arXiv subjects

Rebecca W. Smaha

Publications and source records attributed to Rebecca W. Smaha.

25 records · Page 2Linked to original sources

arXiv2022

Emergence of spin singlets with inhomogeneous gaps in the kagome Heisenberg antiferromagnets Zn-barlowite and herbertsmithite

The kagome Heisenberg antiferromagnet formed by frustrated spins arranged in a lattice of corner-sharing triangles is a prime candidate for hosting a quantum spin liquid (QSL) ground state consisting of entangled spin singlets. But the existence of various competing states makes a convincing theoretical prediction of the QSL ground state difficult, calling for experimental clues from model materials. The kagome lattice materials Zn-barlowite ZnCu$_{3}$(OD)$_{6}$FBr and herbertsmithite ZnCu$_{3}$(OD)$_{6}$Cl$_2$ do not exhibit long range order, and they are considered the best realizations of the kagome Heisenberg antiferromagnet known to date. Here we use $^{63}$Cu nuclear quadrupole resonance combined with the inverse Laplace transform (ILT) to probe locally the inhomogeneity of delicate quantum ground states affected by disorder. We present direct evidence for the gradual emergence of spin singlets with spatially varying excitation gaps, but even at temperatures far below the super-exchange energy scale their fraction is limited to approximately 60\% of the total spins. Theoretical models need to incorporate the role of disorder to account for the observed inhomogeneously gapped behaviour.

cond-mat.str-el↗

arXiv2022

Freezing of the Lattice in the Kagome Lattice Heisenberg Antiferromagnet Zn-barlowite ZnCu$_3$(OD)$_6$FBr

We use $^{79}$Br nuclear quadrupole resonance (NQR) to demonstrate that ultra slow lattice dynamics set in below the temperature scale set by the Cu-Cu super-exchange interaction $J$~($\simeq160$~K) in the kagome lattice Heisenberg antiferromagnet Zn-barlowite. The lattice completely freezes below 50~K, and $^{79}$Br NQR lineshapes become twice broader due to increased lattice distortions. Moreover, the frozen lattice exhibits an oscillatory component in the transverse spin echo decay, a typical signature of pairing of nuclear spins by indirect nuclear spin-spin interaction. This indicates that some Br sites form structural dimers via a pair of kagome Cu sites prior to the gradual emergence of spin singlets below $\sim30$~K. Our findings underscore the significant roles played by subtle structural distortions in determining the nature of the disordered magnetic ground state of the kagome lattice.

cond-mat.str-el↗

arXiv2021

Field-tuned ferroquadrupolar quantum phase transition in the insulator TmVO$_{4}$

We report results of low-temperature heat capacity, magnetocaloric effect and neutron diffraction measurements of TmVO$_{4}$, an insulator that undergoes a continuous ferroquadrupolar phase transition associated with local partially-filled $4f$ orbitals of the thulium (Tm$^{3+}$) ions. The ferroquadrupolar transition, a realization of Ising nematicity, can be tuned to a quantum critical point using a magnetic field oriented along the $c$-axis of the tetragonal crystal lattice, which acts as an effective transverse field for the Ising-nematic order. In small magnetic fields, the thermal phase transition can be well-described using a semi-classical mean field treatment of the transverse field Ising model. However, in higher magnetic fields, closer to the field-tuned quantum phase transition, subtle deviations from this semi-classical behavior are observed due to quantum fluctuations. Although the phase transition is driven by the local $4f$ degrees of freedom, the crystal lattice still plays a crucial role, both in terms of mediating the interactions between the local quadrupoles, and in determining the critical scaling exponents, even though the phase transition itself can be described via mean field. In particular, bilinear coupling of the nematic order parameter to acoustic phonons changes the spatial and temporal fluctuations of the former in a fundamental way, resulting in different critical behavior of the nematic transverse-field Ising model as compared to the usual case of the magnetic transverse-field Ising model. Our results establish TmVO$_{4}$ as a model material, and electronic nematicity as a paradigmatic example, for quantum criticality in insulators.

cond-mat.str-el↗

arXiv2021

High energy spin excitations in the quantum spin liquid candidate Zn-barlowite probed by resonant inelastic x-ray scattering

A quantum spin liquid is a novel ground state that can support long-range entanglement between magnetic moments, resulting in exotic spin excitations involving fractionalized $S=\frac{1}{2}$ spinons. Here, we measure the excitations in single crystals of the spin liquid candidate Zn-barlowite using resonant inelastic X-ray scattering. By analyzing the incident polarization and temperature dependences, we deduce a clear magnetic scattering contribution forming a broad continuum that surprisingly extends up to $\sim$200 meV ($\sim$14$J$, where $J$ is the magnetic exchange). The excitation spectrum reveals that significant contributions arise from multiple pairs of spinons and/or antispinons at high energies.

cond-mat.str-el↗

arXiv2020

Site-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates

Realizing a quantum spin liquid (QSL) ground state in a real material is a leading issue in condensed matter physics research. In this pursuit, it is crucial to fully characterize the structure and influence of defects, as these can significantly affect the fragile QSL physics. Here, we perform a variety of cutting-edge synchrotron X-ray scattering and spectroscopy techniques, and we advance new methodologies for site-specific diffraction and L-edge Zn absorption spectroscopy. The experimental results along with our first-principles calculations address outstanding questions about the local and long-range structures of the two leading kagome QSL candidates, Zn-substituted barlowite Cu$_3$Zn$_{x}$Cu$_{1-x}$(OH)$_6$FBr and herbertsmithite Cu$_3$Zn(OH)$_6$Cl$_2$. On all length scales probed, there is no evidence that Zn substitutes onto the kagome layers, thereby preserving the QSL physics of the kagome lattice. Our calculations show that antisite disorder is not energetically favorable and is even less favorable in Zn-barlowite compared to herbertsmithite. Site-specific X-ray diffraction measurements of Zn-barlowite reveal that Cu$^{2+}$ and Zn$^{2+}$ selectively occupy distinct interlayer sites, in contrast to herbertsmithite. Using the first measured Zn L-edge inelastic X-ray absorption spectra combined with calculations, we discover a systematic correlation between the loss of inversion symmetry from pseudo-octahedral (herbertsmithite) to trigonal prismatic coordination (Zn-barlowite) with the emergence of a new peak. Overall, our measurements suggest that Zn-barlowite has structural advantages over herbertsmithite that make its magnetic properties closer to an ideal QSL candidate: its kagome layers are highly resistant to nonmagnetic defects while the interlayers can accommodate a higher amount of Zn substitution.

cond-mat.str-el↗

arXiv2020

Materializing Rival Ground States in the Barlowite Family of Kagome Magnets: Quantum Spin Liquid, Spin Ordered, and Valence Bond Crystal States

The spin-$\frac{1}{2}$ kagome antiferromagnet is considered an ideal host for a quantum spin liquid ground state. We find that when the bonds of the kagome lattice are modulated with a periodic pattern, new quantum ground states emerge. Newly synthesized crystalline barlowite (Cu$_4$(OH)$_6$FBr) and Zn-substituted barlowite demonstrate the delicate interplay between singlet states and spin order on the spin-$\frac{1}{2}$ kagome lattice. Comprehensive structural measurements demonstrate that our new variant of barlowite maintains hexagonal symmetry at low temperatures with an arrangement of distorted and undistorted kagome triangles, for which numerical simulations predict a pinwheel valence bond crystal (VBC) state instead of a quantum spin liquid (QSL). The presence of interlayer spins eventually leads to an interesting pinwheel $q=0$ magnetic order. Partially Zn-substituted barlowite (Cu$_{3.44}$Zn$_{0.56}$(OH)$_6$FBr) has an ideal kagome lattice and shows QSL behavior, indicating a surprising robustness of the QSL against interlayer impurities. The magnetic susceptibility is similar to that of herbertsmithite, even though the Cu$^{2+}$ impurities are above the percolation threshold for the interlayer lattice and they couple more strongly to the nearest kagome moment. This system is a unique playground displaying QSL, VBC, and spin order, furthering our understanding of these highly competitive quantum states.

cond-mat.str-el↗

arXiv2018

Synthesis-Dependent Properties of Barlowite and Zn-Substituted Barlowite

The mineral barlowite, Cu$_4$(OH)$_6$FBr, has been the focus of recent attention due to the possibility of substituting the interlayer Cu$^{2+}$ site with non-magnetic ions to develop new quantum spin liquid materials. We re-examine previous methods of synthesizing barlowite and describe a novel hydrothermal synthesis method that produces large single crystals of barlowite and Zn-substituted barlowite (Cu$_3$Zn$_x$Cu$_{1-x}$(OH)$_6$FBr). The two synthesis techniques yield barlowite with indistinguishable crystal structures and spectroscopic properties at room temperature; however, the magnetic ordering temperatures differ by 4 K and the thermodynamic properties are clearly different. The dependence of properties upon synthetic conditions implies that the defect chemistry of barlowite and related materials is complex and significant. Zn-substituted barlowite exhibits a lack of magnetic order down to T = 2 K, characteristic of a quantum spin liquid, and we provide a synthetic route towards producing large crystals suitable for neutron scattering.

cond-mat.str-el↗