NMR relaxation studies of electronic structure in NbSe3

NMR spin-lattice relaxation measurements of the Nb93 resonance for each Nb site were performed on an aligned, multicrystalline NbSe3 sample at different temperatures. Results are associated with local electron densities of states for each of the three crystallographic sites, demonstrating Fermi-surface changes associated with the two charge-density-wave phase transitions. The most significant Fermi-surface changes occur for the yellow and orange crystallographic sites, at the high- and low-temperature phase transitions, respectively. The third site, however, is found to be noninsulating. A comparison is made to band theory and other experimental results

Topological nodal line in ZrTe2_2 demonstrated by nuclear magnetic resonance

In this work, we report nuclear magnetic resonance (NMR) combined with density functional theory (DFT) studies of the transition metal dichalcogenide ZrTe$_2$. The measured NMR shift anisotropy reveals a quasi-2D behavior connected to a topological nodal line close to the Fermi level. With the magnetic field perpendicular to the ZrTe$_2$ layers, the measured shift can be well-fitted by a combination of enhanced diamagnetism and spin shift due to high mobility Dirac electrons. The spin-lattice relaxation rates with external field both parallel and perpendicular to the layers at low temperatures match the expected behavior associated with extended orbital hyperfine interaction due to quasi-2D Dirac carriers. In addition, calculated band structures also show clear evidence for the existence of nodal line in ZrTe$_2$ between $\Gamma$ and A. For intermediate temperatures, there is a sharp reduction in spin-lattice relaxation rate which can be explained as due to a reduced lifetime for these carriers, which matches the reported large change in mobility in the same temperature range. Above 200 K, the local orbital contribution starts to dominate in an orbital relaxation mechanism revealing the mixture of atomic functions.Comment: 9 pages, 5 figure

Dirac electron behavior and NMR evidence for topological band inversion in ZrTe5

We report $^{125}$Te NMR measurements of the topological quantum material ZrTe$_5$. Spin-lattice relaxation results, well-explained by a theoretical model of Dirac electron systems, reveal that the topological characteristic of ZrTe$_5$ is $T$-dependent, changing from weak topological insulator to strong topological insulator as temperature increases. Electronic structure calculations confirm this ordering, the reverse of what has been proposed. NMR results demonstrate a gapless Dirac semimetal state occurring at a Lifshitz transition temperature, $T_c=85$ K in our crystals. We demonstrate that the changes in NMR shift at $T_c$ also provide direct evidence of band inversion when the topological phase transition occurs.Comment: 5 pages, 4 figure

Gap-opening transition in Dirac semimetal ZrTe5_5

We apply $^{125}$Te nuclear magnetic resonance (NMR) spectroscopy to investigate the Dirac semimetal ZrTe$_5$. With the NMR magnetic field parallel to the $b$-axis, we observe significant quantum magnetic effects. These include an abrupt drop at 150 K in spin-lattice relaxation rate. This corresponds to a gap-opening transition in the Dirac carriers, likely indicating the onset of excitonic pairing. Below 50 K, we see a more negative shift for the Te$_z$ bridging site indicating the repopulation of Dirac levels with spin polarized carriers at these temperatures. This is the previously reported 3D quantum Hall regime; however, we see no sign of a charge density wave as has been proposed.Comment: 5 pages, 4 figure

Direct Measure of Giant Magnetocaloric Entropy Contributions in Ni-Mn-In

Off-stoichiometric alloys based on Ni 2 MnIn have drawn attention due to the coupled first order magnetic and structural transformations, and the large magnetocaloric entropy associated with the transformations. Here we describe calorimetric and magnetic studies of four compositions. The results provide a direct measure of entropy changes contributions including at the first-order phase transitions, and thereby a determination of the maximum field-induced entropy change corresponding to the giant magnetocaloric effect. We find a large excess entropy change, attributed to magneto-elastic coupling, but only in compositions with no ferromagnetic order in the high-temperature austenite phase. Furthermore, a molecular field model corresponding to antiferromagnetism of the low-temperature phases is in good agreement, and nearly independent of composition, despite significant differences in overall magnetic response of these materials

Superconductivity and Magnetism in Silicon and Germanium Clathrates

Clathrates are materials containing closed polyhedral cages stacked to form crystalline frameworks. With Si, Ge, and Sn atoms populating these frameworks, a wide variety of electronic and vibrational properties can be produced in these materials, by substitution upon framework sites or through incorporation of ions in cage-center positions. Commonly-formed structures include the type I, type II, and chiral clathrate types, whose properties will be described here. Ba8Si46 with the type-I structure has been found to exhibit superconductivity with Tc as high as 9 K. The enhanced Tc in this compound has been shown to arise predominantly from very sharp features in the electronic densities of states associated with the extended sp3- bonded framework. Atomic substitution can tailor these electronic properties, however the associated disorder has been found to inevitably lower the Tc due to the disrupted continuity of the framework. Efforts to produce analogous Ge-based superconductors have not been successful, due to the appearance of spontaneous vacancies, which also serve to disrupt the frameworks. The formation of these vacancies is driven by the Zintl mechanism, which plays a much more significant role for the structural stability of the Ge clathrates. The sharp density of states features in these extended framework materials may also lead to enhanced magnetic features, due to conduction-electron mediated coupling of substituted magnetic ions. This has led to magnetic ordering in Fe and Mn-substituted clathrates. The largest number of clathrates exhibiting magnetic behavior has been produced by substitution of Eu on cage-center sites, with a ferromagnetic Tc as high as 38 K observed in such materials

NMR Study of Ba8Cu5SixGe41-x Clathrate Semiconductors

We have performed 63Cu, 65Cu, and 137Ba NMR on Ba8Cu5SixGe41-x, a series of intermetallic clathrates known for their potential as thermoelectric materials, in order to investigate the electronic behavior of the samples. The spectra and spin - lattice relaxation times were measured at 77 K and 290 K for the entire composition range 0 <= x <= 41. Magnetic and quadrupole shifts and relaxation rates of the Cu NMR data were extracted, and thereby carrier-induced metallic contributions identified. The observed shifts change in a nonlinear way with increasing Si substitution: from x = 0 to about 20 the shifts are essentially constant, while approaching x = 41 they increase rapidly. At the same time, Ba NMR data indicate greater Ba-site participation in the conduction band in Ba8Cu5Si41 than in Ba8Cu5Ge41. The results indicate surprisingly little change in electronic features vs. Si content for most of the composition range, while Ba8Cu5Si41 exhibits enhanced hybridization and a more metallic framework than Ba8Cu5Ge41.Robert A. Welch Foundation, Grant No. A-1526. Austrian Science Fund, FWF project TRP 176-N22