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Register a new userInvestigation of Ionic and Anomalous Magnetic Behavior in CrSe$_2$ Using $^8$Li $beta$-NMR
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We have studied a mosaic of 1T-CrSe$_2$ single crystals using $beta$-detected nuclear magnetic resonance of $^{8}$Li from 4 to 300 K. We identify two broad resonances that show no evidence of quadrupolar splitting, indicating two magnetically distinct environments for the implanted ion. We observe stretched exponential spin lattice relaxation and a corresponding rate ($1/T_1$) that increases monotonically above 200 K, consistent with the onset of ionic diffusion. A pronounced maximum in $1/T_1$ is observed at the low temperature magnetic transition near 20 K. Between these limits, $1/T_1$ instead exhibits a broad minimum with a remarkable absence of strong features in the vicinity of structural and magnetic transitions between 150 and 200 K. Together, the results suggest $^{8}$Li$^{+}$ site occupation within the van der Waals gap between CrSe$_2$ trilayers. Possible origins of the two environments are discussed.
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We report measurements on the high temperature ionic and low temperature electronic properties of the 3D topological insulator Bi$_2$Te$_2$Se using ion-implanted $^8$Li $beta$-detected nuclear magnetic relaxation and resonance. With implantation energies in the range 5-28 keV, the probes penetrate beyond the expected range of the topological surface state, but are still within 250 nm of the surface. At temperatures above ~150 K, spin-lattice relaxation measurements reveal isolated $^8$Li$^{+}$ diffusion with an activation energy $E_{A} = 0.185(8)$ eV and attempt frequency $tau_{0}^{-1} = 8(3) times 10^{11}$ s$^{-1}$ for atomic site-to-site hopping. At lower temperature, we find a linear Korringa-like relaxation mechanism with a field dependent slope and intercept, which is accompanied by an anomalous field dependence to the resonance shift. We suggest that these may be related to a strong contribution from orbital currents or the magnetic freezeout of charge carriers in this heavily compensated semiconductor, but that conventional theories are unable to account for the extent of the field dependence. Conventional NMR of the stable host nuclei may help elucidate their origin.
We report measurements of the dynamics of isolated $^{8}$Li$^{+}$ in single crystal rutile TiO$_{2}$ using $beta$-detected NMR. From spin-lattice relaxation and motional narrowing, we find two sets of thermally activated dynamics: one below 100 K; and one at higher temperatures. At low temperature, the activation barrier is $26.8(6)$ meV with prefactor $1.23(5) times 10^{10}$ s$^{-1}$. We suggest this is unrelated to Li$^{+}$ motion, and rather is a consequence of electron polarons in the vicinity of the implanted $^{8}$Li$^{+}$ that are known to become mobile in this temperature range. Above 100 K, Li$^{+}$ undergoes long-range diffusion as an isolated uncomplexed cation, characterized by an activation energy and prefactor of $0.32(2)$ eV and $1.0(5) times 10^{16}$ s$^{-1}$, in agreement with macroscopic diffusion measurements. These results in the dilute limit from a microscopic probe indicate that Li$^{+}$ concentration does not limit the diffusivity even up to high concentrations, but that some key ingredient is missing in the calculations of the migration barrier. The anomalous prefactors provide further insight into both Li$^{+}$ and polaron motion.
$beta$-NMR of isolated $^8$Li has been investigated in the normal state of 2H-NbSe$_2$. In a high magnetic field of 3T a single resonance is observed with a Gaussian line width of 3.5 kHz. The line shape varies weakly as function of magnetic field and temperature but has a strong orientation dependence. The nuclear electric quadrupole splitting is unresolved implying that the electric field gradients are 10-100 times smaller than in other non-cubic crystals. The nuclear spin relaxation rate is also anomalously small but varies linearly with temperature as expected for Korringa relaxation in a metal. These results suggest that Li adopts an interstitial position between the weakly coupled NbSe$_2$ layers and away from the conduction band.
We report {beta} detected nuclear magnetic resonance ({beta}NMR) measurements of 8Li+ implanted into high purity Pt. The frequency of the 8Li {beta}NMR resonance and the spin-lattice relaxation rates 1/T1 were measured at temperatures ranging from 3 to 300 K. Remarkably, both the spin-lattice relaxation rate and the Knight shift K depend linearly on temperature T although the bulk susceptibility does not. K is found to scale with the Curie-Weiss dependence of the Pt susceptibility extrapolated to low temperatures. This is attributed to a defect response of the enhanced paramagnetism of Pt, i.e. the presence of the interstitial Li+ locally relieves the tendency for the Curie-Weiss susceptibility to saturate at low T . We propose that the low temperature saturation in c{hi} of Pt may be related to an interband coupling between the s and d bands that is disrupted locally by the presence of the Li+.
We report $beta$-detected nuclear magnetic resonance ($beta$-NMR) measurements in Bi$_{2}$Se$_{3}$:Ca (BSC) and Bi$_{2}$Te$_{3}$:Mn (BTM) single crystals using $^{8}$Li$^{+}$ implanted to depths on the order of 100 nm. Above $sim 200$ K, spin-lattice relaxation (SLR) reveals diffusion of $^{8}$Li$^{+}$, with activation energies of $sim 0.4$ eV ($sim 0.2$ eV) in BSC (BTM). At lower temperatures, the nuclear magnetic resonance (NMR) properties are those of a heavily doped semiconductor in the metallic limit, with Korringa relaxation and a small, negative, temperature-dependent Knight shift in BSC. From this, we make a detailed comparison with the isostructural tetradymite Bi$_{2}$Te$_{2}$Se (BTS) [McFadden et al., Phys Rev. B 99, 125201 (2019)]. In the magnetic BTM, the effects of the dilute Mn moments predominate, but remarkably the $^{8}$Li signal is not wiped out through the magnetic transition at 13 K, with a prominent critical peak in the SLR that is suppressed in a high applied field. This detailed characterization of the $^{8}$Li NMR response is an important step towards using depth-resolved $beta$-NMR to study the low-energy properties of the chiral topological surface state (TSS). With the bulk NMR response now established in several Bi$_{2}$Ch$_{3}$ tetradymite topological insulators (TIs), the prospect of directly probing their chiral TSS using the depth resolution afforded by $beta$-NMR remains strong.
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