition-metal (TM) oxides A$M$O$_3$ ($M=$ Ti, V, Mn, and Fe) with the perovskite-type structure and compared the obtained parameters with those obtained from configuration-interaction (CI) cluster-model analyses of photoemission spectra. The values of $epsilon_d-epsilon_p$ from ARPES are found to be similar to the charge-transfer energy $Delta$ from O $2p$ orbitals to empty TM 3d orbitals and much larger than $Delta-U/2$ ($U$: on-site Coulomb energy) expected for Mott-Hubbard-type compounds including SrVO$_3$. $epsilon_d-epsilon_p$ values from {it ab initio} band-structure calculations show similar behaviors to those from ARPES. The values of the $p-d$ transfer integrals to describe the global electronic structure are found to be similar in all the estimates, whereas additional narrowing beyond the TB description occurs in the ARPES spectra of the $d$ band.
Electron gases at the surfaces of (001), (110), and (111) oriented SrTiO3 (STO) have been created using Ar+-irradiation with fully metallic behavior and low-temperature-mobility as large as 5500 cm2V-1s-1, 1300 cm2V-1s-1 and 8600 cm2V-1s-1 for (001)-, (110)-, and (111)-surfaces, respectively. The in-plane anisotropic magnetoresistance (AMR) have been studied for the samples with the current along different crystal axis directions to subtract the Lorentz Force effect. The AMR shows features which coincide with the fixed orientations to the crystalline axes, with 4-fold, 2-fold and nearly-6-fold symmetries for (001)-, (110) and (111)-surfaces, respectively, independent of the current directions. These features are possibly caused by the polarization of spin orbit texture of the 2D Fermi surfaces. In addition, a 6-fold to 2-fold symmetry breaking for (111)-surfaces is observed. Our results demonstrate the effect of symmetry of two-dimensional electronic structure on the transport behaviors for the electron gases at STO surfaces.
The pressure-induced insulator to metal transition (IMT) of layered magnetic nickel phosphorous tri-sulfide NiPS3 was studied in-situ under quasi-uniaxial conditions by means of electrical resistance (R) and X-ray diffraction (XRD) measurements. This sluggish transition is shown to occur at 35 GPa. Transport measurements show no evidence of superconductivity to the lowest measured temperature (~ 2 K). The structure results presented here differ from earlier in-situ work that subjected the sample to a different pressure state, suggesting that in NiPS3 the phase stability fields are highly dependent on strain. It is suggested that careful control of the strain is essential when studying the electronic and magnetic properties of layered van der Waals solids.
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