Epitaxial Stabilization of Ultrathin Films of Rare-Earth Nickelates

Meyers, D. J.; Moon, E. J.; Kareev, M.; Tung, I. C.; Gray, B. A.; Liu, Jian; Bedzyk, M. J.; Freeland, J. W.; Chakhalian, J.

doi:10.48550/arxiv.1112.5348

2011

DOI: 10.48550/arxiv.1112.5348

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Epitaxial Stabilization of Ultrathin Films of Rare-Earth Nickelates

D. J. Meyers,

E. J. Moon,

M. Kareev

et al.

Abstract: We report on the synthesis of ultrathin films of highly distorted EuNiO 3 (ENO) grown by interrupted pulse laser epitaxy on YAlO 3 (YAO) substrates. Through mapping the phase space of nickelate thin film epitaxy, the optimal growth temperatures were found to scale linearly with the Goldschmidt tolerance factor.Considering the gibbs energy of the expanding film, this empirical trend is discussed in terms of epitaxial stabilization and the escalation of the lattice energy due to lattice distortions and decreasin… Show more

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Cited by 2 publications

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“…The thicker sample (35 uc) was required in order to obtain a strong enough (-103) film peak with the conventional source XRD. The H value of this film peak matches well with that of the substrate (demonstrated by the dotted line) confirming the film is fully coherent to the substrate (as was found for ENO on YAO 46 ), while the center L value of ∼ 3.053 r.l.u. gives an out-of-plane lattice constant of 3.793 Å, in excellent agreement with the rocking curve measurement (within 0.2 %).…”

supporting

confidence: 79%

“…R= Nd and Pr) exhibit a first order phase transition emerging directly from the paramagnetic metallic state into the E -type antiferromagnetic insulating ground state, thus bypassing entirely the large param-agnetic insulating region 29,[36][37][38] . Based on such a diverse behavior controlled by the A-site ion, several interesting theory proposals and experimental results have been put forward to control the MIT for potential applications [39][40][41][42] ; however, using different R ions depending on application seems impractical, as synthesis conditions and thermal stability vary wildly and rarely yield macroscopic size crystals of nickelates 13,[43][44][45][46] . Alternatively, one can explore the obligatory strain in ultra-thin films as a tool to engineer the physical properties based on a careful choice of a single member of the family to attempt to modulate the MI and AFM transitions [13][14][15] .…”

mentioning

confidence: 99%

“…ENO films were grown on a variety of substrates incorporating lattice mismatch ranging from +2.5% to -2.4%, the details of which are reported elsewhere 46 . The substrates arXiv:1304.1751v2 [cond-mat.str-el] 29 Jul 2013 used for growth are as follows: YAlO 3 (YAO; -2.4% lattice mismatch), SrLaAlO 4 (SLAO; -1.3%), LaAlO 3 (LAO; -0.3%), NdGaO 3 (NGO; +1.5%), and LaGaO 3 (LGO; +2.5%).…”

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Strain-modulated Mott transition in EuNiO3ultrathin films

et al. 2013

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A series of ultra-thin epitaxial films of EuNiO3 (ENO) were grown on a set of substrates traversing from compressive (-2.4%) to tensile (+2.5%) lattice mismatch. On moving from tensile to compressive strain, transport measurements demonstrate a successively suppressed Mott insulating behavior eventually resulting in a complete suppression of the insulating state at high compressive strain. Corroborating these findings, resonant soft X-ray absorption spectroscopy at Ni L3,2 edge reveal the presence of a strong multiplet splitting in the tensile strained samples that progressively weakens with increasing compressive strain. Combined with the ab initio cluster calculations, the results show how comulatively enhanced covalency (i.e. bandwidth) between Ni d-and O p-orbital derived states leads to the emergent metallic ground state not attainable in the bulk ENO.Complex transition metal oxides with correlated carriers have been at the forefront of condensed matter research towards the understanding of fundamental physics underlying several remarkable physical phenomena including high temperature superconductivity, colossal magnetoresistance, multiferroicity, and the thermally induced metal-insulator transition (MIT) [1][2][3][4][5][6] . In particular, the temperature driven MIT in correlated oxides has garnered a strong investigation effort over last several decades. Understanding of the MIT and its control by external stimuli such as pressure, magnetic field, light, confinement, or chemical doping is not only interesting from the fundamental physics point of view 7-10 , but also demonstrate great opportunities for future electronic devices 11 . On the way to those goals, recent advances in material synthesis by using strain engineering have opened a new dimension in controlling the materials properties. Additionally, the epitaxial relation has been used to stabilize new structural and electronic phases in the form of ultra thin films of coherently strained materials 12 . In such epitaxially stabilized structures, the effect of the lattice modulation on the materials properties can be quite dramatic 13,14,[16][17][18][19][20][21][22][23][24][25][26][27] and is of particular current interest as applications continue to accelerate towards ultra-thin films and heterostructures.The rare-earth (RE) nickelates RNiO 3 (R = Pr, Nd, Eu, ...) in their bulk form, with Ni having formal +3 oxidation state (t 6 2g e 1 g ), all, except for R = La, display a metal-insulator transition, while the nature of the transition and its temperature (T M IT ) depends strongly on the choice of the rare-earth cation as shown in Fig. 1 28-30 . Specifically, the most distorted members with R= Lu, Y, Eu and Sm, etc. first exhibit a second order MIT at higher temperature accompanied by the development of a possible charge ordered state 31-35 while the magnetic moments remain disordered across the transition. Upon further cooling, these compounds undergo another second order transition characterized by a E -type antiferromagnetism. In sharp contrast,...

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confidence: 99%

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Strain-modulated Mott transition in EuNiO3ultrathin films

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“…To create the quantum wells, high-quality epitaxial NdNiO 3 ultrathin slabs oriented along the pseudo-cubic (001) direction were grown by laser molecular beam epitaxy, as described elsewhere in detail [29,30]. In situ reflection High Energy Electron Diffraction was used to monitor the layer-by-layer growth for 'digital' control of the quantum well structure.…”

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Metal-Insulator Transition and Orbital Reconstruction in Mott-Type Quantum Wells Made ofNdNiO3

et al. 2012

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The metal-insulator transition (MIT) and the underlying electronic and orbital structure in e 1 g quantum wells based on NdNiO3 was investigated by d.c. transport and resonant soft x-ray absorption spectroscopy. By comparing quantum wells of the same dimension but with two different confinement structures, we explicitly demonstrate that the quantum well boundary condition of correlated electrons is critical to selecting the manybody ground state. In particular, the long-range orderings and the MIT are found to be strongly enhanced under quantum confinement by sandwiching NdNiO3 with the wide-gap dielectric LaAlO3, while they are suppressed when one of the interfaces is replaced by a surface (interface with vacuum). Resonant spectroscopy reveals that the reduced charge fluctuations in the sandwich structure are supported by the enhanced propensity to charge ordering due to the suppressed eg orbital splitting when interfaced with the confining LaAlO3 layer.Low-dimensional electronic systems have been a focus of condensed matter physics for decades and are known to exhibit numerous fascinating quantum states. A prominent example is quantum well based on semiconductor heterojunctions which has become a foundation of modern technology. Recently, artificial confinement of Mott electrons is emerging as a compelling route to create new two-dimensional (2D) systems unobtainable in the bulk form [1,2]. Heterostructures involving i.e. cuprates, manganites and LaAlO 3 /SrTiO 3 have revealed the spectacular versatility and fascinating playground of complex oxide interfaces [3][4][5][6].In Mott quantum well structures, an ultrathin electronically active slab of correlated oxide is constrained in an epitaxial heterostructure where the vertical hopping of the d-electrons is typically suppressed by dielectric oxide blocks. This geometry was previously shown to provide competing pathways to polar compensation [7,8], and has recently been harnessed to generate unusual confinement-induced orbital reconstruction [9][10][11] and dimensionality-controlled metalinsulator transition (MIT) [12][13][14][15][16]. Appealing many-body phenomena have also been predicted, including proposals of half-metallic semi-Dirac points [17] as well as various engaging orderings of charge, spin and orbital [18,19]. In particular, quantum confinement of e 1 g -system based on the Ni III (3d 7 ) low-spin state in perovskite nickelate RNiO 3 (R=rare earth) is of great interest, due to the possibilities in inducing novel quantum states, e.g. topological phases [20] and unconventional high-T c superconductivity [18,21,22]. To realize these intriguing phenomena, a controlled manipulation of the orbital degeneracy of e g electrons via confinement is required. While confinement-induced orbital polarizations were recently observed in both metallic and insulating states in (001)-oriented superlattices [10,11], the quantum well structure has also been shown to affect the ground state from a three-dimensional (3D) correlated metal to a (quasi-)2D Mott insulator with...

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Epitaxial Stabilization of Ultrathin Films of Rare-Earth Nickelates

Cited by 2 publications

References 24 publications

Strain-modulated Mott transition in EuNiO3ultrathin films

Strain-modulated Mott transition in EuNiO3ultrathin films

Metal-Insulator Transition and Orbital Reconstruction in Mott-Type Quantum Wells Made ofNdNiO3

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