arXiv subjects

H. M. Rønnow

Publications and source records attributed to H. M. Rønnow.

At least 55 records · Page 3Linked to original sources

arXiv2017

$J_1$-$J_2$ square lattice antiferromagnetism in the orbitally quenched insulator MoOPO$_4$

We report magnetic and thermodynamic properties of a $4d^1$ (Mo$^{5+}$) magnetic insulator MoOPO$_4$ single crystal, which realizes a $J_1$-$J_2$ Heisenberg spin-$1/2$ model on a stacked square lattice. The specific-heat measurements show a magnetic transition at 16 K which is also confirmed by magnetic susceptibility, ESR, and neutron diffraction measurements. Magnetic entropy deduced from the specific heat corresponds to a two-level degree of freedom per Mo$^{5+}$ ion, and the effective moment from the susceptibility corresponds to the spin-only value. Using {\it ab initio} quantum chemistry calculations we demonstrate that the Mo$^{5+}$ ion hosts a purely spin-$1/2$ magnetic moment, indicating negligible effects of spin-orbit interaction. The quenched orbital moments originate from the large displacement of Mo ions inside the MoO$_6$ octahedra along the apical direction. The ground state is shown by neutron diffraction to support a collinear Néel-type magnetic order, and a spin-flop transition is observed around an applied magnetic field of 3.5 T. The magnetic phase diagram is reproduced by a mean-field calculation assuming a small easy-axis anisotropy in the exchange interactions. Our results suggest $4d$ molybdates as an alternative playground to search for model quantum magnets.

cond-mat.str-el↗

arXiv2017

Direct control of the skyrmion phase stability by electric field in a magnetoelectric insulator

Magnetic skyrmions are topologically protected spin-whirl quasiparticles currently considered as promising components for ultra-dense memory devices. In the bulk they form lattices that are stable over just a few Kelvin below the ordering temperature. This narrow stability range presents a key challenge for applications, and finding ways to tune the SkL stability over a wider phase space is a pressing issue. Here we show experimentally that the skyrmion phase in the magnetoelectric insulator ${\text{Cu}_2 \text{O} \text{Se} \text{O}_3}$ can either expand or shrink substantially depending on the polarity of a moderate applied electric field. The data are well-described by an expanded mean-field model with fluctuations that show how the electric field provides a direct control of the free energy difference between the skyrmion and the surrounding conical phase. Our finding of the direct electric field control of the skyrmion phase stability offers enormous potential for skyrmionic applications based on a magnetoelectric coupling.

cond-mat.other↗

arXiv2016

Probing strongly hybrid nuclear-electronic states in a model quantum ferromagnet

We present direct local-probe evidence for strongly hybridized nuclear-electronic spin states of an Ising ferromagnet LiHoF$_4$ in a transverse magnetic field. The nuclear-electronic states are addressed via a magnetic resonance in the GHz frequency range using coplanar resonators and a vector network analyzer. The magnetic resonance spectrum is successfully traced over the entire field-temperature phase diagram, which is remarkably well reproduced by mean-field calculations. Our method can be directly applied to a broad class of materials containing rare-earth ions for probing the substantially mixed nature of the nuclear and electronic moments.

cond-mat.str-el↗

arXiv2016

Magnetic excitations and electronic interactions in Sr$_2$CuTeO$_6$: a spin-1/2 square lattice Heisenberg antiferromagnet

Sr$_2$CuTeO$_6$ presents an opportunity for exploring low-dimensional magnetism on a square lattice of $S=1/2$ Cu$^{2+}$ ions. We employ ab initio multi-reference configuration interaction calculations to unravel the Cu$^{2+}$ electronic structure and to evaluate exchange interactions in Sr$_2$CuTeO$_6$. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr$_2$CuTeO$_6$ is an almost realization of a nearest-neighbor Heisenberg antiferromagnet but with relatively weak coupling of 7.18(5) meV.

cond-mat.str-el↗

arXiv2016

Phase diagram of diluted Ising ferromagnet LiHo$_x$Y$_{1-x}$F$_4$

We present a systematic study of the phase diagram of LiHo$_x$Y$_{1-x}$F$_4$ ($0.25<x<1$) Ising ferromagnets obtained from neutron scattering measurements and mean-field calculations. We show that while the thermal phase transition decreases linearly with dilution, as predicted by mean-field theory, the critical transverse field at the quantum critical point is suppressed much faster. This behavior is related to competition between off-diagonal dipolar coupling and quantum fluctuations that are tuned by doping and applied field, respectively. In this paper, we quantify the deviation of the experimental results from mean-field predictions, with the aim that this analysis can be used in future theoretical efforts towards a quantitative description.

cond-mat.str-el↗

arXiv2016

Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$(M = Ir, Rh): A family of 5\textit{\textcolor{black}{d}}/4\textit{\textcolor{black}{d}}-based, diluted quantum spin liquids

We report the structural and magnetic properties of the 4}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Rh) based and 5}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Ir) based systems Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$ (nominally $x$ = 0.5, 1). The studied compositions were found to crystallize in a hexagonal structure with the centrosymmetric space group }$P6_{3}/mmc$.\textcolor{black}{{} The structures comprise of A$_{2}$O$_{9}$ polyhedra (with the A site (possibly) statistically occupied by M and Ti) in which pairs of transition metal ions are stacked along the crystallographic }\textit{\textcolor{black}{c}}\textcolor{black}{-axis. These pairs form triangular bilayers in the $ab$-plane. The magnetic Rh and Ir ions occupy these bilayers, diluted by Ti ions even for $x$ = 1. These bilayers are separated by a triangular layer which is dominantly occupied by Ti ions. From magnetization measurements we infer strong antiferromagnetic couplings for all of the materials but the absence of any spin-freezing or spin-ordering down to 2~K. Further, specific heat measurements down to 0.35~K show no sign of a phase transition for any of the compounds. Based on these thermodynamic measurements we propose the emergence of a quantum spin liquid ground state for Ba$_{3}$Rh$_{0.5}$Ti$_{2.5}$O$_{9}$, and Ba$_{3}$Ir$_{0.5}$Ti$_{2.5}$O$_{9}$, in addition to the already reported Ba$_{3}$IrTi$_{2}$O$_{9}$. }

cond-mat.str-el↗

arXiv2016

Magnetodielectric detection of magnetic quadrupole order in Ba(TiO)Cu$_4$(PO$_4$)$_4$ with Cu$_4$O$_{12}$ square cupolas

In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal, monopole, and quadrupole moments. So far, however, the ME-activity of these multipole moments has only been established experimentally for the toroidal moment. Here, we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu$_4$(PO$_4$)$_4$. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.

cond-mat.str-el↗

arXiv2016

Possibility of an unconventional spin state of Ir$^{4+}$ in Ba$_{21}$Ir$_9$O$_{43}$ single crystal

We report the synthesis of single crystals of a novel layered iridate Ba$_{21}$Ir$_9$O$_{43}$, and present the crystallographic, transport and magnetic properties of this material. The compound has a hexagonal structure with two iridium oxide layers stacked along the $c$ direction. One layer consists of a triangular arrangement of Ir$_2$O$_9$ dimers while the other layer comprises two regular octahedra and one triangular pyramid, forming inter-penetrated triangular lattices. The resistivity as a function of temperature exhibits an insulating behavior, with a peculiar $T^{-3}$ behavior. Magnetic susceptibility shows antiferromagnetic Curie-Weiss behavior with $Θ_\mathrm{CW} \simeq -$90 K while a magnetic transition occurs at substantially lower temperature of 9 K. We discuss possible valence states and effective magnetic moments on Ir ions in different local environments, and argue that the Ir ions in a unique triangular-pyramidal configuration likely carry unusually large magnetic moments.

cond-mat.str-el↗

arXiv2016

Robust metastable skyrmions and their triangular-square lattice-structural transition in a high-temperature chiral magnet

Skyrmions, topologically-protected nanometric spin vortices, are being investigated extensively in various magnets. Among them, many of structurally-chiral cubic magnets host the triangular-lattice skyrmion crystal (SkX) as the thermodynamic equilibrium state. However, this state exists only in a narrow temperature and magnetic-field region just below the magnetic transition temperature $T_\mathrm{c}$, while a helical or conical magnetic state prevails at lower temperatures. Here we describe that for a room-temperature skyrmion material, $β$-Mn-type Co$_8$Zn$_8$Mn$_4$, a field-cooling via the equilibrium SkX state can suppress the transition to the helical or conical state, instead realizing robust metastable SkX states that survive over a very wide temperature and magnetic-field region, including down to zero temperature and up to the critical magnetic field of the ferromagnetic transition. Furthermore, the lattice form of the metastable SkX is found to undergo reversible transitions between a conventional triangular lattice and a novel square lattice upon varying the temperature and magnetic field. These findings exemplify the topological robustness of the once-created skyrmions, and establish metastable skyrmion phases as a fertile ground for technological applications.

cond-mat.str-el↗

arXiv2016

Pressure dependence of the structure and electronic properties of Sr3Ir2O7

We study the structural evolution of Sr$_3$Ir$_2$O$_7$ as a function of pressure using x-ray diffraction. At a pressure of 54 GPa at room temperature, we observe a first-order structural phase transition, associated with a change from tetragonal to monoclinic symmetry, and accompanied by a 4% volume collapse. Rietveld refinement of the high-pressure phase reveals a novel modification of the Ruddlesden-Popper structure, which adopts an altered stacking sequence of the perovskite bilayers. As the positions of the oxygen atoms could not be reliably refined from the data, we use density functional theory (local-density approximation+$U$+spin orbit) to optimize the crystal structure, and to elucidate the electronic and magnetic properties of Sr$_3$Ir$_2$O$_7$ at high pressure. In the low-pressure tetragonal phase, we find that the in-plane rotation of the IrO$_6$ octahedra increases with pressure. The calculations further indicate that a bandwidth-driven insulator-metal transition occurs at $\sim$20 GPa, along with a quenching of the magnetic moment. In the high-pressure monoclinic phase, structural optimization resulted in complex tilting and rotation of the oxygen octahedra, and strongly overlapping $t_{2g}$ and $e_g$ bands. The $t_{2g}$ bandwidth renders both the spin-orbit coupling and electronic correlations ineffectual in opening an electronic gap, resulting in a robust metallic state for the high-pressure phase of Sr$_3$Ir$_2$O$_7$.

cond-mat.str-el↗

arXiv2016

Dimensional Reduction in Quantum Dipolar Antiferromagnets

We report ac susceptibility, specific heat, and neutron scattering measurements on a dipolar-coupled antiferromagnet LiYbF$_4$. For the thermal transition, the order-parameter critical exponent is found to be 0.20(1) and the specific-heat critical exponent -0.25(1). The exponents agree with the 2D XY/h$_4$ universality class despite the lack of apparent two-dimensionality in the structure. The order-parameter exponent for the quantum phase transitions is found to be 0.35(1) corresponding to (2+1)D. These results are in line with those found for LiErF$_4$ which has the same crystal structure, but largely different T$_N$, crystal field environment and hyperfine interactions. Our results therefore experimentally establish that the dimensional reduction is universal to quantum dipolar antiferromagnets on a distorted diamond lattice.

cond-mat.str-el↗

arXiv2016

Converse effect of pressure on quadrupolar and magnetic transition in Ce$_{3}$Pd$_{20}$Si$_{6}$

The heavy fermion compound Ce$_{3}$Pd$_{20}$Si$_{6}$ displays unconventional quantum criticality as the lower of two consecutive phase transitions is fully suppressed by magnetic field. Here we report on the effects of pressure as additional tuning parameter. Specific heat and electrical resistivity measurements reveal a converse effect of pressure on the two transitions, leading to the merging of both transitions at 6.2 kbar. The field-induced quantum criticality is robust under pressure tuning. We rationalize our findings within an extended version of the global phase diagram for antiferromagnetic heavy fermion quantum criticality.

cond-mat.str-el↗

arXiv2015

Dramatic pressure-driven enhancement of bulk skyrmion stability

The recent discovery of magnetic skyrmion lattices initiated a surge of interest in the scientific community. Several novel phenomena have been shown to emerge from the interaction of conducting electrons with the skyrmion lattice, such as a topological Hall-effect and a spin-transfer torque at ultra-low current densities. In the insulating compound Cu2OSeO3, magneto-electric coupling enables control of the skyrmion lattice via electric fields, promising a dissipation-less route towards novel spintronic devices. One of the outstanding fundamental issues is related to the thermodynamic stability of the skyrmion lattice. To date, the skyrmion lattice in bulk materials has been found only in a narrow temperature region just below the order-disorder transition. If this narrow stability is unavoidable, it would severely limit applications. Here we present the discovery that applying just moderate pressure on Cu2OSeO3 substantially increases the absolute size of the skyrmion pocket. This insight demonstrates directly that tuning the electronic structure can lead to a significant enhancement of the skyrmion lattice stability. We interpret the discovery by extending the previously employed Ginzburg-Landau approach and conclude that change in the anisotropy is the main driver for control of the size of the skyrmion pocket. This realization provides an important guide for tuning the properties of future skyrmion hosting materials.

cond-mat.str-el↗

arXiv2015

Sc_{2}Ga_{2}CuO_{7}: A possible Quantum spin liquid near the percolation threshold

Sc$_{2}$Ga$_{2}$CuO$_{7}$ (SGCO) crystallizes in a hexagonal structure (space group: $P$$6$$_{3}/mmc$),\textcolor{black}{{} which can be seen as an alternating stacking of single and double triangular layers. Combining neutron, x-ray, and resonant x-ray diffraction we establish that the single triangular layers are mainly populated by non-magnetic Ga$^{3+}$ ions (85\% Ga and 15\% Cu), while the bi-layers have comparable population of Cu$^{2+}$ and Ga$^{3+}$} ions \textcolor{black}{(43\% Cu and 57\% Ga)}. Our susceptibility measurements in the temperature range 1.8 - 400 K give no indication of any spin-freezing or magnetic long-range order (LRO). We infer an effective paramagnetic moment $μ_{eff}=1.79\pm0.09$ $μ_{B}$ and a Curie-Weiss temperature $θ_{CW}$ of about $-44$ K, suggesting antiferromagnetic interactions between the Cu$^{2+}$($S=1/2$) ions. Low-temperature neutron powder diffraction data showed no evidence for LRO down to 1.5 K. In our specific heat data as well, no anomalies were found down to 0.35 K, in the field range 0-140 kOe.\textcolor{black}{{} The magnetic specific heat, $C_{m}$, exhibits a broad maximum at around 2.5 K followed by a nearly power law $C$$_{m}$$\propto$ $T$$^α$ behavior at lower temperatures, with $α$ increasing from }0.3\textcolor{black}{{} to} 1.9\textcolor{black}{{} as a function of field for fields upto 90 kOe and then remaining at 1.9 for fields upto 140 kOe. Our results point to a disordered ground state in SGCO. }

cond-mat.str-el↗

arXiv2015

Neutron spectroscopic study of crystal-field excitations and the effect of the crystal field on dipolar magnetism in Li$R$F$_4$ ($R$ = Gd, Ho, Er, Tm, and Yb)

We present a systematic study of the crystal field interactions in the Li$R$F$_4$, $R$ = Gd, Ho, Er, Tm and Yb, family of rare-earth magnets. Using detailed inelastic neutron scattering measurements we have been able to quantify the transition energies and wavefunctions for each system. This allows us to quantitatively describe the high-temperature susceptibility measurements for the series of materials and make predictions based on a mean-field approach for the low-temperature thermal and quantum phase transitions. We show that coupling between crystal field and phonon states leads to lineshape broadening in LiTmF$_4$ and level splitting in LiYbF$_4$. Furthermore, using high resolution neutron scattering from LiHoF$_4$, we find anomalous broadening of crystal-field excitations which we attribute to magnetoelastic coupling.

cond-mat.str-el↗

arXiv2015

Quantum Critical Scaling for a Heisenberg Spin-$1/2$ Chain around Saturation

We demonstrate quantum critical scaling for an $S=1/2$ Heisenberg antiferromagnetic chain compound CuPzN in a magnetic field around saturation, by analysing previously reported magnetization [Y. Kono {\it et al.}, Phys. Rev. Lett. {\bf 114}, 037202 (2015)], thermal expansion [J. Rohrkamp {\it et al.}, J. Phys.: Conf. Ser. {\bf 200}, 012169 (2010)] and NMR relaxation data [H. Kühne {\it et al.}, Phys. Rev. B {\bf 80}, 045110 (2009)]. The scaling of magnetization is demonstrated through collapsing the data for a range of both temperature and field onto a single curve without making any assumption for a theoretical form. The data collapse is subsequently shown to closely follow the theoretically-predicted scaling function without any adjustable parameters. Experimental boundaries for the quantum critical region could be drawn from the variable range beyond which the scaled data deviate from the theoretical function. Similarly to the magnetization, quantum critical scaling of the thermal expansion is also demonstrated. Further, the spin dynamics probed via NMR relaxation rate $1/T_1$ close to the saturation is shown to follow the theoretically-predicted quantum critical behavior as $1/T_1\propto T^{-0.5}$ persisting up to temperatures as high as $k_\mathrm{B}T \simeq J$, where $J$ is the exchange coupling constant.

cond-mat.str-el↗

arXiv2015

Investigation of the Magnetic Model in Multiferroic NdFe$_{3}$(BO$_{3}$)$_{4}$ by Inelastic Neutron Scattering

We performed inelastic neutron scattering measurements on single crystals of NdFe$_{3}$($^{11}$BO$_{3}$)$_{4}$ to explore the magnetic excitations, to establish the underlying Hamiltonian, and to reveal the detailed nature of hybridization between the 4$f$ and 3$d$ magnetism. The observed spectra exhibiting a couple of key features, i.e., anti-crossing of Nd- and Fe-excitations and anisotropy gap at the antiferromagnetic zone center, are explained by the magnetic model including spin interaction in the framework of weakly-coupled Fe$^{3+}$ chains, interaction between the Fe$^{3+}$ and Nd$^{3+}$ moments, and single-ion anisotropy derived from Nd$^{3+}$ crystal field. The combination of the measurements and calculations reveals that the hybridization between 4$f$ and 3$d$ magnetism propagates the local magnetic anisotropy of the Nd$^{3+}$ ion to the Fe$^{3+}$ network, resulting in the bulk structure of multiferroics.

cond-mat.str-el↗

arXiv2015

Filming the formation and fluctuation of Skyrmion domains by cryo-Lorentz Transmission Electron Microscopy

Magnetic skyrmions are promising candidates as information carriers in logic or storage devices thanks to their robustness, guaranteed by the topological protection, and their nanometric size. Currently, little is known about the influence of parameters such as disorder, defects or external stimuli, on the long-range spatial distribution and temporal evolution of the skyrmion lattice. Here, using a large (7.3x7.3μm$^{2}$) single crystal nano-slice of Cu$_{2}$OSeO$_{3}$, we image up to 70,000 skyrmions, by means of cryo-Lorentz Transmission Electron Microscopy as a function of the applied magnetic field. The emergence of the skyrmion lattice from the helimagnetic phase is monitored, revealing the existence of a glassy skyrmion phase at the phase transition field, where patches of an octagonally distorted skyrmion lattice are also discovered. In the skyrmion phase, dislocations are shown to cause the emergence and switching between domains with different lattice orientations and the temporal fluctuations of these domains is filmed. These results demonstrate the importance of direct-space and real-time imaging of skyrmion domains for addressing both their long-range topology and stability.

cond-mat.mes-hall↗