arXiv subjects

S. -W. Cheong

Publications and source records attributed to S. -W. Cheong.

At least 55 records · Page 3Linked to original sources

arXiv2017

Surface vibrational modes of the topological insulator Bi$_2$Se$_3$ observed by Raman spectroscopy

We present polarization resolved Raman scattering study of surface vibration modes in the topological insulator Bi$_2$Se$_3$ single crystal and thick films. Besides the four Raman active bulk phonons, we observed four additional modes with much weaker intensity and slightly lower energy than the bulk counterparts. Using symmetry analysis, we assigned these additional modes to out-of-plane surface phonons. Comparing with first principle calculations, we conclude that the appearance of these modes is due to $c$-axis lattice distortion and van der Waals gap expansion near the crystal surface. Two of the surface modes at 60 and 173 cm$^{-1}$ are associated with Raman active $A_{1g}$ bulk phonon modes, the other two at 136 and 158 cm$^{-1}$ are associated with infrared active bulk phonons with $A_{2u}$ symmetry. The latter become Raman allowed due to reduction of crystalline symmetry from $D_{3d}$ in the bulk to $C_{3v}$ on the crystal surface. In particular, the 158 cm$^{-1}$ surface phonon mode shows a Fano lineshape under resonant excitation, suggesting interference in the presence of electron-phonon coupling of the surface excitations.

cond-mat.mtrl-sci↗

arXiv2017

Magnetoelectric Phase Diagrams of Multiferroic GdMn2O5

Electric and magnetic properties of multiferroic GdMn2O5 in external magnetic fields were investigated to map out the magnetoelectric phases in this material. Due to strong magnetoelectric coupling, the dielectric permittivity is highly sensitive to phase boundaries in GdMn2O5, which allowed to construct the field-temperature phase diagrams. Several phase transitions are observed which are strongly field-dependent with respect to field orientation and strength. The phase diagram for a magnetic field along the crystallographic a-axis corresponds well to a polarization step, as induced by 90 degree rotation of Gd magnetic moments. Our results support the model of two ferroelectric sublattices, Mn-Mn and Gd-Mn with strong R-Mn (4f-3d) interaction for the polarization in RMn2O5.

cond-mat.mtrl-sci↗

arXiv2017

Spin glass behavior in frustrated quantum spin system CuAl2O4 with a possible orbital liquid state

CuAl2O4 is a normal spinel oxide having quantum spin, S=1/2 for Cu2+. It is a rather unique feature that the Cu2+ ions of CuAl2O4 sit at a tetrahedral position, not like the usual octahedral position for many oxides. At low temperatures, it exhibits all the thermodynamic evidence of a quantum spin glass. For example, the polycrystalline CuAl2O4 shows a cusp centered at ~2 K in the low-field dc magnetization data and a clear frequency dependence in the ac magnetic susceptibility while it displays logarithmic relaxation behavior in a time dependence of the magnetization. At the same time, there is a peak at ~2.3 K in the heat capacity, which shifts towards higher temperature with magnetic fields. On the other hand, there is no evidence of new superlattice peaks in the high-resolution neutron powder diffraction data when cooled from 40 to 0.4 K. This implies that there is no long-ranged magnetic order down to 0.4 K, thus confirming a spin glass-like ground state for CuAl2O4. Interestingly, there is no sign of structural distortion either although Cu2+ is a Jahn-Teller active ion. Thus, we claim that an orbital liquid state is the most likely ground state in CuAl2O4. Of further interest, it also exhibits a large frustration parameter, f = Theta_CW/Tm ~67, one of the largest values reported for spinel oxides. Our observations suggest that CuAl2O4 should be a rare example of a frustrated quantum spin glass with a good candidate for an orbital liquid state.

cond-mat.str-el↗

arXiv2016

Spontaneous decays of magneto-elastic excitations in noncollinear antiferromagnet (Y,Lu)MnO3

When magnons and phonons, the fundamental quasiparticles of the solid, are coupled to one another, they form a new hybrid quasi-particle, leading to novel phenomena and interesting applications. Despite its wide-ranging importance, however, detailed experimental studies on the underlying Hamiltonian is rare for actual materials. Moreover, the anharmonicity of such magnetoelastic excitations remains largely unexplored although it is essential for a proper understanding of their diverse thermodynamic behaviour as well as intrinsic zero-temperature decay. Here we show that in noncollinear antiferromagnets, a strong magnon-phonon coupling can significantly enhance the anharmonicity, resulting in the creation of magnetoelastic excitations and their spontaneous decay. By measuring the spin waves over the full Brillouin zone and carrying out anharmonic spin wave calculations using a Hamiltonian with an explicit magnon-phonon coupling, we have identified a hybrid magnetoelastic mode in (Y,Lu)MnO3 and quantified its decay rate and the exchange-striction coupling term required to produce it. Our work has wide implications for understanding of the spin-phonon coupling and the resulting excitations of the broad classes of noncollinear magnets.

cond-mat.mtrl-sci↗

arXiv2016

Directly probing spin dynamics in insulating antiferromagnets using ultrashort terahertz pulses

We investigate spin dynamics in the antiferromagnetic (AFM) multiferroic TbMnO3 using optical- pump, terahertz (THz)-probe spectroscopy. Photoexcitation results in a broadband THz transmission change, with an onset time of 25 ps at 6 K that becomes faster at higher temperatures. We attribute this time constant to spin-lattice thermalization. The excellent agreement between our measurements and previous ultrafast resonant x-ray diffraction measurements on the same material confirms that our THz pulse directly probes spin order. We suggest that this could be the case in general for insulating AFM materials, if the origin of the static absorption in the THz spectral range is magnetic.

cond-mat.str-el↗

arXiv2016

Topological defects at octahedral tilting plethora in bi-layered perovskites

Oxygen octahedral distortions including tilts/rotations, deformations and off-centering in (layered) perovskites play the key role in their numerous functional properties. At the polar-centrosymmetric phase boundary in bi-layered perovskite Ca3-xSrxTi2O7 with x~1, we found the presence of abundant topological Z8 vortex-antivortex pairs, associated with four oxygen octahedral tilts at domains and another four different oxygen octahedral tilts at domain boundaries. Our discovery opens a new revenue to unveil topological defects associated with various types of oxygen octahedral distortions.

cond-mat.mtrl-sci↗

arXiv2016

Solitary magnons in the $S={5\over2}$ antiferromagnet CaFe$_{2}$O$_{4}$

CaFe$_{2}$O$_{4}$ is a $S={5\over 2}$ anisotropic antiferromagnet based upon zig-zag chains having two competing magnetic structures, denoted as the A ($\uparrow \uparrow \downarrow \downarrow$) and B ($\uparrow \downarrow \uparrow \downarrow$) phases, which differ by the $c$-axis stacking of ferromagnetic stripes. We apply neutron scattering to demonstrate that the competing A and B phase order parameters results in magnetic antiphase boundaries along $c$ which freeze on the timescale of $\sim$ 1 ns at the onset of magnetic order at 200 K. Using high resolution neutron spectroscopy, we find quantized spin wave levels and measure 9 such excitations localized in regions $\sim$ 1-2 $c$-axis lattice constants in size. We discuss these in the context of solitary magnons predicted to exist in anisotropic systems. The magnetic anisotropy affords both competing A+B orders as well as localization of spin excitations in a classical magnet.

cond-mat.str-el↗

arXiv2016

Electronic Structure, Optical and Dielectric Spectroscopy Study of TbMnO3

Spectral ellipsometry studies of the optical functions, first observation of photoluminescence and low frequency dielectric permittivity investigations were performed in ferroelectric - multiferroic TbMnO3 single crystals. The main attention was paid to electronic band structure, nature of the main optical transitions and unusual behavior of the dielectric permittivity in the region of the sharp narrow temperature maximum, associated with ferroelectric phase transition. It was found that magnitude of the permittivity maximum decreases strongly with frequency, whereas position of maximum is frequency independent. Observed features of polarization response can be described satisfactorily in the frame of on the basis of the Landau-Khalatnikov theory for critical relaxation polarization

cond-mat.mtrl-sci↗

arXiv2016

Domain Topology and Domain Switching Kinetics in a Hybrid Improper Ferroelectric

Charged polar interfaces such as charged ferroelectric domain walls or heterostructured interfaces of ZnO/(Zn,Mg)O and LaAlO3/SrTiO3, across which the normal component of electric polarization changes suddenly, can host large two-dimensional conduction. Charged ferroelectric walls, which are energetically unfavorable in general, were found to be mysteriously abundant in hybrid improper ferroelectric (Ca,Sr)3Ti2O7 crystals. From the exploration of antiphase boundaries in bilayer-perovskites, we discover that each of four polarization-direction states is degenerated with two antiphase domains, and these eight structural variants form a Z4xZ2 domain structure with Z3 vortices and five distinct types of domain walls, whose topology is directly relevant to the presence of abundant charged walls. We also discover a zipper-like nature of antiphase boundaries; they are the reversible creation/annihilation centers of pairs of two types of ferroelectric walls (and also Z3-vortex pairs) in 90 and 180 degree polarization switching. Our results demonstrate the unexpectedly rich nature of hybrid improper ferroelectricity.

cond-mat.mtrl-sci↗

arXiv2015

Ambipolar Transport and Magneto-resistance Crossover in a Mott Insulator, Sr$_{2}$IrO$_{4}$

Electric field effect (EFE) controlled magnetoelectric transport in thin films of undoped and La-doped Sr$_{2}$IrO$_{4}$ (SIO) were investigated under the action of ionic liquid gating. Despite large carrier density modulation, the temperature dependent resistance measurements exhibit insulating behavior in chemically and EFE doped samples with the band filling up to 10\%. The ambipolar transport across the Mott gap is demonstrated by EFE tuning of the activation energy. Further, we observe a crossover from a negative magnetoresistance (MR) at high temperatures to positive MR at low temperatures. The crossover temperature was around $\sim$80-90 K, irrespective of the filling. This temperature and magnetic field dependent crossover is qualitatively associated with a change in the conduction mechanism from Mott to Coulomb gap mediated variable range hopping (VRH). This explains the origin of robust insulating ground state of SIO in electrical transport studies and highlights the importance of disorder and Coulombic interaction on electrical properties of SIO.

cond-mat.str-el↗

arXiv2015

Successive magnetic field-induced transitions and colossal magnetoelectric effect in Ni$_{3}$TeO$_{6}$

We report the discovery of a metamagnetic phase transition in a polar antiferromagnet Ni$_3$TeO$_6$ that occurs at 52 T. The new phase transition accompanies a colossal magnetoelectric effect, with a magnetic-field-induced polarization change of 0.3 $μ$C/cm$^2$, a value that is 4 times larger than for the spin-flop transition at 9 T in the same material, and also comparable to the largest magnetically-induced polarization changes observed to date. Via density-functional calculations we construct a full microscopic model that describes the data. We model the spin structures in all fields and clarify the physics behind the 52 T transition. The high-field transition involves a competition between multiple different exchange interactions which drives the polarization change through the exchange-striction mechanism. The resultant spin structure is rather counter-intuitive and complex, thus providing new insights on design principles for materials with strong magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2015

Spin waves and revised crystal structure of honeycomb iridate Na2IrO3

We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zig-zag magnetic order. The onset of long-range magnetic order below 15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90 deg Ir-O-Ir bonds required for dominant Kitaev exchange.

cond-mat.str-el↗

arXiv2015

High-resolution structure studies and magnetoelectric coupling of relaxor multiferroic Pb(Fe$_{0.5}$Nb$_{0.5}$)O$_3$

Pb(Fe$_{0.5}$Nb$_{0.5}$)O$_3$ (PFN), one of the few relaxor multiferroic systems, has a $G$-type antiferromagnetic transition at $T_N$ = 143 K and a ferroelectric transition at $T_C$ = 385 K. By using high-resolution neutron-diffraction experiments and a total scattering technique, we paint a comprehensive picture of the long- and short-range structures of PFN: (i) a clear sign of short-range structural correlation above $T_C$, (ii) no sign of the negative thermal expansion behavior reported in a previous study, and (iii) clearest evidence thus far of magnetoelectric coupling below $T_N$. We conclude that at the heart of the unusual relaxor multiferroic behavior lies the disorder between Fe$^{3+}$ and Nb$^{5+}$ atoms. We argue that this disorder gives rise to short-range structural correlations arising from O disorder in addition to Pb displacement.

cond-mat.mtrl-sci↗

arXiv2014

Dimerization-Induced Fermi-Surface Reconstruction in IrTe2

We report a de Haas-van Alphen (dHvA) oscillation study on IrTe2 single crystals showing complex dimer formations. By comparing the angle dependence of dHvA oscillations with band structure calculations, we show distinct Fermi surface reconstruction induced by a 1/5-type and a 1/8-type dimerizations. This verifies that an intriguing quasi-two-dimensional conducting plane across the layers is induced by dimerization in both cases. A phase transition to the 1/8 phase with higher dimer density reveals that local instabilities associated with intra- and interdimer couplings are the main driving force for complex dimer formations in IrTe2.

cond-mat.str-el↗

arXiv2014

Quadrupolar Singlet Ground State of Praseodymium in a Modulated Pyrochlore

The complex structure and magnetism of Pr$_{2-x}$Bi$_x$Ru$_2$O$_7$ was investigated by neutron scattering and EXAFS. Pr has an approximate doublet ground-state and the first excited state is a singlet. This overall crystal field level scheme is similar to metallic Pr$_2$Ir$_2$O$_7$, which is also reported here. While the B-site (Ru) is well ordered throughout, this is not the case for the A-site (Pr/Bi). A distribution of the Pr-O2 bond length indicates the Pr environment is not uniform even for $x=0$. The Bi environment is highly disordered ostensibly due to the 6s lone pairs on Bi$^{3+}$. Correspondingly we find the non-Kramers doublet ground state degeneracy otherwise anticipated for Pr in the pyrochlore structure is lifted so as to produce a quadrupolar singlet ground state with a spatially varying energy gap. For $x=0$, below T$_N$, the Ru sublattice orders antiferromagnetically, with propagation vector \textbf{k}= (0,0,0), as for Y$_2$Ru$_2$O$_7$. No ordering associated with the Pr sublattice is observed down to 100 mK. The low energy magnetic response of Pr$_{2-x}$Bi$_x$Ru$_2$O$_7$ features a broad spectrum of magnetic excitations associated with inhomogeneous splitting of the Pr quasi-doublet ground state. For $x=0$ ($x=0.97$) the spectrum is temperature dependent (independent). It appears disorder associated with Bi alloying enhances the inhomogeneous Pr crystal field level splitting so that inter-site interactions become irrelevant for $x=0.97$. The structural complexity for the A-site may be reflected in the hysteretic uniform magnetization of B-site ruthenium in the Néel phase.

cond-mat.str-el↗

arXiv2014

Pressure Dependent Structural Changes and Predicted Electrical Polarization in Perovskite RMnO3

High pressure x-ray diffraction (XRD) measurements on RMnO3 (R=Dy, Ho and Lu) reveals that varying structural changes occurs for different R ions. Large lattice changes (orthorhombic strain) occur in DyMnO3 and HoMnO3 while the Jahn-Teller (JT) distortion remains stable. On the other hand, in LuMnO3, Mn-O bond distortions are observed in the region 4-8 GPa with the broad minimum in the JT distortion. High pressure IR measurements indicate that a phonon near 390 cm-1 corresponding to the complex motion of the Mn and O ions changes anomalously for LuMnO3. It softens in the 4-8 GPa region, which is consistent with the structural change in Mn-O bonds and then hardens at high pressures. By contrast, the phonons continuously harden with increasing pressure for DyMnO3 and HoMnO3. DFT calculations show that the E-phase LuMnO3 is the most stable phase up to the 10 GPa pressure examined. Simulations indicate that the distinct structural change under pressure in LuMnO3 can possibly be used to optimize the electric polarization by pressure/strain.

cond-mat.str-el↗

arXiv2014

Multiferroicity with coexisting isotropic and anisotropic spins in Ca$_{3}$Co$_{2-x}$Mn$_{x}$O$_{6}$

We study magnetic and multiferroic behavior in Ca$_3$Co$_{2-x}$Mn$_{x}$O$_6$ ($x \sim$0.97) by high-field measurements of magnetization ($M$), magnetostriction ($L$($H$)/$L$), electric polarization ($P$), and magnetocaloric effect. This study also gives insight into the zero and low magnetic field magnetic structure and magnetoelectric coupling mechanisms. We measured $M$ and $Δ$$L$/$L$ up to pulsed magnetic fields of 92 T, and determined the saturation moment and field. On the controversial topic of the spin states of Co$^{2+}$ and Mn$^{4+}$ ions, we find evidence for $S$ = 3/2 spins for both ions with no magnetic field-induced spin-state crossovers. Our data also indicate that Mn$^{4+}$ spins are quasi-isotropic and develop components in the $ab$-plane in applied magnetic fields of 10 T. These spins cant until saturation at 85 T whereas the Ising Co$^{2+}$ spins saturate by 25 T. Furthermore, our results imply that mechanism for suppression of electric polarization with magnetic fields near 10 T is flopping of the Mn$^{4+}$ spins into the $ab$-plane, indicating that appropriate models must include the coexistence of Ising and quasi-isotropic spins.

cond-mat.str-el↗

arXiv2013

Magnetic fan structures in Ba$_{0.5}$Sr$_{1.5}$Zn$_2$Fe$_{12}$O$_{22}$ hexaferrite revealed by resonant soft X-ray diffraction

The hexaferrites are known to exhibit a wide range of magnetic structures, some of which are connected to important technological applications and display magnetoelectric properties. We present data on the low field magnetic structures stabilised in a Y-type hexaferrite as observed by resonant soft X-ray diffraction. The helical spin block arrangement that is present in zero applied magnetic field becomes fan-like as a field is applied in plane. The propagation vectors associated with each fan structure are studied as a function of field, and a new magnetic phase is reported. Mean field calculations indicate this phase should stabilise close to the boundary of the previously reported phases.

cond-mat.str-el↗