arXiv subjects

S. T. Bramwell

Publications and source records attributed to S. T. Bramwell.

At least 19 recordsLinked to original sources

arXiv2024

Power spectrum of magnetic relaxation in spin ice: anomalous diffusion in a Coulomb fluid

Magnetization noise measurements on the spin ice Dy${}_2$Ti${}_2$O${}_7$ have revealed a remarkable `pink noise' power spectrum $S(f,T)$ below 4 K, including evidence of magnetic monopole excitations diffusing in a fractal landscape. However, at higher temperatures, the reported values of the anomalous exponent $b(T)$ describing the high frequency tail of $S(f,T)$ are not easy to reconcile with other results in the literature, which generally suggest significantly smaller deviations from the Brownian motion value of $b=2$, that become negligible above $T=20$ K. We accurately estimate $b(T)$ at temperatures between 2~K and 20~K, using a.c. susceptibility measurements that, crucially, stretch up to the relatively high frequency of $f = 10^6$ Hz. We show that previous noise measurements underestimate $b(T)$ and we suggest reasons for this. Our results establish deviations in $b(T)$ from $b=2$ up to about 20 K. However studies on different samples confirms that $b(T)$ is sample dependent: the details of this dependence agree in part, though not completely, with previous studies of the effect of crystal defects on monopole population and diffusion. Our results establish the form of $b(T)$ which characterises the subtle, and evolving, nature of monopole diffusion in the dense Coulomb fluid, a highly correlated state, where several dynamical processes combine. They do not rule out the importance of a fractal landscape picture emerging at lower temperatures where the monopole gas is dilute.

cond-mat.str-el↗

arXiv2024

Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation

Tuning magnetic properties in layered van der Waals (vdW) materials has captured a significant attention due to the efficient control of ground-states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature ($T_{\text{C}}$) and magnetic anisotropy. Here, we discover an uncharted role of intercalation to generate magnetic frustration. As a model study, we intercalate Na atoms into the vdW gaps of pristine Cr$_2$Ge$_2$Te$_6$ (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of $T_{\text{C}}$ from 66\,K to 240\,K and the switching of magnetic easy-hard axis direction. Our study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

cond-mat.mtrl-sci↗

arXiv2021

Experimental measurement of the isolated magnetic susceptibility

The isolated susceptibility $χ_{\rm I}$ may be defined as a (non-thermodynamic) average over the canonical ensemble, but while it has often been discussed in the literature, it has not been clearly measured. Here, we demonstrate an unambiguous measurement of $χ_{\rm I}$ at avoided nuclear-electronic level crossings in a dilute spin ice system, containing well-separated holmium ions. We show that $χ_{\rm I}$ quantifies the superposition of quasi-classical spin states at these points, and is a direct measure of state concurrence and populations.

quant-ph↗

arXiv2021

Tunable critical correlations in kagome ice

We present a comprehensive experimental and theoretical study of the kagome ice Coulomb phase, that explores the fine tuning of critical correlations by applied field, temperature and crystal orientation. The continuous modification of algebraic correlations is observed by polarised neutron scattering experiments and is found to be well described by numerical simulations of an idealised model. We further clarify the thermodynamics of field tuned Kasteleyn transitions and demonstrate some dramatic finite size scaling properties that depend on how topological string defects wind around the system boundaries. We conclude that kagome ice is a remarkable example of a critical and topological state in a real system that may be subject to fine experimental control.

cond-mat.stat-mech↗

arXiv2019

Nuclear spin assisted quantum tunnelling of magnetic monopoles in spin ice

Extensive work on single molecule magnets has identified a fundamental mode of relaxation arising from the nuclear-spin assisted quantum tunnelling of nearly independent and quasi-classical magnetic dipoles. Here we show that nuclear-spin assisted quantum tunnelling can also control the dynamics of purely emergent excitations: magnetic monopoles in spin ice. Our low temperature experiments were conducted on canonical spin ice materials with a broad range of nuclear spin values. By measuring the magnetic relaxation, or monopole current, we demonstrate strong evidence that dynamical coupling with the hyperfine fields bring the electronic spins associated with magnetic monopoles to resonance, allowing the monopoles to hop and transport magnetic charge. Our result shows how the coupling of electronic spins with nuclear spins may be used to control the monopole current. It broadens the relevance of the assisted quantum tunnelling mechanism from single molecular spins to emergent excitations in a strongly correlated system.

cond-mat.str-el↗

arXiv2018

Special temperatures in frustrated ferromagnets

The description and detection of unconventional magnetic states such as spin liquids is a recurring topic in condensed matter physics. While much of the efforts have traditionally been directed at geometrically frustrated antiferromagnets, recent studies reveal that systems featuring competing antiferromagnetic and ferromagnetic interactions are also promising candidate materials. We find that this competition leads to the notion of special temperatures, analogous to those of gases, at which the competing interactions balance, and the system is quasi-ideal. Although induced by weak perturbing interactions, these special temperatures are surprisingly high and constitute an accessible experimental diagnostic of eventual order or spin liquid properties. The well characterised Hamiltonian and extended low-temperature susceptibility measurement of the canonical frustrated ferromagnet Dy$_2$Ti$_2$O$_7$ enables us to formulate both a phenomenological and microscopic theory of special temperatures for magnets. Other members of this new class of magnets include kapellasite Cu$_3$Zn(OH)$_6$Cl$_2$ and the spinel GeCo$_2$O$_4$.

cond-mat.str-el↗

arXiv2018

Pauling entropy, metastability and equilibrium in Dy$_2$Ti$_2$O$_7$ spin ice

Determining the fate of the Pauling entropy in the classical spin ice material Dy$_2$Ti$_2$O$_7$ with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice - the dipolar spin ice model - predicts an ordering transition at $T\approx 0.15$ K, but recent experiments by Pomaranski $et\ al.$ suggest an entropy recovery over long time scales at temperatures as high as $0.5$ K, much too high to be compatible with theory. Using neutron scattering and specific heat measurements at low temperatures and with long time scales ($0.35$ K$/10^6$ s and $0.5$ K$/10^5$ s respectively) on several isotopically enriched samples we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Further, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez $et\ al.$ are, after all, essentially correct: the short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.

cond-mat.str-el↗

arXiv2017

Experimental signature of the attractive Coulomb force between positive and negative magnetic monopoles in spin ice

A non-Ohmic current that grows exponentially with the square root of applied electric field is well known from thermionic field emission (the Schottky effect), electrolytes (the second Wien effect) and semiconductors (the Poole-Frenkel effect). It is a universal signature of the attractive Coulomb force between positive and negative electrical charges, which is revealed as the charges are driven in opposite directions by the force of an applied electric field. Here we apply thermal quenches to spin ice to prepare metastable populations of bound pairs of positive and negative emergent magnetic monopoles at millikelvin temperatures. We find that the application of a magnetic field results in a universal exponential-root field growth of magnetic current, thus confirming the microscopic Coulomb force between the magnetic monopole quasiparticles and establishing a magnetic analogue of the Poole-Frenkel effect. At temperatures above 300 mK, gradual restoration of kinetic monopole equilibria causes the non-Ohmic current to smoothly evolve into the high field Wien effect for magnetic monopoles, as confirmed by comparison to a recent and rigorous theory of the Wien effect in spin ice. Our results extend the universality of the exponential-root field form into magnetism and illustrate the power of emergent particle kinetics to describe far-from equilibrium response in complex systems.

cond-mat.str-el↗

arXiv2014

Dynamic behavior of magnetic avalanches in the spin-ice compound Dy$_2$Ti$_2$O$_7$

Avalanches of the magnetization, that is to say an abrupt reversal of the magnetization at a given field, have been previously reported in the spin-ice compound Dy$_{2}$Ti$_{2}$O$_{7}$. This out-of-equilibrium process, induced by magneto-thermal heating, is quite usual in low temperature magnetization studies. A key point is to determine the physical origin of the avalanche process. In particular, in spin-ice compounds, the origin of the avalanches might be related to the monopole physics inherent to the system. We have performed a detailed study of the avalanche phenomena in three single crystals, with the field oriented along the [111] direction, perpendicular to [111] and along the [100] directions. We have measured the changing magnetization during the avalanches and conclude that avalanches in spin ice are quite slow compared to the avalanches reported in other systems such as molecular magnets. Our measurements show that the avalanches trigger after a delay of about 500 ms and that the reversal of the magnetization then occurs in a few hundreds of milliseconds. These features suggest an unusual propagation of the reversal, which might be due to the monopole motion. The avalanche fields seem to be reproducible in a given direction for different samples, but they strongly depend on the initial state of magnetization and on how the initial state was achieved.

cond-mat.str-el↗

arXiv2014

Far from equilibrium monopole dynamics in spin ice

Condensed matter in the low temperature limit reveals much exotic physics associated with unusual orders and excitations, examples ranging from helium superfluidity to magnetic monopoles in spin ice. The far-from-equilibrium physics of such low temperature states may be even more exotic, yet to access it in the laboratory remains a challenge. Here we demonstrate a simple and robust technique, the 'magnetothermal avalanche quench', and its use in the controlled creation of nonequilibrium populations of magnetic monopoles in spin ice at millikelvin temperatures. These populations are found to exhibit spontaneous dynamical effects that typify far-from-equilibrium systems, yet are captured by simple models. Our method thus opens the door to the study of far-from-equilibrium states in spin ice and other exotic magnets.

cond-mat.str-el↗

arXiv2013

Determination of the Entropy via Measurement of the Magnetization: Application to the Spin ice Dy2Ti2O7

The residual entropy of spin ice and other frustrated magnets is a property of considerable interest, yet the usual way of determining it, by integrating the heat capacity, is generally ambiguous. Here we note that a straightforward alternative method based on Maxwell's thermodynamic relations can yield the residual entropy on an absolute scale. The method utilises magnetization measurements only and hence is a useful alternative to calorimetry. We confirm that it works for spin ice, Dy2Ti2O7, which recommends its application to other systems. The analysis described here also gives an insight into the dependence of entropy on magnetic moment, which plays an important role in the theory of magnetic monopoles in spin ice. Finally, we present evidence of a field-induced crossover from correlated spin ice behaviour to ordinary paramagnetic behaviour with increasing applied field, as signalled by a change in the effective Curie constant.

cond-mat.str-el↗

arXiv2013

Dynamic susceptibility and dynamic correlations in spin ice

Here we calculate the dynamic susceptibility and dynamic correlation function in spin ice using the model of emergent magnetic monopoles. Calculations are based on a method originally suggested for the description of dynamic processes in water ice (non-equilibrium thermodynamics approach). We show that for zero temperature the dynamic correlation function reproduces the transverse dipole correlations (static correlation function) characteristic of spin ice in its ground state. At non-zero temperatures the dynamic correlation function includes an additional longitudinal component which decreases as the temperature decreases. Both terms (transverse and longitudinal) exhibit identical Debye-like dependences on frequency but with different relaxation times: the magnetic Coulomb interaction of monopoles reduces the longitudinal relaxation time with respect to the transverse one. We calculate the dielectric function for the magnetic monopole gas and discuss how the non-equilibrium thermodynamics approach exposes corrections to the Debye-Huckel theory of magnetic monopoles and the concept of "entropic charge".

cond-mat.str-el↗

arXiv2013

Crystal Shape-Dependent Magnetic Susceptibility and Curie Law Crossover in the Spin Ices Dy2Ti2O7 and Ho2Ti2O7

We present an experimental determination of the isothermal magnetic susceptibility of the spin ice materials Dy2Ti2O7 and Ho2Ti2O7 in the temperature range 1.8-300 K. The use of spherical crystals has allowed the accurate correction for demagnetizing fields and allowed the true bulk isothermal susceptibility X_T(T) to be estimated. This has been compared to a theoretical expression based on a Husimi tree approximation to the spin ice model. Agreement between experiment and theory is excellent at T > 10 K, but systematic deviations occur below that temperature. Our results largely resolve an apparent disagreement between neutron scattering and bulk measurements that has been previously noted. They also show that the use of non-spherical crystals in magnetization studies of spin ice may introduce very significant systematic errors, although we note some interesting - and possibly new - systematics concerning the demagnetizing factor in cuboidal samples. Finally, our results show how experimental susceptibility measurements on spin ices may be used to extract the characteristic energy scale of the system and the corresponding chemical potential for emergent magnetic monopoles.

cond-mat.str-el↗

arXiv2012

Brownian Motion and Quantum Dynamics of Magnetic Monopoles in Spin Ice

Spin ice illustrates many unusual magnetic properties, including zero point entropy, emergent monopoles and a quasi liquid-gas transition. To reveal the quantum spin dynamics that underpin these phenomena is an experimental challenge. Here we show how crucial information is contained in the frequency dependence of the magnetic susceptibility and in its high frequency or adiabatic limit. These measures indicate that monopole diffusion is strictly Brownian but is underpinned by spin tunnelling and is influenced by collective monopole interactions. We also find evidence of driven monopole plasma oscillations in weak applied field, and unconventional critical behaviour in strong applied field. Our results resolve contradictions in the present understanding of spin ice, reveal unexpected physics and establish adiabatic susceptibility as a revealing characteristic of exotic spin systems.

cond-mat.other↗

arXiv2011

Comment on 'Spin Ice: Magnetic Excitations without Monopole Signature Using $μ$SR' (arXiv:1110.0877)

Dunsiger and co-workers have criticised our paper on magnetic monopole dynamics spin ice [S. T. Bramwell et al., Nature, 461 956 (2009)]. We consider their criticisms and results but show that these do not warrant any revision of our earlier conclusions. In contrast, we point out that their conclusion of a `new' type of spin dynamics in spin ice is inconsistent with established facts.

cond-mat.str-el↗

arXiv2011

Magnetic frustration in the context of pseudo-dipolar ionic disorder

We consider an alternative to the usual spin glass paradigm for disordered magnetism, consisting of the previously unstudied combination of frustrated magnetic interactions and pseudo-dipolar disorder in spin positions. We argue that this model represents a general limiting case for real systems as well as a realistic model for certain binary fluorides and oxides. Furthermore, it is of great relevance to the highly topical subjects of the Coulomb phase and `charge ice'. We derive an analytical solution for the ground state phase diagram of a model system constructed in this paradigm and identify magnetic phases that remain either disordered or partially ordered even at zero temperature. These phases are of a hitherto unobserved type, but may be broadly classified as either `spin liquids' or `semi-spin liquids' in contrast to the usual spin glass or semi-spin glass. Numerical simulations are used to show that the spin liquid phase exhibits no spin glass transition at finite temperature, despite the combination of frustration and disorder. By mapping onto a model of uncoupled loops of Ising spins, we show that the magnetic structure factor of this phase acts, in the limit $T\rightarrow0$, as a sensitive probe of the positional disorder correlations. We suggest that this result can be generalized to more complex systems, including experimental realizations of canonical spin glass models.

cond-mat.other↗

arXiv2009

Magnetic Charge Transport

It has recently been predicted that certain magnetic materials contain mobile magnetic charges or `monopoles'. Here we address the question of whether these magnetic charges and their associated currents (`magnetricity') can be directly measured in experiment, without recourse to any material-specific theory. By mapping the problem onto Onsager's theory of weak electrolytes, we show that this is possible, and devise an appropriate method. Then, using muon spin rotation as a convenient local probe, we apply the method to a real material: the spin ice Dy2Ti2O7. Our experimental measurements prove that magnetic charges exist in this material, interact via a Coulomb interaction, and have measurable currents. We further characterise deviations from Ohm's Law, and determine the elementary unit of magnetic charge to be 5 muB per Angstrom, which is equal to that predicted by Castelnovo, Moessner and Sondhi using the microscopic theory of spin ice. Our demonstration of magnetic charge transport has both conceptual and technological implications.

cond-mat.other↗

arXiv2009

Experimental Proof of a Magnetic Coulomb Phase

Spin ice materials are magnetic substances in which the spin directions map onto hydrogen positions in water ice. Recently this analogy has been elevated to an electromagnetic equivalence, indicating that the spin ice state is a Coulomb phase, with magnetic monopole excitations analogous to ice's mobile ionic defects. No Coulomb phase has yet been proved in a real magnetic material, as the key experimental signature is difficult to resolve in most systems. Here we measure the scattering of polarised neutrons from the prototypical spin ice Ho2Ti2O7. This enables us to separate different contributions to the magnetic correlations to clearly demonstrate the existence of an almost perfect Coulomb phase in this material. The temperature dependence of the scattering is consistent with the existence of deconfined magnetic monopoles connected by Dirac strings of divergent length.

cond-mat.mtrl-sci↗