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Designing heterostructures to control oxygen stoichiometry in helimagnetic perovskite strontium ferrite
Authors:
Jennifer Fowlie,
Bernat Mundet,
Danilo Puggioni,
Lopa Bhatt,
Eric R. Hoglund,
Woo Jin Kim,
Jiarui Li,
Sang Jun Lee,
Wenchi Liu,
Antoine Devincenti,
James M. Rondinelli,
David A. Muller,
Harold Y. Hwang
Abstract:
A large challenge in determining the physics of helimagnetic SrFeO3 is in stabilizing the stoichiometric chemical phase over long enough time scales to conduct extensive measurements. Degradation in SrFeO3 manifests mainly as a crossover from metallic to insulating behavior. Using a combination of electronic transport and density functional theory, we show that this degradation is dominated by oxy…
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A large challenge in determining the physics of helimagnetic SrFeO3 is in stabilizing the stoichiometric chemical phase over long enough time scales to conduct extensive measurements. Degradation in SrFeO3 manifests mainly as a crossover from metallic to insulating behavior. Using a combination of electronic transport and density functional theory, we show that this degradation is dominated by oxygen loss, possibly on the order of one percent. We further demonstrate that high quality SrFeO3 thin films can be stabilized long-term by combining a nanoscale band insulator capping layer with an ex situ ozone anneal. We show that this produces a nearly-pristine cation sublattice and preserves metallicity for at least several weeks. These results establish a reliable pathway for producing chemically stable SrFeO3 thin films, enabling reproducible studies of its unusual helimagnetism.
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Submitted 24 February, 2026;
originally announced February 2026.
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Optical conductivity signatures of strong correlations and multiband superconductivity in infinite-layer nickelates
Authors:
Woo Jin Kim,
Kyuho Lee,
Eun Kyo Ko,
Jaeseok Son,
Yonghun Lee,
Yijun Yu,
Soon Jae Moon,
Tae Won Noh,
Harold Y. Hwang
Abstract:
Since the discovery of superconductivity in infinite-layer nickelates, there have been extensive efforts to unravel their electronic structure and pairing mechanism. In particular, understanding how the electronic structure evolves with doping is essential for clarifying theoretical models of superconductivity in nickelates. Here we present studies of the optical conductivity of Nd1-xSrxNiO2 thin…
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Since the discovery of superconductivity in infinite-layer nickelates, there have been extensive efforts to unravel their electronic structure and pairing mechanism. In particular, understanding how the electronic structure evolves with doping is essential for clarifying theoretical models of superconductivity in nickelates. Here we present studies of the optical conductivity of Nd1-xSrxNiO2 thin films spanning the full phase diagram 0.025 < x < 0.30 using spectroscopic ellipsometry. The data are consistent with a two-band Drude model, which allows the decomposition of the intraband response into distinct contributions. One is from a "narrow" Drude term which we associate with electron bands, and the other a "broad" Drude term linked to the hole band with strong correlations. Increasing Sr doping leads to an expansion of the hole band spectral weight, and a corresponding reduction in the electron band, indicative of the multiband electronic structure and a doping-dependent reconstruction of the Fermi surface. Both doping and temperature-dependent optical spectra display significant spectral weight transfer from high to low energy, a hallmark of strong electronic correlations. In the superconducting state at optimal doping (x = 0.15), both electron and hole bands contribute to the superconducting condensate, signifying multiband superconductivity.
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Submitted 10 February, 2026;
originally announced February 2026.
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Orbital inversion and emergent lattice dynamics in infinite layer CaCoO$_2$
Authors:
Daniel Jost,
Eder G. Lomeli,
Woo Jin Kim,
Emily M. Been,
Matteo Rossi,
Stefano Agrestini,
Kejin Zhou,
Chunjing Jia,
Brian Moritz,
Zhi-Xun Shen,
Harold Y. Hwang,
Thomas P. Devereaux,
Wei-Sheng Lee
Abstract:
The layered cobaltate CaCoO$_2$ exhibits a unique herringbone-like structure. Serving as a potential prototype for a new class of complex lattice patterns, we study the properties of CaCoO$_2$ using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Our results reveal a significant inter-plane hybridization between the Ca $4s-$ and Co $3d-$orbitals, leading to an i…
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The layered cobaltate CaCoO$_2$ exhibits a unique herringbone-like structure. Serving as a potential prototype for a new class of complex lattice patterns, we study the properties of CaCoO$_2$ using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Our results reveal a significant inter-plane hybridization between the Ca $4s-$ and Co $3d-$orbitals, leading to an inversion of the textbook orbital occupation of a square planar geometry. Further, our RIXS data reveal a strong low energy mode, with anomalous intensity modulations as a function of momentum transfer close to a quasi-static response suggestive of electronic and/or orbital ordering. These findings indicate that the newly discovered herringbone structure exhibited in CaCoO$_2$ may serve as a promising laboratory for the design of materials having strong electronic, orbital and lattice correlations.
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Submitted 11 September, 2024;
originally announced September 2024.
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Character of the "normal state" of the nickelate superconductors
Authors:
Kyuho Lee,
Bai Yang Wang,
Motoki Osada,
Berit H. Goodge,
Tiffany C. Wang,
Yonghun Lee,
Shannon Harvey,
Woo Jin Kim,
Yijun Yu,
Chaitanya Murthy,
Srinivas Raghu,
Lena F. Kourkoutis,
Harold Y. Hwang
Abstract:
The occurrence of superconductivity in proximity to various strongly correlated phases of matter has drawn extensive focus on their normal state properties, to develop an understanding of the state from which superconductivity emerges. The recent finding of superconductivity in layered nickelates raises similar interests. However, transport measurements of doped infinite-layer nickelate thin films…
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The occurrence of superconductivity in proximity to various strongly correlated phases of matter has drawn extensive focus on their normal state properties, to develop an understanding of the state from which superconductivity emerges. The recent finding of superconductivity in layered nickelates raises similar interests. However, transport measurements of doped infinite-layer nickelate thin films have been hampered by materials limitations of these metastable compounds - in particular, a relatively high density of extended defects. Here, by moving to a substrate (LaAlO$_{3}$)$_{0.3}$(Sr$_{2}$TaAlO$_{6}$)$_{0.7}$ which better stabilizes the growth and reduction conditions, we can synthesize the doping series of Nd$_{1-x}$Sr$_{x}$NiO$_{2}$ essentially free from extended defects. This enables the first examination of the 'intrinsic' temperature and doping dependent evolution of the transport properties. The normal state resistivity exhibits a low-temperature upturn in the underdoped regime, linear behavior near optimal doping, and quadratic temperature dependence for overdoping. This is strikingly similar to the copper oxides, despite key distinctions - namely the absence of an insulating parent compound, multiband electronic structure, and a Mott-Hubbard orbital alignment rather than the charge-transfer insulator of the copper oxides. These results suggest an underlying universality in the emergent electronic properties of both superconducting families.
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Submitted 4 March, 2022;
originally announced March 2022.
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Insulator-to-Metal Crossover near the Edge of the Superconducting Dome in Nd$_{1-x}$Sr$_x$NiO$_2$
Authors:
Yu-Te Hsu,
Bai Yang Wang,
Maarten Berben,
Danfeng Li,
Kyuho Lee,
Caitlin Duffy,
Thom Ottenbros,
Woo Jin Kim,
Motoki Osada,
Steffen Wiedmann,
Harold Y. Hwang,
Nigel E. Hussey
Abstract:
We report a systematic magnetotransport study of superconducting infinite-layer nickelate thin films Nd$_{1-x}$Sr$_x$NiO$_2$ with $0.15 \leq x \leq 0.225$. By suppressing superconductivity with out-of-plane magnetic fields up to 37.5 T, we find that the normal state resistivity of Nd$_{1-x}$Sr$_x$NiO$_2$ is characterized by a crossover from a metallic $T^2$-behavior to an insulating log(1/$T$)-beh…
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We report a systematic magnetotransport study of superconducting infinite-layer nickelate thin films Nd$_{1-x}$Sr$_x$NiO$_2$ with $0.15 \leq x \leq 0.225$. By suppressing superconductivity with out-of-plane magnetic fields up to 37.5 T, we find that the normal state resistivity of Nd$_{1-x}$Sr$_x$NiO$_2$ is characterized by a crossover from a metallic $T^2$-behavior to an insulating log(1/$T$)-behavior for all $x$ except $x = 0.225$, at which the resistivity is predominantly metallic. The log(1/$T$)-behavior is found to be robust against magnetic fields, inconsistent with scenarios involving localization or Kondo scattering, and points to an anomalous insulating state possibly driven by strong correlations. In the metallic state, we find no evidence for non-Fermi-liquid behavior arising from proximity to a putative quantum critical point located inside the superconducting dome.
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Submitted 8 November, 2021; v1 submitted 17 May, 2021;
originally announced May 2021.
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Electronic band structure of (111) $SrRuO_{3}$ thin film$-$an angle-resolved photoemission spectroscopy study
Authors:
Hanyoung Ryu,
Yukiaki Ishida,
Bongju Kim,
Jeong Rae Kim,
Woo Jin Kim,
Yoshimitsu Kohama,
Shusaku Imajo,
Zhuo Yang,
Wonshik Kyung,
Sungsoo Hahn,
Byungmin Sohn,
Inkyung Song,
Minsoo Kim,
Soonsang Huh,
Jongkeun Jung,
Donghan Kim,
Tae Won Noh,
Saikat Das,
Changyoung Kim
Abstract:
We studied the electronic band structure of pulsed laser deposition (PLD) grown (111)-oriented SrRuO$_3$ (SRO) thin films using \textit{in situ} angle-resolved photoemission spectroscopy (ARPES) technique. We observed previously unreported, light bands with a renormalized quasiparticle effective mass of about 0.8$m_{e}$. The electron-phonon coupling underlying this mass renormalization yields a ch…
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We studied the electronic band structure of pulsed laser deposition (PLD) grown (111)-oriented SrRuO$_3$ (SRO) thin films using \textit{in situ} angle-resolved photoemission spectroscopy (ARPES) technique. We observed previously unreported, light bands with a renormalized quasiparticle effective mass of about 0.8$m_{e}$. The electron-phonon coupling underlying this mass renormalization yields a characteristic "kink" in the band dispersion. The self-energy analysis using the Einstein model suggests five optical phonon modes covering an energy range 44 to 90 meV contribute to the coupling. Besides, we show that the quasiparticle spectral intensity at the Fermi level is considerably suppressed, and two prominent peaks appear in the valance band spectrum at binding energies of 0.8 eV and 1.4 eV, respectively. We discuss the possible implications of these observations. Overall, our work demonstrates that high-quality thin films of oxides with large spin-orbit coupling can be grown along the polar (111) orientation by the PLD technique, enabling \textit{in situ} electronic band structure study. This could allow for characterizing the thickness-dependent evolution of band structure of (111) heterostructures$-$a prerequisite for exploring possible topological quantum states in the bilayer limit.
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Submitted 25 January, 2021; v1 submitted 11 February, 2020;
originally announced February 2020.
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Unconventional anomalous Hall effect from antiferromagnetic domain walls of Nd2Ir2O7 thin films
Authors:
Woo Jin Kim,
John H. Gruenewald,
Taekoo Oh,
Sangmo Cheon,
Bongju Kim,
Oleksandr B. Korneta,
Hwanbeom Cho,
Daesu Lee,
Yoonkoo Kim,
Miyoung Kim,
Je-Geun Park,
Bohm-Jung Yang,
Ambrose Seo,
Tae Won Noh
Abstract:
Ferroic domain walls (DWs) create different symmetries and ordered states compared with those in single-domain bulk materials. In particular, the DWs of an antiferromagnet (AFM) with non-coplanar spin structure have a distinct symmetry that cannot be realized in those of their ferromagnet counterparts. In this paper, we show that an unconventional anomalous Hall effect (AHE) can arise from the DWs…
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Ferroic domain walls (DWs) create different symmetries and ordered states compared with those in single-domain bulk materials. In particular, the DWs of an antiferromagnet (AFM) with non-coplanar spin structure have a distinct symmetry that cannot be realized in those of their ferromagnet counterparts. In this paper, we show that an unconventional anomalous Hall effect (AHE) can arise from the DWs of a non-coplanar AFM, Nd2Ir2O7. Bulk Nd2Ir2O7 has a cubic symmetry; thus, its Hall signal should be zero without an applied magnetic field. The DWs generated in this material break the two-fold rotational symmetry, which allows for finite anomalous Hall conductivity. A strong f-d exchange interaction between the Nd and Ir magnetic moments significantly influences antiferromagnetic domain switching. Our epitaxial Nd2Ir2O7 thin film showed a large enhancement of the AHE signal when the AFM domains switched, indicating that the AHE is mainly due to DWs. Our study highlights the symmetry broken interface of AFM materials as a new means of exploring topological effects and their relevant applications.
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Submitted 6 July, 2018;
originally announced July 2018.
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Development of a high-sensitivity torsion balance to investigate the thermal Casimir force
Authors:
T. Graveson,
C. Rackson,
W. J. Kim
Abstract:
We report development of a high-sensitivity torsion balance to measure the thermal Casimir force. Special emphasis is placed on experimental investigations of a possible surface electric force originating from surface patch potentials that have been recently noticed by several experimental groups. By gaining a proper understanding of the actual contribution of the surface electric force in real ma…
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We report development of a high-sensitivity torsion balance to measure the thermal Casimir force. Special emphasis is placed on experimental investigations of a possible surface electric force originating from surface patch potentials that have been recently noticed by several experimental groups. By gaining a proper understanding of the actual contribution of the surface electric force in real materials, we aim to undertake precision force measurements to resolve the Casimir force at finite temperature in real metals, as well as in other semiconducting materials, such as graphene.
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Submitted 12 February, 2012;
originally announced February 2012.
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Reply to "Comment on 'Anomalies in electrostatic calibrations for the measurement of the Casimir force in a sphere-plane geometry'"
Authors:
W. J. Kim,
M. Brown-Hayes,
D. A. R. Dalvit,
J. H. Brownell,
R. Onofrio
Abstract:
In a recent Comment, Decca et al. [Phys. Rev. A 79, 026101 (2009); arXiv:0809.3576] discussed the origin of the anomalies recently reported by us in Phys. Rev. A 78, 036102(R) (2008); arXiv:0812.0028 . Here we restate our view, corroborated by their considerations, that quantitative geometrical and electrostatic characterizations of the conducting surfaces (a topic not discussed explicitly in th…
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In a recent Comment, Decca et al. [Phys. Rev. A 79, 026101 (2009); arXiv:0809.3576] discussed the origin of the anomalies recently reported by us in Phys. Rev. A 78, 036102(R) (2008); arXiv:0812.0028 . Here we restate our view, corroborated by their considerations, that quantitative geometrical and electrostatic characterizations of the conducting surfaces (a topic not discussed explicitly in the literature until very recently) are critical for the assessment of precision and accuracy of the demonstration of the Casimir force and for deriving meaningful limits on the existence of Yukawian components possibly superimposed to the Newtonian gravitational interaction.
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Submitted 5 March, 2009;
originally announced March 2009.
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On electrostatic and Casimir force measurements between conducting surfaces in a sphere-plane configuration
Authors:
W. J. Kim,
M. Brown-Hayes,
D. A. R. Dalvit,
J. H. Brownell,
R. Onofrio
Abstract:
We report on measurements of forces acting between two conducting surfaces in a spherical-plane configuration in the 35 nm-1 micrometer separation range. The measurements are obtained by performing electrostatic calibrations followed by a residual analysis after subtracting the electrostatic-dependent component. We find in all runs optimal fitting of the calibrations for exponents smaller than t…
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We report on measurements of forces acting between two conducting surfaces in a spherical-plane configuration in the 35 nm-1 micrometer separation range. The measurements are obtained by performing electrostatic calibrations followed by a residual analysis after subtracting the electrostatic-dependent component. We find in all runs optimal fitting of the calibrations for exponents smaller than the one predicted by electrostatics for an ideal sphere-plane geometry. We also find that the external bias potential necessary to minimize the electrostatic contribution depends on the sphere-plane distance. In spite of these anomalies, by implementing a parametrixation-dependent subtraction of the electrostatic contribution we have found evidence for short-distance attractive forces of magnitude comparable to the expected Casimir-Lifshitz force. We finally discuss the relevance of our findings in the more general context of Casimir-Lifshitz force measurements, with particular regard to the critical issues of the electrical and geometrical characterization of the involved surfaces.
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Submitted 1 December, 2008;
originally announced December 2008.
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Anomalies in electrostatic calibrations for the measurement of the Casimir force in a sphere-plane geometry
Authors:
W. J. Kim,
M. Brown-Hayes,
D. A. R. Dalvit,
J. H. Brownell,
R. Onofrio
Abstract:
We have performed precision electrostatic calibrations in the sphere-plane geometry and observed anomalous behavior. Namely, the scaling exponent of the electrostatic signal with distance was found to be smaller than expected on the basis of the pure Coulombian contribution and the residual potential found to be distance dependent. We argue that these findings affect the accuracy of the electros…
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We have performed precision electrostatic calibrations in the sphere-plane geometry and observed anomalous behavior. Namely, the scaling exponent of the electrostatic signal with distance was found to be smaller than expected on the basis of the pure Coulombian contribution and the residual potential found to be distance dependent. We argue that these findings affect the accuracy of the electrostatic calibrations and invite reanalysis of previous determinations of the Casimir force.
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Submitted 1 December, 2008;
originally announced December 2008.