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Register a new userElectronic Localization in CaVO3 Films via Bandwidth Control
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Understanding and controlling the electronic structure of thin layers of quantum materials is a crucial first step towards designing heterostructures where new phases and phenomena, including the metal-insulator transition (MIT), emerge. Here, we demonstrate control of the MIT via tuning electronic bandwidth and local site environment through selection of the number of atomic layers deposited. We take CaVO3, a correlated metal in its bulk form that has only a single electron in its V4+ 3d manifold, as a representative example. We find that thick films and ultrathin films (6 unit cells, uc, and below) are metallic and insulating, respectively, while a 10 uc CaVO3 film exhibits a clear thermal MIT. Our combined X-ray absorption spectroscopy and resonant inelastic x-ray scattering (RIXS) study reveals that the thickness-induced MIT is triggered by electronic bandwidth reduction and local moment formation from V3+ ions, that are both a consequence of the thickness confinement. The thermal MIT in our 10 uc CaVO3 film exhibits similar changes in the RIXS response to that of the thickness-induced MIT in terms of reduction of bandwidth and V 3d - O 2p hybridization.
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The 4f-electron delocalization plays a key role in the low-temperature properties of rare-earth metals and intermetallics, including heavy fermions and mix-valent compounds, and is normally realized by the many-body Kondo coupling between 4f and conduction electrons. Due to the large onsite Coulomb repulsion of 4f electrons, the bandwidth-control Mott-type delocalization, commonly observed in d-electron systems, is difficult in 4f-electron systems and remains elusive in spectroscopic experiments. Here we demonstrate that the bandwidth-control orbital-selective delocalization of 4f electrons can be realized in epitaxial Ce films by thermal annealing, which results in a metastable surface phase with a reduced layer spacing. The resulting quasiparticle bands exhibit large dispersion with exclusive 4f character near E_F and extend reasonably far below the Fermi energy, which can be explained from the Mott physics. The experimental quasiparticle dispersion agrees surprisingly well with density-functional theory calculation and also exhibits unusual temperature dependence, which could be a direct consequence of the delicate interplay between the bandwidth-control Mott physics and the coexisting Kondo hybridization. Our work therefore opens up the opportunity to study the interaction between two well-known localization-delocalization mechanisms in correlation physics, i.e., Kondo vs Mott, which can be important for a fundamental understanding of 4f-electron systems.
We present parameter-free LDA+DMFT (local density approximation + dynamical mean field theory) results for the many-body spectra of cubic SrVO3 and orthorhombic CaVO3. Both systems are found to be strongly correlated metals, but not on the verge of a metal-insulator transition. In spite of the considerably smaller V-O-V bond angle in CaVO3 the LDA+DMFT spectra of the two systems for energies E<E_F are very similar, their quasiparticle parts being almost identical. The calculated spectrum for E>E_F shows more pronounced, albeit still small, differences. This is in contrast to earlier theoretical and experimental conclusions, but in good agreement with recent bulk-sensitive photoemission and x-ray absorption experiments.
The magnetic properties of perovskite CaVO3 single crystals have been studied by means of magnetoresistance r(T, H) and magnetization M(H) measurements in fields to 18T. At 2 K, the magnetoresistance is positive and a maximum value of Dr(18T)/r(0) = 16.5% is found for H//a. The magnetization exhibits a smooth increase at 2 K, reaching values of M(18T) = 0.03, 0.05, 0.17 mB/f.u. for H//a, H//b, and H//c, respectively. This anisotropy found in M(H) is consistent with that observed for Dr(H//a) > Dr(H//b) > Dr(H//c). These results can be interpreted in terms of the field-dependent scattering mechanism of CaVO3.
Nickelates are known for their metal to insulator transition (MIT) and an unusual magnetic ordering, occurring at T=T_Neel. Here, we investigate thin films of SmNiO_3 subjected to different levels of epitaxial strain. We find that the original bulk behavior (T_Neel<T_MI) is strongly affected by applying compressive strain to the films. For small compressive strains, a regime where T_Neel=T_MI is achieved, the paramagnetic insulating phase characteristic of the bulk compound is suppressed and the MIT becomes 1st order. Further increasing the in-plane compression of the SmNiO_3 lattice leads to the stabilization of a single metallic paramagnetic phase.
Perovskite SrIrO3 (SIO) films epitaxially deposited with a thickness of about 60 nm on various substrate materials display nearly strain-relieved state. Films grown on orthorhombic (110) DyScO3 (DSO) are found to display untwinned bulk-like orthorhombic structure. However, film deposition on cubic (001) SrTiO3 induces a twinned growth of SIO. Resistance measurements on the SIO films reveal only weak temperature dependence, where the resistance R increases with decreasing temperature T. Hall measurements show dominant electron-like transport throughout the temperature range from 2 K to 300 K. At 2 K, the electron concentration and resistivity for SIO on STO amount to ne = 1.4*10^20 cm-3 and 1 mohmcm. Interestingly, the film resistance of untwinned SIO on DSO along the [1-10] and the [001] direction differs by up to 25% indicating pronounced anisotropic electronic transport. The anisotropy of the resistance increases with decreasing T and displays a distinct maximum around 86 K. The specific T-dependence is similar to that of the structural anisotropy sqrt(a2+b2)/c of bulk SIO. Therefore, anisotropic electronic transport in SIO is very likely induced by the orthorhombic distortion. Consequently, for twinned SIO films on STO anisotropy vanishes nearly completely. The experimental results show that structural changes are very likely responsible for the observed anisotropic electronic transport. The strong sensitivity of the electronic transport in SIO films may be explained in terms of the narrow electron-like bands in SIO caused by spin-orbit-coupling and orthorhombic distortion.
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