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P. M. Singer

Publications and source records attributed to P. M. Singer.

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$^{139}$La NMR investigation of the interplay between the lattice, charge, and spin dynamics in charge ordered high $T_c$ cuprate La$_{1.875}$Ba$_{0.125}$CuO$_{4}$

We investigate the interplay between the lattice, charge, and spin dynamics in charge ordered high $T_c$ cuprate La$_{1.875}$Ba$_{0.125}$CuO$_{4}$ ($T_{c} =4$~K) based on the inverse Laplace transform (ILT) analysis of the $^{139}$La nuclear spin-lattice relaxation rate $1/T_1$ (dubbed ILTT$_{1}$ analysis here after). A major thrust of the ILTT$_{1}$ analysis is that one can deduce the probability density function $P(1/T_1)$ of distributed $1/T_1$. We demonstrate that $1/T_{1}^{lm}$, defined as the log-mean (i.e. the center of gravity on a logarithmic scale) of $P(1/T_1)$, can be well approximated by $1/T_{1}^{str}$ deduced from the phenomenological stretched fit, however, $P(1/T_1)$ can provide much richer insight into how the lattice, charge, and spin fluctuations and their distribution develop near and below the long range charge order at $T_{charge} \sim 54$~K. Upon entering the charge ordered state, a divergent increase of $1/T_{1}^{lm}$ toward the spin ordering at $T_{spin}^{\mu SR} \simeq 35$~K is accompanied by an asymmetric broadening of $P(1/T_1)$. Even deep inside the charge ordered state, $1/T_{1}$ at a gradually diminishing fraction of $^{139}$La sites continues to slow down as temperature is lowered, as expected for canonical superconducting CuO$_2$ planes without enhanced spin fluctuations. The fraction of such canonical $^{139}$La sites almost disappears by $\simeq 40$~K. In contrast, nearly a half of the $^{139}$La sites in La$_{1.885}$Sr$_{0.115}$CuO$_{4}$ ($T_{charge} \simeq 80$~K) still exhibits the canonical behavior without enhanced spin fluctuations even near its $T_{c} = 31$~K. These contrasting behaviors explain why superconductivity in La$_{1.875}$Ba$_{0.125}$CuO$_{4}$ is more strongly suppressed than in La$_{1.885}$Sr$_{0.115}$CuO$_{4}$ despite the lower onset temperature of the charge order.

cond-mat.str-el

Revisiting the $^{63}$Cu NMR signature of charge order in La$_{1.875}$Ba$_{0.125}$CuO$_{4}$

We use single crystal $^{63}$Cu NMR techniques to revisit the early $^{63}$Cu NQR signature of charge order observed for La$_{1.875}$Ba$_{0.125}$CuO$_{4}$ ($T_{\text{c}} =4$~K) [A. W. Hunt et al., Phys. Rev. Lett. {\bf 82}, 4300 (1999)]. We show that the growth of spin correlations is accelerated below $\sim 80$~K, where the inverse Laplace transform (ILT) T$_{1}$ analysis of the $^{139}$La NMR spin-lattice relaxation curve recently uncovered emergence of the slow components in the lattice and/or charge fluctuations [P. M. Singer et al., {\bf 101}, 174508 (2020)]. From the accurate measurements of the $^{63}$Cu NMR signal intensity, spin echo decay $M(2\tau)$, spin-lattice relaxation rate $^{63}1/T_1$, and its density distribution function $P(^{63}1/T_{1})$, we also demonstrate that charge order at $T_{\text{charge}}\simeq 54$~K turns on strong enhancement of spin fluctuations {\it within charge ordered domains}, thereby making the CuO$_2$ planes extremely inhomogeneous. The charge ordered domains grow quickly below $T_{\text{charge}}$, and the volume fraction $F_{\text{CA}}$ of the canonical domains unaffected by charge order gradually diminishes by $\sim 35$~K. This finding agrees with our independent estimations of $F_{\text{CA}}$ based entirely on the $^{139}$La ILTT$_{1}$ analyses, but is in a stark contrast with much slower growth of charge ordered domains observed for La$_{1.885}$Sr$_{0.115}$CuO$_{4}$ from its $T_{\text{charge}}\simeq 80$~K to $T_{\text{c}}\simeq 30$~K.

cond-mat.supr-con

Distribution of the magnetic environment in charge ordered La$_{1.885}$Sr$_{0.115}$CuO$_{4}$

We report the inverse Laplace transform (ILT) analysis of the $^{139}$La nuclear spin-lattice relaxation rate $1/T_1$ in charge ordered La$_{1.885}$Sr$_{0.115}$CuO$_4$ ($T_{charge} \sim 80$K, $T_{c} \simeq T_{spin}^{neutron}=30$K), and shed new light on its magnetic inhomogeneity. We deduce the probability density function $P(1/T_{1})$ of the distributed $1/T_1$ (i.e. the histogram of distributed $1/T_1$) by taking the inverse Laplace transform of the experimentally observed nuclear magnetization recovery curve $M(t)$. We demonstrate that spin freezing sets in in some domains precisely below the onset of charge order at $T_{charge}$, but their volume fraction grows only gradually toward $T_{c}$. Nearly a half of the sample volume exhibits properties expected for canonical high $T_c$ cuprates without charge order even near $T_c$. Our findings explain why charge order does not suppress $T_c$ of La$_{1.885}$Sr$_{0.115}$CuO$_4$ as significantly as in La$_{1.875}$Ba$_{0.125}$CuO$_4$.

cond-mat.supr-con

Molecular Dynamics Simulations of NMR Relaxation and Diffusion of Bulk Hydrocarbons and Water

Molecular dynamics (MD) simulations are used to investigate $^1$H nuclear magnetic resonance (NMR) relaxation and diffusion of bulk $n$-C$_5$H$_{12}$ to $n$-C$_{17}$H$_{36}$ hydrocarbons and bulk water. The MD simulations of the $^1$H NMR relaxation times $T_{1,2}$ in the fast motion regime where $T_1 = T_2$ agree with measured (de-oxygenated) $T_2$ data at ambient conditions, without any adjustable parameters in the interpretation of the simulation data. Likewise, the translational diffusion $D_T$ coefficients calculated using simulation configurations are well-correlated with measured diffusion data at ambient conditions. The agreement between the predicted and experimentally measured NMR relaxation times and diffusion coefficient also validate the forcefields used in the simulation. The molecular simulations naturally separate intramolecular from intermolecular dipole-dipole interactions helping bring new insight into the two NMR relaxation mechanisms as a function of molecular chain-length (i.e. carbon number). Comparison of the MD simulation results of the two relaxation mechanisms with traditional hard-sphere models used in interpreting NMR data reveals important limitations in the latter. With increasing chain length, there is substantial deviation in the molecular size inferred on the basis of the radius of gyration from simulation and the fitted hard-sphere radii required to rationalize the relaxation times. This deviation is characteristic of the local nature of the NMR measurement, one that is well-captured by molecular simulations.

physics.chem-ph

NMR Evidence for Gapped Spin Excitations in Metallic Carbon Nanotubes

We report on the spin dynamics of 13C isotope enriched inner-walls in double-wall carbon nanotubes (DWCNT) using 13C nuclear magnetic resonance (NMR). Contrary to expectations, we find that our data set implies that the spin-lattice relaxation time (T1) has the same temperature (T) and magnetic field (H) dependence for most of the innerwall nanotubes detected by NMR. In the high temperature regime (T > 150 K), we find that the T and H dependence of 1/T1T is consistent with a 1D metallic chain. For T < 150 K, we find a significant increase in 1/T1T with decreasing T, followed by a sharp drop below 20 K. The data clearly indicates the formation of a gap in the spin excitation spectrum, where the gap value 2 Delta = 40 K (= 3.7 meV) is H independent.

cond-mat.str-el

Isotope engineering in carbon nanotube systems

We report on single-wall carbon nanotube (SWCNT) specific $^{13}$C isotope enrichment. The high temperature annealing of isotope enriched fullerenes encapsulated in SWCNTs yields double-wall carbon nanotubes (DWCNTs) with a high isotope enrichment of the inner wall. The vibrational spectra evidences that no carbon exchange occurs between the two walls. The method facilitates the identification of the Raman signal of the outer and inner tubes. Nuclear magnetic resonance proves the significant contrast of the isotope enriched SWCNTs as compared to other carbon phases, and provides information on the electronic properties of the small diameter inner tubes of the DWCNTs.

cond-mat.mtrl-sci

{63}Cu NQR Study of the Inhomogeneous Electronic State in La{2-x}Sr{x}CuO{4}

We report detailed systematic measurements of the spatial variation in electronic states in the high T{c} superconductor La{2-x}Sr{x}CuO{4} (0.04<= x <= 0.16) using {63}Cu NQR for {63}Cu isotope enriched poly-crystalline samples. We demonstrate that the spatial variation in local hole concentration {63}x{local} given by {63}x{local} = x +/- {63}Dx{local}, where x is the nominal hole concentration and {63}Dx{local} is defined as the amplitude (or extent) of the spatial variation, is reflected in the frequency dependence of the spin-lattice relaxation rate {63}1/T{1} across the inhomogeneous linebroadening of the {63}Cu NQR spectrum. By using high precision measurements of the temperature dependence of {63}1/T_{1} at various positions across the {63}Cu NQR lineshape, we demonstrate that {63}Dx{local} increases below 500 - 600 K and reaches values as large as {63}Dx{local} / x ~ 0.5 in the temperature region > 150 K. By incorporating the random positioning of {+2}Sr donor ions in the lattice in a novel approach, a lower bound to the length scale of the spatial variation {63}R{patch} is deduced by fitting the entire {63}Cu NQR spectrum (including the ``B'' -line) using a patch-by-patch distribution of the spatial variation {63}x{local} with the patch radius {63}R_{patch} > 3.0 nm as the only free parameter. A corresponding upper bound to the amplitude of the spatial variation {63}Dx{patch} (~ 1/{63}R_{patch}) is deduced within the model, and consistent results are found with {63}Dx{local} . We also deduce the onset temperature T{Q} (> 400 K) for local orthorhombic lattice distortions which, in the region x > 0.04, is found to be larger than the onset temperature of long range structural order.

cond-mat.str-el

What has NMR taught us about stripes and inhomogeneity?

The purpose of this brief invited paper is to summarize what we have (not) learned from NMR on stripes and inhomogeneity in La{2-x}Sr{x}CuO{4}. We explain that the reality is far more complicated than generally accepted.

cond-mat.str-el

Systematic (63)Cu NQR and (89)Y NMR Study of Spin Dynamics in Y(1-z)Ca(z)Ba(2)Cu(3)O(y) Across Superconductor-Insulator Boundary

We demonstrate that the spin dynamics in underdoped Y(1-z)Ca(z)Ba(2)Cu(3)O(y) for y=~6.0 exhibit qualitatively the same behavior to underdoped La(2-x)Sr(x)CuO(4) for an equal amount of hole concentration p=z/2=x<0.11. However,a spin-gap appears as more holes are doped into the CuO(2) plane by increasing the oxygen concentration to y=~6.5 for a fixed value of Ca concentration z. Our results also suggest that Ca doping causes disorder effects that enhance the low frequency spin fluctuations.

cond-mat.supr-con

(63)Cu NQR Evidence for Spatial Variation of Hole Concentration in La(2-x)Sr(x)CuO(4)

We report experimental evidence for the spatial variation of hole concentration x_(hole) in the high Tc superconductor La(2-x)Sr(x)CuO(4) (0.04 <= x <= 0.16) by using (63)Cu NQR for (63)Cu isotope enriched samples. We demonstrate that the extent of the spatial variation of the local hole concentration D(x)_(hole) is reflected on (63)1/T1 and deduce the temperature dependence. D(x)_(hole) increases below 500 - 600K, and reaches values as large as D(x)_(hole)/x ~ 0.5 below ~ 150K. We estimate the length scale of the spatial variation in x_(hole) to be R_(hole) >~ 3nm from analysis of the NQR spectrum.

cond-mat.supr-con

(13)C NMR investigation of the superconductor MgCNi_3 up to 800K

We report (13)C NMR characterization of the new superconductor MgCNi_3 (He et al., Nature (411), 54 (2001)). We found that both the uniform spin susceptibility and the spin fluctuations show a strong enhancement with decreasing temperature, and saturate below ~50K and ~20K respectively. The nuclear spin-lattice relaxation rate 1/(13)T_1T exhibits typical behaviour for isotropic s-wave superconductivity with a coherence peak below Tc=7.0K that grows with decreasing magnetic field.

cond-mat.supr-con

Glassy Slowing of Stripe Modulation in (La,Eu,Nd)(2-x)(Sr,Ba)(x)CuO4: A Cu-63 and La-139 NQR Study Down to 350mK

We report a comprehensive Cu and La NQR study down to 350mK in the stripe phase of the hole-doped high temperature superconductors with hole concentration approximately 1/8. We observe the hyperfine broadened NQR lineshape only below 8-20K for x=1/8, indicating that the ordered moments continue to fluctuate slowly even below the temperature range where they appear static in other measurements. Detailed numerical simulations of the Zeeman perturbed Cu NQR lineshape establish that widely accepted models of periodic modulation of spin density waves with maximum moment approxiamtely 0.3mu_B can not account for the NQR lineshape. These results suggest that significant disorder exists at NQR time scales. By fitting a single model to several sets of experimental data, we deduce the spatial distribution of the spin fluctuation frequency scale and its temperature dependence. Our results indicate that as soon as charge dynamics slow down, the spin fluctuationsbegin to slow dramatically with spin stiffness approximately 200K. However, the motional narrowing feature observed in the Zeeman perturbed NQR measurements suggest that the slowing of the spin fluctuations levels off at frequencies somewhat below the NQR frequency. By extending the analysis to other hole concentrations, we find a qualitative difference above and below x=1/8.

cond-mat.supr-con

Systematic Cu-63 NQR studies of the stripe phase in La(1.6-x)Nd(0.4)Sr(x)CuO(4) for 0.07 <= x <= 0.25

We demonstrate that the integrated intensity of Cu-63 nuclear quadrupole resonance (NQR) in La(1.6-x)Nd(0.4)Sr(x)CuO(4) decreases dramatically below the charge-stripe ordering temperature T(charge). Comparison with neutron and X-ray scattering indicates that the wipeout fraction F(T) (i.e. the missing fraction of the integrated intensity of the NQR signal) represents the charge-stripe order parameter. The systematic study reveals bulk charge-stripe order throughout the superconducting region 0.07 <= x <= 0.25. As a function of the reduced temperature t = T/T(charge), the temperature dependence of F(t) is sharpest for the hole concentration x=1/8, indicating that x=1/8 is the optimum concentration for stripe formation.

cond-mat.supr-con

Cu-63 NQR Measurement of Stripe Order Parameter in La(2-x)Sr(x)CuO(4)

We demonstrate that one can measure the charge-stripe order parameter in the hole-doped CuO(2) planes of La(1.875)Ba(0.125)CuO(4), La(1.48)Nd(0.4)Sr(0.12)CuO(4) and La(1.68)Eu(0.2)Sr(0.12)CuO(4) utilizing the wipeout effects of Cu-63 NQR. Application of the same approach to La(2-x)Sr(x)CuO(4) reveals the presence of similar stripe order for the entire underdoped superconducting regime 1/16 < x < 1/8.

cond-mat.supr-con