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Henrik M. Rønnow

Publications and source records attributed to Henrik M. Rønnow.

At least 19 recordsLinked to original sources

Modified anisotropy and distinct phase diagrams in the nearly isotropic $S=1$ triangular-lattice antiferromagnet $\mathrm{Rb_2Ni(SeO_3)_2}$

The triangular-lattice antiferromagnet serves as a benchmark platform for realizing exotic quantum phases, in which magnetic anisotropy plays an essential role. In this work, we report modified magnetic anisotropy and phase diagrams in the nearly isotropic $S=1$ triangular-lattice antiferromagnet $\mathrm{Rb_2Ni(SeO_3)_2}$, compared with those of its isostructural analog $\mathrm{K_2Ni(SeO_3)_2}$. The magnetic susceptibility of $\mathrm{Rb_2Ni(SeO_3)_2}$ exhibits an easy-axis anisotropy with $g_c > g_{ab}$, opposite to the easy-plane anisotropy observed in $\mathrm{K_2Ni(SeO_3)_2}$. The single Néel transition observed at zero field splits into two transitions at around 10~T, and a magnetization plateau is observed between 21~T and 37~T for both out-of-plane ($H\parallel c$) and in-plane ($H\parallel ab$) field directions in $\mathrm{Rb_2Ni(SeO_3)_2}$. We construct magnetic phase diagrams that are distinct between $\mathrm{Rb_2Ni(SeO_3)_2}$ and $\mathrm{K_2Ni(SeO_3)_2}$. These findings highlight the sensitivity of field-induced magnetic phase behavior to anisotropy in nearly isotropic triangular-lattice antiferromagnets.

cond-mat.str-el↗

Single-ion anisotropy-stabilized short-period helimagnetism in frustrated chiral Co$_5$TeO$_8$

Chiral spin textures in magnetic insulators promise magneto-electric (ME) spintronics with orders-of-magnitude lower power consumption than metallic systems. However, realizing the short magnetic periods required for high-density device integration remains difficult, as conventional Dzyaloshinskii-Moriya interaction (DMI)-based mechanisms typically constrain spiral periods to tens of nanometers. While theory predicts that strong single-ion anisotropy (SIA) on frustrated lattices can stabilize complex non-coplanar textures, the potential for using this mechanism to engineer such compact textures remains largely unexplored. Here we report that a cubic chiral insulator Co$_5$TeO$_8$ provides an experimental example of this paradigm. Comprehensive neutron scattering and magnetometry reveal helimagnetic spirals with continuously tunable pitch of 5.7-10 nm embedded in a complex phase diagram spanning eight distinct phases. Capacitance anomalies throughout the phase diagram indicate magneto-electric coupling, pointing to the possibility of future $E$-field control of these textures. The temperature- and field-dependence of the helical wavevector strongly support a scenario in which site-dependent SIA provides the leading contribution to the selection of the helical period from a frustration-induced degenerate manifold. Consistent with this interpretation, $ab\,initio$ calculations place SIA approximately an order of magnitude above DMI, distinct from conventional helimagnets. Co$_5$TeO$_8$ thus offers an experimental realization of sub-10 nm helimagnetism and motivates a design principle for anisotropy-engineered correlated insulators.

cond-mat.str-el↗

Photostationary Lifshitz transition in High Tc superconductor Bi2Sr2CaCu2O8+δ

To date, controlling the steady-state electronic band structure in high-Tc cuprate superconductors has been achieved primarily through chemical doping or magnetic fields. Here, we present that ultrafast optical excitation can instead drive the electronic band structure of Bi2Sr2CaCu2O8+δ into a photostationary, long-lived excited state. At sufficiently high pump fluences, this state undergoes a Lifshitz transition of the Fermi surface, characterized by a change in topology from hole-like to electron-like. Time- and angle-resolved photoemission spectroscopy, supported by single-band tight-binding calculations, reveals that 1.6 eV photoexcitation induces band-structure evolutions closely analogous to those produced by chemical doping. These results point to an efficient photodoping mechanism involving cooperative effects, including charge transfer, renormalization of effective electronic correlations, and defect-assisted charge trapping. Our findings raise fundamental questions regarding thermalization processes occurring on timescales comparable to the laser repetition period in cuprates. More broadly, ultrafast optical control enables access to otherwise inaccessible regions of the phase diagram by tuning the pump fluence.

cond-mat.str-el↗

Probing the real-space density of spin-entangled electrons

On the textbook example of an isolated antiferromagnetic Heisenberg dimer, we demonstrate that the magnetic form factor and the magnetic electron density distribution can be extracted from the momentum-dependence of the inelastic neutron scattering (INS) intensity of a magnetic excitation. We measure the three-dimensional (3D) magnetic structure factor of the singlet-to-triplet excitation in Cu(II) acetate monohydrate with INS. Using a minimal parametrization of the magnetic electron density, we deduce the real-space density of the spin-entangled electrons and the transfer of magnetic electron density between metal and ligand atoms from the experimental data. Density functional theory (DFT) calculations reproduce the measured structure factor quantitatively, providing a direct validation of DFT broken-symmetry spin densities against full 3D INS data. The quantitative agreement between experiment, parametrization, and theory establishes a robust framework for determining magnetic form factors and the magnetic electron density in a broad range of magnetic materials and demonstrates INS as a probe of the envelope of spatial electronic wavefunctions.

cond-mat.str-el↗

Nuclear quadrupole interaction and zero first-order Zeeman transitions of $^{167}$Er$^{3+}$ in CaWO$_4$

We report microwave spectroscopy of $^{167}$Er$^{3+}$ doped in CaWO$_4$ which reveals the hyperfine splitting of the erbium electronic ground state ($Z_1$, $J_\mathrm{eff.}$=15/2) induced by the $I$=7/2 nuclear spin. From spectra measured below$\sim$50 mK in magnetic fields up to 200 mT, we extract spin Hamiltonian parameters including the electron $\textbf{g}$, hyperfine $\textbf{A}$, and nuclear electric quadrupolar $\textbf{Q}$ tensors. Crucially, our analysis demonstrate unambiguously, that the previously unobserved nuclear electric quadrupolar moment is essential to reproduce the experimental data. With these refined parameters, we identify zero first-order Zeeman (ZEFOZ) transitions at zero magnetic field. Extending the analysis to finite fields, we uncover that ZEFOZ points lie either along the $c$ axis or within the $a$-$b$ plane. These results establish CaWO$_4$ as a promising host for long lifetime quantum memories.

cond-mat.mtrl-sci↗

Approximate resolution convolution function for fitting a dispersion gap measured on a triple-axis spectrometer

We present an analytic convoluted-gap function, eq. 11 in the manuscript, for fitting dispersion gaps measured on triple-axis spectrometers (TAS). At the gap, the instrumental resolution skews the signal, producing a high-energy tail that complicates fitting. Our function assumes an instrumental $Q$-resolution with two equal wide and one narrow direction (typical of focused TAS instruments), and a parabolic dispersion at the gap, which is exact for quadratic and accurate for linear dispersions if the resolution is moderate. We demonstrate, that our function outperforms previous methods of fitting a gap, by giving a better fit and more accurate gap determination, seen in figure 4. Here, the anti-ferromagnetically gapped material; MnF$_2$ is simulated in a double-focusing TAS instrument. We also tested our function on experimental data on MnF$_2$ from a TAS-like instrument, where we reproduce the gap size from previous accurate experimentally determined measurements. The function is simple to implement, converges reliably, and we recommend its use for future gap fitting on TAS data.

physics.ins-det↗

Optical spectroscopy of single- and two-ion transitions in an antiferromagnetic stoichiometric rare-earth crystal

We characterise optical transitions of neodymium ions (Nd3+) in antiferromagnetic neodymium gallate (NdGaO3) with applied fields up to 3 T. The magnetic phase of this material has not previously been studied with the field along its magnetisation axis. The measured optical spectra indicate three magnetic phases -- antiferromagnetic, intermediate, and paramagnetic -- where the intermediate phase likely forms a different magnetic structure from typical spin-flop phases. The observed absorptions were classified into two distinct families of optical transitions: single-Nd and two-Nd absorptions. We demonstrate that the optical transitions in the antiferromagnetic and paramagnetic phases can be modelled using a standard single-ion crystal-field Hamiltonian that interacts with a mean magnetisation from the rest of the lattice, and we expand that model to encompass pairs of ions, explaining the origins of the two-Nd transitions. This study offers a deeper understanding of the optical transitions in rare-earth antiferromagnetic crystals, which have been recently attracting significant interest for microwave-to-optical quantum transduction, despite being relatively unexplored to date.

quant-ph↗

Coexistence of insulator-like paramagnon and metallic spin-orbit exciton modes in SrIrO$_3$

We probe the spectrum of elementary excitations in SrIrO$_3$ by using heterostructured [(SrIrO$_3$)$_m$/(SrTiO$_3$)$_l$] samples to approach the bulk limit. Our resonant inelastic x-ray scattering (RIXS) measurements at the Ir $L_3$-edge reveal a robust low-lying collective magnetic mode with an antiferromagnetic (AF) dispersion similar to the insulators Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, albeit with a large gap and much larger linewidth. At higher energies we find the spin-orbit exciton, also strongly broadened, but with an inverted dispersion and doubled periodicity that are controlled by the charge hopping. These results demonstrate that the AF paramagnon persists, somewhat counterintuitively, far into the metallic regime of the insulator-metal transition driven by the degree of confinement in the heterostructure. We conclude that these two excitations, which are contrasting but coexisting hallmarks of strong AF pseudospin and charge fluctuations in a spin-orbit-coupled Mott-Slater material, are properties intrinsic to the ground state of semimetallic perovskite SrIrO$_3$.

cond-mat.str-el↗

Refined spin Hamiltonian on the Cairo pentagonal lattice of Bi2Fe4O9

The frustrated magnet Bi2Fe4O9 has been reported to exhibit complex spin dynamics coexisting with conventional spin wave excitations. The magnetic Fe3+ (S = 5/2) ions are arranged into a distorted two-dimensional Cairo pentagonal lattice with weak couplings between the layers, developing long-ranged non-collinear antiferromagnetic order below 245 K. In order to enable studies and modelling of the complex dynamics close to TN, we have reexamined the magnetic excitations across the complete energy scale (0 < E < 90 meV) at 10 K. We discover two distinct gaps, which can be explained by introducing, respectively, easy axis and easy plane anisotropy on the two unequivalent Fe-sites. We develop a refined spin Hamiltonian that accurately accounts for the dispersion of essentially all spin-wave branches across the full spectral range, except around 40 meV, where a splitting and dispersion are observed. We propose that this mode is derived from phonon hybridization. Polarisation analysis shows that the system has magnetic anisotropic fluctuations, consistent with our model. A continuum of scattering is observed above the spin wave branches and is found to principally be explained by an instrumental resolution effect. The full experimental mapping of the excitation spectrum and the refined spin Hamiltonian provides a foundation for future quantitative studies of spin waves coexisting with unconventional magnetic fluctuations in this frustrated magnet found at higher temperatures.

cond-mat.str-el↗

Confinement, deconfinement, and bound states in the spin-$1$ and spin-$3/2$ generalizations of the Majumdar--Ghosh chain

We investigate the nature of low-energy excitations in a spin chain with antiferrmomagnetic nearest-neighbor $J_1$, next-nearest-neighbor $J_2$, and three-site $J_3$ interactions using the time-dependent density matrix renormalization group and the single mode approximation techniques. In the absence of the $J_2$ interaction, we identify clear distinctions in the spectral functions in the fully dimerized phase across the exactly dimerized line for different magnitudes of the spins. In contrast to the spin-$1/2$ chain, where the spinon continuum dominates the spectral functions, the magnon modes are prominent in the spectral functions of the spin-$1$ and spin-$3/2$ chains. Through single mode approximation and valence bond solid approaches, we disentangle magnon and spinon contributions to the spectral functions. After including the $J_2$ interactions, for the spin-$1$ chain we trace the evolution of the dynamical structure factor along the phase transition line between the Haldane phase and the fully dimerized phase. We find that the excitation spectrum is a continuum along this line and the spectral gap closes as the order of the transition changes from first order to second order. Along the line of first-order transitions, the spinon-like domain walls are deconfined, and the model exhibits their confinement into discrete bound states away from the transition line. A similar phenomenon occurs in the spin-$3/2$ chain across the phase transition between partially dimerized to fully dimerized phases, revealing a universal spinon confinement phenomenon across first-order phase transitions. This study presents the dynamical structure factor corresponding to the ground state phase diagram and establishes a unified quasiparticle framework for understanding the fundamental nature of excitations across distinct quantum phases in frustrated $J_1$-$J_2$-$J_3$ Heisenberg spin chains.

cond-mat.str-el↗

Short-wave magnons with multipole spin precession detected in the topological bands of a skyrmion lattice

Topological magnon bands enable uni-directional edge transport without backscattering, enhancing the robustness of magnonic circuits and providing a novel platform for exploring quantum transport phenomena. Magnetic skyrmion lattices, in particular, host a manifold of topological magnon bands with multipole character and non-reciprocal dispersions. These modes have been explored already in the short and long wavelength limit, but previously employed techniques were unable to access intermediate wavelengths comparable to inter-skyrmion distances. Here, we report the detection of such magnons with wavevectors $|{\bf q}|\simeq 48$ rad $μ$m$^{-1}$ in the metastable skyrmion lattice phase of the bulk chiral magnet Cu$_2$OSeO$_3$ using Brillouin light scattering microscopy. Thanks to its high sensitivity and broad bandwidth various multipole excitation modes could be resolved over a wide magnetic field regime. Besides the known counterclockwise, breathing and clockwise modes with dipole character, quantitative comparison of frequencies and spectral weights to theoretical predictions enabled the additional identification of a quadrupole mode and, possibly, a sextupole mode. Our work highlights the potential of skyrmionic phases for the design of magnonic devices exploiting topological magnon states at GHz frequencies.

cond-mat.mes-hall↗

Bullet pressure-cell design for neutron scattering experiments with horizontal magnetic fields and dilution temperatures

The simultaneous application of high magnetic fields and high pressures for controlling magnetic ground states is important for testing our understanding of many-body quantum theory. However, the implementation for neutron scattering experiments presents a technical challenge. To overcome this challenge we present an optimized pressure-cell design with a novel bullet shape, which is compatible with horizontal-field magnets, in particular the high-field magnet operating at the Helmholtz-Zentrum Berlin. The cell enabled neutron diffraction and spectroscopy measurements with the combination of three extreme conditions: high pressures, high magnetic fields, and dilution temperatures, simultaneously reaching 0.7 GPa, 25.9 T, and 200 mK. Our results demonstrate the utility of informed material choices and the efficiency of finite-element analysis for future pressure-cell designs to be used in combination with magnetic fields and dilution temperatures for neutron scattering purposes.

cond-mat.str-el↗

Bound states and deconfined spinons in the dynamical structure factor of the $J_1 - J_2$ spin-1 chain

Using a time-dependent density matrix renormalization group approach, we study the dynamical structure factor of the $J_1 - J_2$ spin-1 chain. As $J_2$ increases, the magnon mode develops incommensurability. The system undergoes a first-order transition at $J_2 = 0.76 J_1$, and at that point, domain walls lead to a continuum of fractional quasi-particles or spinons. By studying small variations in $J_2$ around the transition point, we observe the confinement of spinons into bound states in the spectral function and find a smooth evolution of the spectrum into magnon modes away from the phase transition. We employ the single-mode approximation to accurately account for the dispersion of the magnon mode away from the phase transition and describe the associated continua and bound states. We extend the single-mode approximation to describe the dispersion of a spinon at the phase transition point and obtain its dispersion throughout the Brillouin zone. This allows us to relate the incommensurability at and around the transition point to the competition between a negative nearest-neighbour hopping amplitude and a positive next-nearest-neighbour one for the domain wall.

cond-mat.str-el↗

High-resolution MHz time- and angle-resolved photoemission spectroscopy based on a tunable vacuum ultraviolet source

Time and angle-resolved photoemission spectroscopy (trARPES) allows direct mapping of the electronic band structure and its dynamic response on femtosecond timescales. Here, we present a new ARPES system, powered by a new fiber-based femtosecond light source in the vacuum ultraviolet (VUV) range, accessing the complete first Brillouin zone for most materials. We present trARPES data on Au(111), polycrystalline Au, Bi2Se3 and TaTe2, demonstrating an energy resolution of 21 meV with a time resolution of <360 fs, at a high repetition rate of 1 MHz. The system is integrated with an extreme ultraviolet (EUV) high harmonic generation (HHG) beamline, enabling excellent tunability of the time-bandwidth resolution.

physics.ins-det↗

A compact approach to higher-resolution resonant inelastic X-ray scattering detection using photoelectrons

The detection of inelastically scattered soft X-rays with high energy resolution usually requires large grating spectrometers. Recently, photoelectron spectrometry for analysis of X-rays (PAX) has been rediscovered for modern spectroscopy experiments at synchrotron light sources. By converting scattered photons to electrons and using an electron energy analyser, the energy resolution for resonant inelastic X-ray scattering (RIXS) becomes decoupled from the X-ray spot size and instrument length. In this work, we develop PAX towards high energy resolution using a modern photoemission spectroscopy setup studying Ba2Cu3O4Cl2 at the Cu L3-edge. We measure a momentum transfer range of 24% of the first Brillouin zone simultaneously. Our results hint at the observation of a magnon excitation below 100 meV energy transfer and show intensity variations related to the dispersion of dd-excitations. With dedicated setups, PAX can become an alternative to the best and largest RIXS instruments, while at the same time opening new opportunities to acquire RIXS at a range of momentum transfers simultaneously and combine it with angle-resolved photoemission spectroscopy in a single instrument.

cond-mat.mtrl-sci↗

Kapitza stabilization of quantum critical order

Dynamical perturbations modify the states of classical systems in surprising ways and give rise to important applications in science and technology. For example, Floquet engineering exploits the possibility of band formation in the frequency domain when a strong, periodic variation is imposed on parameters such as spring constants. We describe here Kapitza engineering, where a drive field oscillating at a frequency much higher than the characteristic frequencies for the linear response of a system changes the potential energy surface so much that maxima found at equilibrium become local minima, in precise analogy to the celebrated Kapitza pendulum where the unstable inverted configuration, with the mass above rather than below the fulcrum, actually becomes stable. Our starting point is a quantum field theory of the Ginzburg-Devonshire type, suitable for many condensed matter systems, including particularly ferroelectrics and quantum paralectrics. We show that an off-resonance oscillatory electric field generated by a laser-driven THz source can induce ferroelectric order in the quantum-critical limit. Heating effects are estimated to be manageable using pulsed radiation; ``hidden" radiation-induced order can persist to low temperatures without further pumping due to stabilization by strain. We estimate the Ginzburg-Devonshire free-energy coefficients in SrTiO${}_{3}$ using density-functional theory (DFT) and the stochastic self-consistent harmonic approximation accelerated by a machine-learned force field. Although we find that SrTiO${}_{3}$ is not an optimal choice for Kapitza stabilization, we show that scanning for further candidate materials can be performed at the computationally convenient density-functional theory level. We suggest second-harmonic-generation, soft-mode-spectroscopy, and X-ray-diffraction experiments to characterize the induced order.

cond-mat.str-el↗

Spectroscopic signatures and origin of a hidden order in Ba$_2$MgReO$_6$

Clarifying the underlying mechanisms that govern ordering transitions in condensed matter systems is crucial for comprehending emergent properties and phenomena. While transitions are often classified as electronically driven or lattice-driven, we present a departure from this conventional paradigm in the case of the double perovskite Ba$_2$MgReO$_6$. Leveraging resonant and non-resonant elastic x-ray scattering techniques, we unveil the simultaneous ordering of structural distortions and charge quadrupoles at a critical temperature of $T_\mathrm{q}$$\sim$33 K. Using a variety of complementary first-principles-based computational techniques, we demonstrate that while electronic interactions drive the ordering at $T_\mathrm{q}$, it is ultimately the lattice that dictates the specific ground state that emerges. Our findings highlight the crucial interplay between electronic and lattice degrees of freedom, providing a unified framework to understand and predict unconventional emergent phenomena in quantum materials.

cond-mat.str-el↗

Structure, spin correlations and magnetism of the $S = 1/2$ square-lattice antiferromagnet Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ ($0 \leq x \leq 1$)

Quantum spin liquids are highly entangled magnetic states with exotic properties. The $S = 1/2$ square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are physical realizations of this model, but have distinctly different types magnetic order and interactions due to a $d^{10}/d^0$ effect. Long-range magnetic order is suppressed in the solid solution Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ in a wide region of $x = 0.05-0.6$, where the ground state has been proposed to be a disorder-induced spin liquid. Here we show that the spin-liquid-like $x = 0.2$ and $x = 0.5$ samples have distinctly different local spin correlations, which suggests they have different ground states. Furthermore, the previously ignored interlayer coupling between the square-planes is likely to play a role in the suppression of magnetic order on the W-rich side at $x \approx 0.6$. These results highlight the complex magnetism of Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ and hint at a new quantum critical point at $x \approx 0.3$.

cond-mat.str-el↗