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Direct confirmation of long-range magnetic order and evidence for multipoles in Ce$_{2}$O$_{3}$
Authors:
Alexandra Cote,
J. Eddie Slimak,
Astha Sethi,
Dalmau Reig-i-Plessis,
Qiang Zhang,
Yang Zhao,
Devashibhai Adroja,
Gerald Morris,
Taras Kolodiazhnyi,
Alannah M. Hallas,
Jeffrey W. Lynn,
S. Lance Cooper,
Gregory J. MacDougall
Abstract:
The sesquioxide, Ce$_{2}$O$_{3}$, has been a material of intense interest in recent years due to reports of an anomalous giant magnetodielectric effect and emergent mixed crystal field-phonon (vibronic) excitations below a putative antiferromagnetic transition at T$_{N}$ = 6.2 K. The claim of long-range magnetic order in this material is based on heat capacity and temperature-dependent susceptibil…
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The sesquioxide, Ce$_{2}$O$_{3}$, has been a material of intense interest in recent years due to reports of an anomalous giant magnetodielectric effect and emergent mixed crystal field-phonon (vibronic) excitations below a putative antiferromagnetic transition at T$_{N}$ = 6.2 K. The claim of long-range magnetic order in this material is based on heat capacity and temperature-dependent susceptibility measurements; however, multiple neutron diffraction studies have been unable to distinguish any magnetic Bragg peaks. In this article, we present the results of a comprehensive investigation of the low-temperature phase in symmetry-broken polycrystalline Ce$_{2}$O$_{3}$ using a combination of magnetic susceptibility, heat capacity, neutron diffraction, triple-axis and time-of-flight (TOF) inelastic neutron scattering (INS), and muon spin rotation ($μ$SR). Our measurements and subsequent analysis confirm that the transition at T$_{N}$ can be associated with the ordering of moments on the Ce$^{3+}$ site. Both a spontaneous magnetic order observed with $μ$SR and a dispersive spin-wave spectrum observed with inelastic neutron scattering suggest a model wherein planar dipoles order antiferromagnetically. Notable inconsistencies between $μ$SR and neutron scattering data within the dipole picture provide strong evidence for the ordering of higher-order moments.
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Submitted 21 March, 2023;
originally announced March 2023.
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Fast Design of Plasmonic Metasurfaces Enabled by Deep Learning
Authors:
Abhishek Mall,
Abhijeet Patil,
Dipesh Tamboli,
Amit Sethi,
Anshuman Kumar
Abstract:
Metasurfaces is an emerging field that enables the manipulation of light by an ultra-thin structure composed of sub-wavelength antennae and fulfills an important requirement for miniaturized optical elements. Finding a new design for a metasurface or optimizing an existing design for a desired functionality is a computationally expensive and time consuming process as it is based on an iterative pr…
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Metasurfaces is an emerging field that enables the manipulation of light by an ultra-thin structure composed of sub-wavelength antennae and fulfills an important requirement for miniaturized optical elements. Finding a new design for a metasurface or optimizing an existing design for a desired functionality is a computationally expensive and time consuming process as it is based on an iterative process of trial and error. We propose a deep learning (DL) architecture dubbed bidirectional autoencoder for nanophotonic metasurface design via a template search methodology. In contrast with the earlier approaches based on DL, our methodology addresses optimization in the space of multiple metasurface topologies instead of just one, in order to tackle the one to many mapping problem of inverse design. We demonstrate the creation of a Geometry and Parameter Space Library (GPSL) of metasurface designs with their corresponding optical response using our DL model. This GPSL acts as a universal design and response space for the optimization. As an example application, we use our methodology to design a multi-band gap-plasmon based half-wave plate metasurface. Through this example, we demonstrate the power of our technique in addressing the non-uniqueness problem of common inverse design. Our network converges aptly to multiple metasurface topologies for the desired optical response with a low mean absolute error between desired optical response and the optical response of topologies searched. Our proposed technique would enable fast and accurate design and optimization of various kinds of metasurfaces with different functionalities.
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Submitted 3 October, 2020; v1 submitted 27 March, 2020;
originally announced March 2020.
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Emergent Vibronic Excitations in the Magnetodielectric Regime of $\text{Ce}_2\text{O}_3$: Raman Scattering Studies
Authors:
A. Sethi,
J. E. Slimak,
T. Kolodiazhnyi,
S. L. Cooper
Abstract:
The strong coupling between spin, lattice and electronic degrees of freedom in magnetic materials can produce interesting phenomena, including multiferroic and magnetodielectric (MD) behavior, and exotic coupled excitations, such as electromagnons. We present a temperature- and magnetic-field-dependent inelastic light (Raman) scattering study that reveals the emergence of vibronic modes, i.e., cou…
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The strong coupling between spin, lattice and electronic degrees of freedom in magnetic materials can produce interesting phenomena, including multiferroic and magnetodielectric (MD) behavior, and exotic coupled excitations, such as electromagnons. We present a temperature- and magnetic-field-dependent inelastic light (Raman) scattering study that reveals the emergence of vibronic modes, i.e., coupled vibrational and crystal-electric-field (CEF) electronic excitations, in the unconventional rare-earth MD material, $\text{Ce}_2\text{O}_3$. The energies and intensities of these emergent vibronic modes are indicative of enhanced vibronic coupling and increased modulation of the dielectric susceptibility in the Néel state ($T_\text{N} \approx 6.2\,\text{K}$). The field-dependences of the energies and intensities of these vibronic modes are consistent with a decrease of both the vibronic coupling and the dielectric fluctuations associated with these modes below $T_\text{N}$. These results suggest a distinctive mechanism for MD behavior in $\text{Ce}_2\text{O}_3$ that is associated with a field-tunable coupling between CEF and phonon states.
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Submitted 11 March, 2019;
originally announced March 2019.
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Magnons and Magnetodielectric Effects in CoCr$_2$O$_4$: Raman Scattering Studies
Authors:
A. Sethi,
T. Byrum,
R. D. McAuliffe,
S. L. Gleason,
J. E. Slimak,
D. P. Shoemaker,
S. L. Cooper
Abstract:
Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$_2$O$_4$, is a particularly interesting example of a multiferroic material,…
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Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$_2$O$_4$, is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. This paper reports an inelastic light scattering study of the magnon and phonon spectrum of CoCr$_2$O$_4$ as simultaneous functions of temperature, pressure, and magnetic field. Below the Curie temperature ($T_C \sim 94$ K) of CoCr$_2$O$_4$ we observe a $ω\sim 16 \,\text{cm}^{-1}$ $\boldsymbol q=0$ magnon having T$_{1g}$-symmetry, which has the transformation properties of an axial vector. The anomalously large Raman intensity of the T$_{1g}$-symmetry magnon is characteristic of materials with a large magneto-optical response and likely arises from large magnetic fluctuations that strongly modulate the dielectric response in CoCr$_2$O$_4$. The Raman susceptibility of the T$_{1g}$-symmetry magnon exhibits a strong magnetic-field dependence that is consistent with the magnetodielectric response observed in CoCr$_2$O$_4$, suggesting that magnetodielectric behavior in CoCr$_2$O$_4$ primarily arises from the field-dependent suppression of magnetic fluctuations that are strongly coupled to long-wavelength phonons. Increasing the magnetic anisotropy in CoCr$_2$O$_4$ with applied pressure decreases the magnetic field-dependence of the T$_{1g}$-symmetry magnon Raman susceptibility in CoCr$_2$O$_4$, suggesting that strain can be used to control the magnetodielectric response in CoCr$_2$O$_4$.
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Submitted 15 December, 2016;
originally announced December 2016.
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Isotropic and Anisotropic Regimes of the Field-Dependent Spin Dynamics in Sr2IrO4: Raman Scattering Studies
Authors:
Y. Gim,
A. Sethi,
Q. Zhao,
J. F. Mitchell,
G. Cao,
S. L. Cooper
Abstract:
A major focus of experimental interest in Sr2IrO4 has been to clarify how the magnetic excitations of this strongly spin-orbit coupled system differ from the predictions of anisotropic 2D spin-1/2 Heisenberg model and to explore the extent to which strong spin-orbit coupling affects the magnetic properties of iridates. Here, we present a high-resolution inelastic light (Raman) scattering study of…
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A major focus of experimental interest in Sr2IrO4 has been to clarify how the magnetic excitations of this strongly spin-orbit coupled system differ from the predictions of anisotropic 2D spin-1/2 Heisenberg model and to explore the extent to which strong spin-orbit coupling affects the magnetic properties of iridates. Here, we present a high-resolution inelastic light (Raman) scattering study of the low energy magnetic excitation spectrum of Sr2IrO4 and doped Eu-doped Sr2IrO4 as functions of both temperature and applied magnetic field. We show that the high-field (H>1.5 T) in-plane spin dynamics of Sr2IrO4 are isotropic and governed by the interplay between the applied field and the small in-plane ferromagnetic spin components induced by the Dzyaloshinskii-Moriya interaction. However, the spin dynamics of Sr2IrO4 at lower fields (H<1.5 T) exhibit important effects associated with interlayer coupling and in-plane anisotropy, including a spin-flop transition at Hc in Sr2IrO4 that occurs either discontinuously or via a continuous rotation of the spins, depending upon the in-plane orientation of the applied field. These results show that in-plane anisotropy and interlayer coupling effects play important roles in the low-field magnetic and dynamical properties of Sr2IrO4.
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Submitted 21 September, 2015;
originally announced September 2015.