arXiv subjects

S. E. Brown

Publications and source records attributed to S. E. Brown.

At least 19 recordsLinked to original sources

arXiv2022

Controlling frustrated magnetism on the kagome lattice by uniaxial-strain tuning

It is predicted that strongly interacting spins on a frustrated lattice may lead to a quantum disordered ground state or even form a quantum spin liquid with exotic low-energy excitations. However, a thorough tuning of the frustration strength, separating its effects from those of disorder and other factors, is pending. Here we break the symmetry of a kagome-lattice compound in a controlled manner by applying $in$ $situ$ uniaxial stress. The transition temperature of $\rm Y_3Cu_9(OH)_{18}OCl_8$ is linearly enhanced with strain, $ΔT_{\rm N}/T_{\rm N} \approx 10\%$ upon in-plane compression of order $1\%$, providing clear evidence for a release of frustration and its pivotal role for magnetic order. Our comprehensive $^1$H NMR results suggest a $\overrightarrow{Q}=(1/3\times 1/3)$ state under unstrained conditions and further reveal an incomplete antiferromagnetic transition with fluctuating moments in this strongly frustrated system.

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arXiv2019

Impurity Moments Conceal Low-Energy Relaxation of Quantum Spin Liquids

We scrutinize the magnetic properties of $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl through its first-order metal-insulator transition at $T_{\rm CO}=30$ K by means of $^1$H nuclear magnetic resonance (NMR). While in the metal we find Fermi-liquid behavior with temperature-independent $(T_1T)^{-1}$, the relaxation rate exhibits a pronounced enhancement when charge order sets in. The NMR spectra remain unchanged through the transition and no magnetic order stabilizes down to 25 mK. Similar to the isostructural spin-liquid candidates $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ and $κ$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$, $T_1^{-1}$ acquires a dominant maximum (here around 5 K). Field-dependent experiments identify the low-temperature feature as a dynamic inhomogeneity contribution that is typically dominant over the intrinsic relaxation but gets suppressed with magnetic field.

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arXiv2019

Normal state $^{17}$O NMR studies of Sr$_{2}$RuO$_{4}$ under uniaxial stress

The effects of uniaxial compressive stress on the normal state $^{17}$O nuclear magnetic resonance properties of the unconventional superconductor Sr$_{2}$RuO$_{4}$ are reported. The paramagnetic shifts of both planar and apical oxygen sites show pronounced anomalies near the nominal $\mathbf{a}$-axis strain $\varepsilon_{aa}\equiv\varepsilon_v$, that maximizes the superconducting transition temperature, $T_{c}$. The spin susceptibility weakly increases on lowering the temperature below $T$$\simeq$10 K, consistent with an enhanced density of states associated with passing the Fermi energy through a van Hove singularity. Although such a Lifshitz transition occurs in the $γ$ band, formed by the Ru $d_{xy}$ states hybridized with in-plane O $p_π$ orbitals, the large Hund's coupling renormalizes the uniform spin susceptibilty, which, in turn, affects the hyperfine fields of all nuclei. We estimate this \textquotedblleft Stoner\textquotedblright\ renormalization, $S,$ by combining the data with first-principles calculations and conclude that this is an important part of the strain effect, with implications for superconductivity.

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arXiv2019

Pronounced drop of $^{17}$O NMR Knight shift in superconducting state of Sr$_2$RuO$_4$

The superconducting state in the quasi-two-dimensional and strongly correlated Sr$_2$RuO$_4$ is uniquely held up as a solid state analog to superfluid $^3$He-$A$, with an odd-parity order parameter that also breaks time reversal symmetry, and for which the vector order parameter has the same direction in spin space for all electron momenta. The recent discovery that uniaxial pressure causes a steep rise and maximum in transition temperature ($T_c$) in strained samples motivated the study of $^{17}$O nuclear magnetic resonance (NMR) that we describe in this article. A reduction of Knight shifts $K$ was observed for all strain values and temperatures $T<T_c$, consistent with a drop in spin polarization in the superconducting state. In unstrained samples, our results are in contradiction with a body of previous NMR work, and with the most prominent previous proposals for the order parameter of Sr$_2$RuO$_4$. Possible alternative scenarios are discussed.

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arXiv2018

Nuclear magnetic resonance investigation of the heavy fermion system Ce$_2$CoAl$_7$Ge$_4$

We present nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements performed on single crystalline \ccag{}, a member of a recently discovered family of heavy fermion materials Ce$_2M$Al$_7$Ge$_4$ ($M$ = Co, Ir, Ni, or Pd). Previous measurements indicated a strong Kondo interaction as well as magnetic order below $T_M = 1.8$ K. Our NMR spectral measurements show that the Knight shift $K$ is proportional to the bulk magnetic susceptibility $χ$ at high temperatures. A clear Knight shift anomaly ($K \not\propto χ$) is observed at coherence temperatures $T^* \sim 17.5$ K for $H_0 \parallel \hat{c}$ and 10 K for $H_0 \parallel \hat{a}$ at the ${}^{59}$Co site, and $T^* \sim 12.5$ K at the ${}^{27}$Al(3) site for $H_0 \parallel \hat{a}$ characteristic of the heavy fermion nature of this compound. At high temperatures the ${}^{59}$Co NMR spin-lattice relaxation rate $T_1^{-1}$ is dominated by spin fluctuations of the 4$f$ local moments with a weak metallic background. The spin fluctuations probed by ${}^{59}$Co NMR are anisotropic and larger in the basal plane than in the $c$ direction. Furthermore, we find $(T_1TK)^{-1} \propto T^{-1/2}$ at the ${}^{59}$Co site as expected for a Kondo system for $T > T^*$ and $T> T_K$. ${}^{59}$Co NQR \slrr{} measurements at low temperatures indicate slowing down of spin fluctuations above the magnetic ordering temperature $T_M \sim 1.8$ K. A weak ferromagnetic character of fluctuations around $\mathbf{q}=0$ is evidenced by an increase of $χT$ versus $T$ above the magnetic ordering temperature. We also find good agreement between the observed and calculated electric field gradients at all observed sites.

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arXiv2016

Charge fluctuations and superconductivity in organic conductors: the case of $β"$-(BEDT-TTF)$_2$SF$_5$CH$_2$CF$_2$SO$_3$

A $^{13}$C NMR study of the normal and superconducting states of the all-organic charge-transfer salt $β"$-(BEDT-TTF)$_2$SF$_5$CH$_2$CF$_2$SO$_3$ is presented. We find that the normal state is a charge-ordered metal configured as vertical stripes, produced by a combination of 1/4-filling, correlations, and a polar counterion sublattice. The NMR properties associated with the superconducting state are consistent with gap nodes and singlet pairing, and therefore similar to other organic superconductors. Quite distinct, however, is the absence of evidence for low-energy antiferromagnetic spin fluctuations for $T>T_c=4.5$ K. Both aspects are discussed in the context of a proposal that the pairing in this compound is driven by charge fluctuations.

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arXiv2015

Microscopic study of the Fulde-Ferrell-Larkin-Ovchinnikov state in an all-organic superconductor

Quasi-two dimensional superconductors with sufficiently weak interlayer coupling allow magnetic flux to penetrate in the form of Josephson vortices for in-plane applied magnetic fields. A consequence is the dominance of the Zeeman interaction over orbital effects. In the clean limit, the normal state is favored over superconductivity for fields greater than the paramagnetic limiting field, unless an intermediate, inhomogeneous state is stabilized. Presented here are nuclear magnetic resonance (NMR) studies of the inhomogeneous (FFLO) state for $β^{\prime \prime}$-(ET)$_2$SF$_5$CH$_2$CF$_2$SO$_3$. The uniform superconductivity-FFLO transition is identified at an applied field value of 9.3(0.1) T at low temperature ($T=130$ mK), and evidence for a possible second transition between inhomogeneous states at $\sim11$ T is presented. The spin polarization distribution inferred from the NMR absorption spectrum compares favorably to a single-Q modulation of the superconducting order parameter.

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arXiv2014

Quantum phase diagram of the $S=1/2$ triangular-lattice antiferromagnet Ba$_3$CoSb$_2$O$_9$

The magnetic phases of the ideal spin-1/2 triangular-lattice antiferromagnet Ba$_3$CoSb$_2$O$_9$ are identified and studied using $^{135,137}$Ba nuclear magnetic resonance (NMR) spectroscopy in magnetic fields ranging to 30T, oriented parallel and near perpendicular to the crystallographic $ab$-plane. For both directions, the saturation field is approximately 33T. Notably, the NMR spectra provide microscopic evidence for the stabilization of an up-up-down spin configuration for in-plane fields, giving rise to an one-third magnetization plateau ($M_\text{sat}/3$), as well as for a higher field phase transition near to $\sim (3/5)M_\text{sat}$ for both field orientations. Phase transitions are signaled by the evolution of the NMR spectra, and in some cases through spin-lattice relaxation measurements. The results are compared with expectations obtained from a semi-classical energy density modeling, in which quantum effects are incorporated by effective interactions extracted from the spin-wave analysis of the two-dimensional model. The interlayer coupling also plays a significant role in the outcome. Good agreement between the model and the experimental results is achieved, except for the case of fields approaching the saturation value applied along the c-axis.

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arXiv2012

Antiferromagnetic order in Ca$_{10}$(Pt$_3$As$_8$)(Fe$_2$As$_2$)$_5$ observed by $^{75}$As NMR

$^{75}$As nuclear magnetic resonance (NMR) measurements carried out on underdoped, non-superconducting Ca$_{10}$(Pt$_3$As$_8$)(Fe$_2$As$_2$)$_5$ reveal physical properties that are similar but not identical to the 122 superconductor parent compounds such as BaFe$_2$As$_2$. Results from the single crystal study indicate a phase transition to an antiferromagnetic (AF) state on cooling through T~100K, albeit nonuniformly. Specifically, the NMR lineshape reflects the presence of staggered hyperfine fields on the As sites associated with a striped AF order. The variation of the internal hyperfine field with temperature suggests that the phase transition to the AF state is discontinuous, and therefore likely coincident with the structural transition inferred from transport experiments.

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arXiv2009

NMR investigation of superconductivity and antiferromagnetism in CaFe$_2$As$_2$ under pressure

We report $^{75}$As NMR measurements in CaFe$_2$As$_2$, made under applied pressures up to 0.83 GPa produced by a standard clamp pressure cell. Our data reveal phase segregation of paramagnetic (PM) and antiferromagnetic (AFM) phases over a range of pressures, with the AFM phase more than 90 % dominant at low temperatures. In situ RF susceptibility measurements indicate the presence of superconductivity. $^{75}$As spin-lattice relaxation experiments indicate that the $^{75}$As nuclei sample the superconductivity while in the magnetically-ordered environment.

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arXiv2009

Critical properties of the S=1 spin dimer compound Ba3Mn2O8

Ba3Mn2O8 is a hexagonally coordinated Mn5+ S=1 spin dimer system with small uniaxial single-ion anisotropy. 135,137Ba NMR spectroscopy is used to establish the lower critical field Hc1 of distinct field-induced phases for H parallel to c,H perpendicular to c, and measure the longitudinal (Ml) and transverse (Mt) magnetizations in the vicinity of the quantum critical point (QCP). Ml_parallel (T, Hc1), Ml_perpendicular (T, Hc1) are reproduced by solving a low-energy model for a dilute gas of interacting bosons. Ml_parallel(T goes to 0, H = Hc1) (Ml_perpendicular(T goes to 0, H = Hc1)) follows the expectation for a BEC (Ising-like) QCP.

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arXiv2008

$^{77}$Se NMR investigation of the field-induced spin-density-wave transitions in (TMTSF)$_2$ClO$_4$

Complementary $^{77}$Se nuclear magnetic resonance (NMR) and electrical transport have been used to correlate the spin density dynamics with the subphases of the field-induced spin density wave (FISDW) ground state in \tmt. We find that the peaks in the spin-lattice relaxation rate 1/T$_1$ appear within the metal-FISDW phase boundary and/or at first-order subphase transitions. In the quantum limit above 25 T, the NMR data gives an insight into the FISDW electronic structure.

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arXiv2007

$^{77}$Se NMR measurements of the $π-d$ exchange field in the organic conductor $λ-$(BETS)$_{2}$FeCl$_{4}$

$^{77}$Se-NMR spectrum and frequency shift measurements in the paramagnetic metal (PM) and antiferromagnetic insulating (AFI) phases are reported for a small single crystal of the organic conductor $λ-$(BETS)$_{2}$FeCl$_{4}$ as a function of temperature ($T$) and field alignment for an applied magnetic field $B_{0}$ = 9 T. The results show that in the low $T$ limit, where the localized Fe$^{3+}$ spins ($S_{d}$ = 5/2) are almost fully polarized, the conduction electrons (Se $π$-electrons, spin $s_π$ = 1/2) in the BETS molecules experience an exchange field ($\bf{B}$$_{πd}$) from the Fe$^{3+}$ spins with a value of $-$ 32.7 $\pm$ 1.5 T at 5 K and 9 T aligned opposite to $\bf{B}$$_{0}$. This large negative value of $\bf{B}$$_{πd}$ is consistent with that predicted by the resistivity measurements and supports the Jaccarino-Peter internal field-compensation mechanism being responsible for the origin of field-induced superconductivity.

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arXiv2007

On the superconducting state of the organic conductor $(TMTSF)_2ClO_4$

$(TMTSF)_2ClO_4$ is a quasi-one dimensional organic conductor and superconductor with $T_c=1.4$K, and one of at least two Bechgaard salts observed to have upper critical fields far exceeding the paramagnetic limit. Nevertheless, the $^{77}$Se NMR Knight shift at low fields reveals a decrease in spin susceptibility $χ_s$ consistent with singlet spin pairing. The field dependence of the spin-lattice relaxation rate at 100mK exhibits a sharp crossover (or phase transition) at a field $H_s\sim15$kOe, to a regime where $χ_s$ is close to the normal state value, even though \hc2 $\gg H_s$.

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arXiv2007

$^{1}$H-NMR spin-echo measurements of the static and dynamic spin properties in $λ$-(BETS)$_{2}$FeCl$_{4}$

$^{1}$H-NMR spin-echo measurements of the spin-echo decay $M(2τ)$ with a decay rate 1/$T_{2}$ and the frequency shift $Δν/ν_{0}$ under applied magnetic field $\mathbf{B}$$_{0}$ = 9 T along the a-axis over a temperature range 2.0$-$180 K are reported for a single crystal of the organic conductor $λ$-(BETS)$_{2}$FeCl$_{4}$. It provides the spin dynamic and static properties in the paramagnetic metal (PM) and antiferromagnetic insulator (AFI) states as well as across the PM$-$AFI phase transition. A large slow beat structure in the spin-echo decay is observed with a typical beat frequency of $f$ $\sim$ 7 kHz and it varies across the spectrum. Its origin is attributed to the $^{1}$H$-$$^{1}$H dipole interactions rather than to the much larger dipolar field contribution from the Fe$^{3+}$ electrons (spin $S$ = 5/2). A simple phenomenological model provides an excellent fit to the data. The dominant $^{1}$H-NMR frequency shift comes from the dipolar field from the 3d Fe$^{3+}$ ions, and the Fe$^{3+}$ $-$ Fe$^{3+}$ exchange interactions ($J_{0}$) ($J_{0} $ includes the d$-$d exchange interactions through the $π-$electrons) have a substantial effect to the local field at the proton sites expecially at low temperatures. A good fit is obtained with $J_{0}$ = - 1.7 K. The data of the spin-echo decay rate 1/$T_{2}$ indicates that there is a significant change in the slow fluctuations of the local magnetic field at the $^{1}$H-sites on traversing the PM to AFI phase. This evidence supports earlier reports that the PM$-$AFI phase transition in $λ$-(BETS)$_{2}% $FeCl$_{4} $ is driven magnetically and first order.

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arXiv2006

Proton NMR measurements of the local magnetic field in the paramagnetic metal and antiferromagnetic insulator phases of $λ$-(BETS)$_{2}$FeCl$_{4}$

Measurements of the $^{1}$H-NMR spectrum of a small ($\sim$ 4 $μ$g) single crystal of the organic conductor $λ$-(BETS)$_{2}$FeCl$_{4}$ are reported with an applied magnetic field $\bf{B}$$_{0}$ = 9 T parallel to the a-axis in the $ac$-plane over a temperature $(T)$ range 2.0 $-$ 180 K. They provide the distribution of the static local magnetic field at the proton sites in the paramagnetic metal (PM) and antiferromagnetic insulator (AFI) phases, along with the changes that occur at the PM$-$AFI phase transition. The spectra have six main peaks that are significantly broadened and shifted at low $T$. The origin of these features is attributed to the large dipolar field from the 3d Fe$^{3+}$ ion moments (spin $S_{\rm{d}}$ = 5/2). Their amplitude and $T-$dependence are modeled using a modified Brillouin function that includes a mean field approximation for the total exchange interaction ($J_{0}$) between one Fe$^{3+}$ ion and its two nearest neighbors. A good fit is obtained using $J_{0}$ = $-$ 1.7 K. At temperatures below the PM$-$AFI transition temperature $T_{MI}$ = 3.5 K, an extra peak appears on the high frequency side of the spectrum and the details of the spectrum become smeared. Also, the rms linewidth and the frequency shift of the spectral distribution are discontinuous, consistent with the transition being first-order. These measurements verify that the dominant local magnetic field contribution is from the Fe$^{3+}$ ions and indicate that there is a significant change in the static local magnetic field distribution at the proton sites on traversing the PM to AFI phase transition.

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arXiv2005

NMR evidence for very slow carrier density fluctuations in the organic metal (TMTSF)$_2$ClO$_4$

We have investigated the origin of the large increase in spin-echo decay rates for the $^{77}$Se nuclear spins at temperatures near to $T=30K$ in the organic superconductor (TMTSF)$_2$ClO$_4$. The measured angular dependence of $T_2^{-1}$ demonstrates that the source of the spin-echo decays lies with carrier density fluctuations rather than fluctuations in TMTSF molecular orientation. The very long time scales are directly associated with the dynamics of the anion ordering occurring at $T=25K$, and the inhomogeneously broadened spectra at lower temperatures result from finite domain sizes. Our results are similar to observations of line-broadening effects associated with charge-ordering transitions in quasi-two dimensional organic conductors.

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arXiv2005

Coexistence of Superconductivity and Antiferromagnetism Probed by Simultaneous NMR and Electrical Transport in (TMTSF)2PF6

We report simultaneous NMR and electrical transport experiments in the pressure range near the boundary of the antiferromagnetic spin density wave (SDW) insulator and the metal-lic/superconducting (SC) phase in (TMTSF)2PF6. Measurements indicate a tricritical point separat-ing a line of second order SDW/metal transitions from a line of first order SDW/metal(SC) transi-tions with coexistence of macroscopic regions of SDW and metal(SC) order, with little mutual in-teraction but strong hysteretic effects. NMR results quantify the fraction of each phase.

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