arXiv subjects

J. M. Lawrence

Publications and source records attributed to J. M. Lawrence.

At least 19 recordsLinked to original sources

arXiv2026

Magnetic Field Dependence of the Spin Fluctuations in CeCu$_{5.8}$Ag$_{0.2}$

Quantum phase transitions are among the most intriguing phenomena that can occur when the electronic ground state of correlated metals are tuned by external parameters such as pressure, magnetic field or chemical substitution. Such transitions between distinct states of matter are driven by quantum fluctuations, and can give rise to macroscopically coherent phases that are at the forefront of condensed matter research. However, the nature of the critical fluctuations, and thus the fundamental physics controlling many quantum phase transitions, remain poorly understood in numerous strongly correlated metals. Here we study the model material CeCu$_{5.8}$Ag$_{0.2}$ to gain insight into the implications of critical fluctuations originating from different regions in reciprocal space. By employing an external magnetic field along the crystallographic $a$- and $c$-axis as auxiliary tuning parameter we observe a pronounced anisotropy in the suppression of the quantum critical fluctuations, reflecting the spin anisotropy of the long-range ordered ground state at larger silver concentration. Coupled with the temperature dependence of the quantum critical fluctuations, these results suggest that the quantum phase transition in CeCu$_{5.8}$Ag$_{0.2}$ is driven by three-dimensional spin-density wave fluctuations.

cond-mat.str-el↗

arXiv2024

Quantum Critical Scaling in Quasi-One-Dimensional YbFe$_5$P$_3$

We report measurements of the low temperature magnetization $M$ and specific heat $C$ as a function of temperature and magnetic field of the quasi-one-dimensional spin chain, heavy fermion compound YbFe$_5$P$_3$, which resides close to a quantum critical point. The results are compared to the predictions of scaling laws obtained from a generalized free energy function expected near an antiferromagnetic quantum critical point (AFQCP). The scaling behavior depends on the dimensionality $d$ of the fluctuations, the coherence length exponent $ν$, and the dynamic exponent $z$. The free energy treats the magnetic field as a relevant renormalization group variable, which leads to a new exponent $ϕ=νz_h$, where $z_h$ is a dynamic exponent expected in the presence of a magnetic field. When $z_h=z$, $T/H$ scaling is expected, as observed in several compounds close to a QCP; whereas in YbFe$_5$P$_3$, a $T/H^{3/4}$ dependence of the scaling is observed. This dependence reflects the relationship $z_h=(4z/3)$ and a field exponent $ϕ=4/3$. A feature of the scaling law is that it restricts the possible values of the exponents to two cases for YbFe$_5$P$_3$: $d$=1, $ν$=1, $z$=1, and $d$=2, $ν$=1/2, $z$=2.

cond-mat.str-el↗

arXiv2022

Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd$_3$ to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature - the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

cond-mat.str-el↗

arXiv2017

Unveiling the role of competing fluctuations at an unconventional quantum critical point

Quantum critical points (QCPs) are widely accepted as a source of a diverse set of collective quantum phases of matter. A central question is how the order parameters of phases near a QCP interact and determine the fundamental character of the critical dynamics which drive the quantum critical behavior. One of the most interesting proposals for the quantum critical behavior that occurs in correlated electron systems is that the behavior may arise from local, as opposed to long wavelength, critical fluctuations of the order parameter. The local criticality is believed to give rise to energy over temperature ($E/T$) scaling of the dynamic susceptibility with a fractional exponent near the quantum critical point (QCP). Here we show that $E/T$ scaling is indeed observed for CeCu$_{6-x}$Ag$_x$ but on closer inspection, the fluctuations can be separated into two components, implying that multiple order parameters play an important role in the unconventional critical behavior. Additionally, when the fluctuations corresponding to the magnetically ordered side of the phase diagram are separated, they are found to be three dimensional and to obey the scaling behavior expected for long wavelength fluctuations near an itinerant antiferromagnetic QCP.

cond-mat.str-el↗

arXiv2016

Comments on 'Phonon and magnetic structure in δ-plutonium from density-functional theory' by P. Söderlind et al

In their recent paper [Söderlind, P. et al., Sci. Rep. 5, 15958 (2015)], Söderlind et al. discuss two subjects from a theoretical point of view: the phonon spectra and the possible magnetic structure of δ-plutonium (Pu). Here, we comment on the second subject. Söderlind et al. compare the Pu magnetic form factor F(Q) calculated via density functional theory (DFT) with measurements of F(Q) by neutron spectroscopy [Janoschek, M. et al., Sci. Adv. 1, e1500188 (2015)]. In particular, this comparison does not consider a number of experimental facts established in the neutron spectroscopy study.

cond-mat.str-el↗

arXiv2015

The Valence-Fluctuating Ground State of Plutonium

A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise due to the competition of localized and itinerant electronic degrees of freedom. While the respective limits of well-localized or entirely itinerant ground states are well-understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and non-bonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum-mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium's magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

cond-mat.str-el↗

arXiv2014

Quantum Critical Fluctuations in the Heavy fermion compound Ce(Ni$_{0.935}$Pd$_{0.065}$)$_2$Ge$_2$

Electric resistivity, specific heat, magnetic susceptibility, and inelastic neutron scattering experiments were performed on a single crystal of the heavy fermion compound Ce(Ni$_{0.935}$Pd$_{0.065}$)$_2$Ge$_2$ in order to study the spin fluctuations near an antiferromagnetic (AF) quantum critical point (QCP). The resistivity and the specific heat coefficient for $T \leq$ 1 K exhibit the power law behavior expected for a 3D itinerant AF QCP ($ρ(T) \sim T^{3/2}$ and $γ(T) \sim γ_0 - b T^{1/2}$). However, for 2 $\leq T \leq$ 10 K, the susceptibility and specific heat vary as $log T$ and the resistivity varies linearly with temperature. Furthermore, despite the fact that the resistivity and specific heat exhibit the non-Fermi liquid behavior expected at a QCP, the correlation length, correlation time, and staggered susceptibility of the spin fluctuations remain finite at low temperature. We suggest that these deviations from the divergent behavior expected for a QCP may result from alloy disorder.

cond-mat.str-el↗

arXiv2014

Q-dependence of the spin fluctuations in the intermediate valence compound CePd3

We report inelastic neutron scattering experiments on a single crystal of the intermediate valence compound CePd3. At 300 K the magnetic scattering is quasielastic, with halfwidth of 23 meV, and is independent of momentum transfer Q. At low temperature, the Q-averaged magnetic spectrum is inelastic, exhibiting a broad peak centered near Emax = 55 meV. These results, together with the temperature dependence of the susceptibility, 4f occupation number, and specific heat, can be fit by the Kondo/Anderson impurity model. The low temperature scattering near Emax, however, shows significant variations with Q, reflecting the coherence of the 4f lattice. The intensity is maximal at (1/2, 1/2,0), intermediate at (1/2,0,0) and (0,0,0), and weak at (1/2,1/2,1/2). We discuss this Q-dependence in terms of current ideas about coherence in heavy fermion systems.

cond-mat.str-el↗

arXiv2011

Crystal fields, disorder, and antiferromagnetic short-range order in Yb0.24Sn0.76Ru

We report extensive measurements on a new compound (Yb0.24Sn0.76)Ru that crystallizes in the cubic CsCl structure. Valence band photoemission and L3 x-ray absorption show no divalent component in the 4f configuration of Yb. Inelastic neutron scattering (INS) indicates that the eight-fold degenerate J-multiplet of Yb3+ is split by the crystalline electric field (CEF) into a Γ7 doublet ground state and a Γ8 quartet at an excitation energy 20 meV. The magnetic susceptibility can be fit very well by this CEF scheme under the assumption that a Γ6 excited state resides at 32 meV; however, the Γ8/Γ6 transition expected at 12 meV was not observed in the INS. The resistivity follows a Bloch- Grüneisen law shunted by a parallel resistor, as is typical of systems subject to phonon scattering with no apparent magnetic scattering. All of these properties can be understood as representing simple local moment behavior of the trivalent Yb ion. At 1 K, there is a peak in specific heat that is too broad to represent a magnetic phase transition, consistent with absence of magnetic reflections in neutron diffraction. On the other hand, this peak also is too narrow to represent the Kondo effect in the Γ7 ground state doublet. On the basis of the field-dependence of the specific heat, we argue that antiferromagnetic shortrange order (possibly co-existing with Kondo physics) occurs at low temperatures. The long-range magnetic order is suppressed because the Yb site occupancy is below the percolation threshold for this disordered compound.

cond-mat.str-el↗

arXiv2011

Quantum critical behavior in the heavy Fermion single crystal Ce(Ni$_{0.935}$Pd$_{0.065}$)$_2$Ge$_2$

We have performed magnetic susceptibility, specific heat, resistivity, and inelastic neutron scattering measurements on a single crystal of the heavy Fermion compound Ce(Ni$_{0.935}$Pd$_{0.065}$)$_2$Ge$_2$, which is believed to be close to a quantum critical point (QCP) at T = 0. At lowest temperature(1.8-3.5 K), the magnetic susceptibility behaves as $χ(T)-χ(0)$ $\propto$ $T^{-1/6}$ with $χ(0) = 0.032 \times 10^{-6}$ m$^3$/mole (0.0025 emu/mole). For $T<$ 1 K, the specific heat can be fit to the formula $ΔC/T = γ_0 - T^{1/2}$ with $γ_0$ of order 700 mJ/mole-K$^2$. The resistivity behaves as $ρ= ρ_0 + AT^{3/2}$ for temperatures below 2 K. This low temperature behavior for $γ(T)$ and $ρ(T)$ is in accord with the SCR theory of Moriya and Takimoto\cite{Moriya}. The inelastic neutron scattering spectra show a broad peak near 1.5 meV that appears to be independent of $Q$; we interpret this as Kondo scattering with $T_K =$ 17 K. In addition, the scattering is enhanced near $Q$=(1/2, 1/2, 0) with maximum scattering at $ΔE$ = 0.45 meV; we interpret this as scattering from antiferromagnetic fluctuations near the antiferromagnetic QCP.

cond-mat.str-el↗

arXiv2011

Heavy Fermion scaling: Uranium versus Cerium and Ytterbium compounds

In an effort to explore the differences between rare-earth-based and uranium-based heavy Fermion (HF) compounds that reflect the underlying difference between local 4$f$ moments and itinerant 5$f$ moments we analyze scaling laws that relate the low temperature neutron spectra of the primary ("Kondo-esque") spin fluctuation to the specific heat and susceptibility. While the scaling appears to work very well for the rare earth intermediate valence compounds, for a number of key uranium compounds the scaling laws fail badly. There are two main reasons for this failure. First, the presence of antiferromagnetic (AF) fluctuations, which contribute significantly to the specific heat, alters the scaling ratios. Second, the scaling laws require knowledge of the high temperature moment degeneracy, which is often undetermined for itinerant 5$f$ electrons. By making plausible corrections for both effects, better scaling ratios are obtained for some uranium compounds. We point out that while both the uranium HF compounds and the rare earth intermediate valence (IV) compounds have spin fluctuation characteristic energies of order 5 - 25 meV, they differ in that the AF fluctuations that are usually seen in the U compounds are never seen in the rare earth IV compounds. This suggests that the 5f itineracy increases the f-f exchange relative to the rare earth case.

cond-mat.str-el↗

arXiv2010

Unusual signatures of the ferromagnetic transition in the heavy Fermion compound UMn$_2$Al$_{20}$

Magnetic susceptibility results for single crystals of the new cubic compounds UT$_2$Al$_{20}$ (T=Mn, V, and Mo) are reported. Magnetization, specific heat, resistivity, and neutron diffraction results for a single crystal and neutron diffraction and inelastic spectra for a powder sample are reported for UMn$_2$Al$_{20}$. For T = V and Mo, temperature independent Pauli paramagnetism is observed. For UMn$_2$Al$_{20}$, a ferromagnetic transition is observed in the magnetic susceptibility at $T_c$ = 20 K. The specific heat anomaly at $T_c$ is very weak while no anomaly in the resistivity is seen at $T_c$. We discuss two possible origins for this behavior of UMn$_2$Al$_{20}$: moderately small moment itinerant ferromagnetism, or induced local moment ferromagnetism.

cond-mat.str-el↗

arXiv2010

The Transition from Heavy Fermion to Mixed Valence in Ce1-xYxAl3: A Quantitative Comparison with the Anderson Impurity Model

We present a neutron scattering investigation of Ce1-xYxAl3 as a function of chemical pressure, which induces a transition from heavy-fermion behavior in CeAl3 (TK=5 K) to a mixed-valence state at x=0.5 (TK=150 K). The crossover can be modeled accurately on an absolute intensity scale by an increase in the k-f hybridization, Vkf, within the Anderson impurity model. Surprisingly, the principal effect of the increasing Vkf is not to broaden the low-energy components of the dynamic magnetic susceptibility but to transfer spectral weight to high energy.

cond-mat.str-el↗

arXiv2010

Kondo behavior, ferromagnetic correlations, and crystal fields in the heavy Fermion compounds Ce3X (X=In, Sn)

We report measurements of inelastic neutron scattering, magnetic susceptibility, magnetization, and the magnetic field dependence of the specific heat for the heavy Fermion compounds Ce$_3$In and Ce$_3$Sn. The neutron scattering results show that the excited crystal field levels have energies $E_1$ = 13.2 meV, $E_2$ = 44.8 meV for Ce$_3$In and $E_1$ = 18.5 meV, $E_2$ = 36.1 meV for Ce$_3$Sn. The Kondo temperature deduced from the quasielastic linewidth is 17 K for Ce$_3$In and 40 K for Ce$_3$Sn. The low temperature behavior of the specific heat, magnetization, and susceptibility can not be well-described by J=1/2 Kondo physics alone, but require calculations that include contributions from the Kondo effect, broadened crystal fields, and ferromagnetic correlations, all of which are known to be important in these compounds. We find that in Ce$_3$In the ferromagnetic fluctuation makes a 10-15 % contribution to the ground state doublet entropy and magnetization. The large specific heat coefficient $γ$ in this heavy fermion system thus arises more from the ferromagnetic correlations than from the Kondo behavior.

cond-mat.str-el↗

arXiv2010

Neutron scattering and scaling behavior in URu2Zn20 and YbFe2Zn20

The dynamic susceptibility chi"(deltaE), measured by inelastic neutron scattering measurements, shows a broad peak centered at Emax = 16.5 meV for the cubic actinide compound URu2Zn20 and 7 meV at the (1/2, 1/2, 1/2) zone boundary for the rare earth counterpart compound YbFe2Zn20. For URu2Zn20, the low temperature susceptibility and magnetic specific heat coefficient gamma = Cmag/T take the values chi = 0.011 emu/mole and gamma = 190 mJ/mole-K2 at T = 2 K. These values are roughly three times smaller, and Emax is three times larger, than recently reported for the related compound UCo2Zn20, so that chi and gamma scale inversely with the characteristic energy for spin fluctuations, Tsf = Emax/kB. While chi(T), Cmag(T), and Emax of the 4f compound YbFe2Zn20 are very well described by the Kondo impurity model, we show that the model works poorly for URu2Zn20 and UCo2Zn20, suggesting that the scaling behavior of the actinide compounds arises from spin fluctuations of itinerant 5f electrons.

cond-mat.str-el↗

arXiv2009

Inelastic Neutron Scattering Studies of the Intermediate Valence Compound CePd3

Inelastic neutron scattering measurements on a CePd3 single crystal show a magnetic response at 300 K that is independent of momentum transfer with a Lorentzian quasielastic energy spectrum with a half width of 23 meV. This is in agreement with the Anderson impurity model (AIM), that predicts local moment relaxational behavior in this temperature regime. The 7 K magnetic response has an inelastic Lorentzian spectrum, with characteristic energy of 53 meV and half width 32 meV at the (h, 1/2, 0) zone boundary. Such an inelastic spectrum is expected for the AIM at low temperature. Unlike the Q-independence of the impurity model, a variation of intensity with momentum transfer, including intensity maxima at the zone boundary, is observed in the data. However, this variation is only of order 20 percent, which is much smaller than that predicted by the Anderson lattice model (ALM). The large shifts in spectral weight expected for the ALM as Q varies from zone boundary to zone center are not observed in the experimental spectra.

cond-mat.str-el↗

arXiv2006

Ytterbium divalency and lattice disorder in near-zero thermal expansion YbGaGe

While near-zero thermal expansion (NZTE) in YbGaGe is sensitive to stoichiometry and defect concentration, the NZTE mechanism remains elusive. We present x-ray absorption spectra that show unequivocally that Yb is nearly divalent in YbGaGe and the valence does not change with temperature or with nominally 1% B or 5% C impurities, ruling out a valence-fluctuation mechanism. Moreover, substantial changes occur in the local structure around Yb with B and C inclusion. Together with inelastic neutron scattering measurements, these data indicate a strong tendency for the lattice to disorder, providing a possible explanation for NZTE in YbGaGe.

cond-mat.mtrl-sci↗

arXiv2006

Low temperature behavior of the heavy Fermion Ce3Co4Sn13

The compound Ce3Co4Sn13 is an extremely heavy cubic heavy fermion system with a low temperature electronic specific heat of order ~4 J/mol-K2. If the compound is nonmagnetic, it would be one of the heaviest nonmagnetic Ce-based heavy fermions reported to date and therefore would be expected to lie extremely close to a quantum critical point. However, a broad peak of unknown origin is observed at 0.8 K in the specific heat and magnetic susceptibility, suggesting the possibility of antiferromagnetic order. We present neutron diffraction data from polycrystalline samples which do not show any sign of magnetic scattering below 0.8 K. In addition, we present inelastic neutron scattering data from a single crystal sample which is consistent with the 1.2 K energy scale for Kondo spin fluctuations determined from specific heat measurements.

cond-mat.str-el↗