Damjan Pelc

Determination of the hyperfine magnetic field in magnetic carbon-based materials: DFT calculations and NMR experiments.

The prospect of carbon-based magnetic materials is of immense fundamental and practical importance, and information on atomic-scale features is required for a better understanding of the mechanisms leading to carbon magnetism. Here we report the first direct detection of the microscopic magnetic field produced at 13C nuclei in a ferromagnetic carbon material by zero-field nuclear magnetic resonance (NMR). Electronic structure calculations carried out in nanosized model systems with different classes of structural defects show a similar range of magnetic field values (18–21 T) for all investigated systems, in agreement with the NMR experiments. Our results are strong evidence of the intrinsic nature of defect-induced magnetism in magnetic carbons and establish the magnitude of the hyperfine magnetic field created in the neighbourhood of the defects that lead to magnetic order in these materials.Information on atomic-scale features is required for a better understanding of the mechanisms leading to magnetism in non-metallic, carbon-based materials. This work reports a direct evaluation of the hyperfine magnetic field produced at 13C nuclei in ferromagnetic graphite by nuclear magnetic resonance (NMR). The experimental investigation was made possible by the results of first-principles calculations carried out in model systems, including graphene sheets with atomic vacancies and graphite nanoribbons with edge sites partially passivated by oxygen. A similar range of maximum hyperfine magnetic field values (18-21T) was found for all systems, setting the frequency span to be investigated in the NMR experiments; accordingly, a significant 13C NMR signal was detected close to this range without any external applied magnetic field in ferromagnetic graphite.

Role of microscopic phase separation in gelation of aqueous gelatin solutions

Using a unique home-made cell for four-contact impedance spectroscopy of conductive liquid samples, we establish the existence of two low frequency conductivity relaxations in aqueous solutions of gelatin, in both liquid and gel states. A comparison with diffusion measurements using pulsed field gradient NMR, and circular dichroism spectroscopy, shows that the faster relaxation process is due to gelatin macromolecule self-diffusion. This single molecule diffusion is mostly insensitive to the macroscopic state of the sample, implying that we have a clear separation of gelatin molecules into a free and network-bound phase. Scaling relationships for the self-diffusion indicate that the gelation process is not a percolative phenomenon, but is caused by aggregation of triple helices into a system-spanning fibre network.

Four-contact impedance spectroscopy of conductive liquid samples

We present an improved approach to the impedance spectroscopy of conductive liquid samples using four-electrode measurements. Our method enables impedance measurements of conductive liquids down to the sub-Hertz frequencies, avoiding the electrode polarization effects that usually cripple standard impedance analysers. We have successfully tested our apparatus with aqueous solutions of potassium chloride and gelatin. The first substance has shown flat spectra from ~100 kHz down to sub-Hz range, while the results on gelatin clearly show the existence of two distinct low frequency conductive relaxations.

Contactless measurement of nonlinear conductivity in the radio-frequency range

We have developed a system for contactless measurement of nonlinear conductivity in the radio-frequency band, and over a wide temperature range. A non-resonant circuit is used to electrically excite the sample, and the induced signal is detected by a resonant circuit whose natural frequency matches higher harmonics of the excitation. A simple modification of the probe allows non-resonant detection suitable for stronger signals. Two measurement procedures are proposed that allow significant excitation power variation, up to 150 W. The apparatus has been validated through the measurement of the nonlinear response at the superconducting transition of a high-Tc superconductor, and the nematic transition of an iron pnictide.

17 O-NMR Knight shift study of the interplay between superconductivity and pseudogap in (Cax La1-x)(Ba1.75-x La0.25+x) Cu3 Oy

We report systematic 17O-NMR measurements on the high-Tc cuprate (Ca_xLa_1−x )(Ba_1.75−xLa_0.25+x )Cu_3O_y , for four different families (differen

Effective numbers of charge carriers in doped graphene: Generalized Fermi liquid approach

The single-band current-dipole Kubo formula for the dynamical conductivity of heavily doped graphene from Kupcic [Phys. Rev. B 91, 205428 (2015)] is extended to a two-band model for conduction pi electrons in lightly doped graphene. Using a posteriori relaxation-time approximation in the two-band quantum transport equations, with two different relaxation rates and one quasi-particle lifetime, we explain a seemingly inconsistent dependence of the dc conductivity of ultraclean and dirty lightly doped graphene samples on electron doping, in a way consistent with the charge continuity equation. It is also shown that the intraband contribution to the effective number of conduction electrons in the dc conductivity vanishes at T=0 K in the ultraclean regime, but it remains finite in the dirty regime. The present model is shown to be consistent with a picture in which the intraband and interband contributions to the dc conductivity are characterized by two different mobilities of conduction electrons, the values of which are well below the widely accepted value of mobility in ultraclean graphene. The dispersions of Dirac and pi plasmon resonances are reexamined to show that the present, relatively simple expression for the dynamical conductivity tensor can be used to study simultaneously single-particle excitations in the dc and optical conductivity and collective excitations in energy loss spectroscopy experiments.

Unconventional charge order in a co-doped high-Tc superconductor

Charge-stripe order has recently been established as an important aspect of cuprate high-Tc superconductors. However, owing to the complex interplay between competing phases and the influence of disorder, it is unclear how it emerges from the parent high-temperature state. Here we report on the discovery of an unconventional ordered phase between charge-stripe order and (pseudogapped) metal in the cuprate La1.8−xEu0.2SrxCuO4. We use three complementary experiments—nuclear quadrupole resonance, nonlinear conductivity and specific heat—to demonstrate that the order appears through a sharp phase transition and exists in a dome-shaped region of the phase diagram. Our results imply that the new phase is a state, which preserves translational symmetry: a charge nematic. We thus resolve the process of charge-stripe development in cuprates, show that this nematic phase is distinct from high-temperature pseudogap and establish a link with other strongly correlated electronic materials with prominent nematic order.

Mechanism of metallization and superconductivity suppression in YBa2(Cu0.97 Zn0.03)3 O6.92 revealed by 67Zn NQR

We measure the nuclear quadrupole resonance signal on the Zn site in nearly optimally doped YBa2Cu3O6.92, when Cu is substituted by 3% of isotopically pure 67Zn. We observe that Zn creates large insulating islands, confirming two earlier conjectures: that doping provokes an orbital transition in the CuO2 plane, which is locally reversed by Zn substitution, and that the islands are antiferromagnetic. Also, we find that the Zn impurity locally induces a breaking of the D4 symmetry. Cluster and DFT calculations show that the D4 symmetry breaking is due to the same partial lifting of degeneracy of the nearest-neighbor oxygen sites as in the LTT transition in BaxCuO4, similarly well-known to strongly suppress superconductivity (SC). These results show that in-plane oxygen 2p5 orbital configurations are principally involved in the metallicity and SC of all high-Tc cuprates, and provide a qualitative symmetry-based constraint on the SC mechanism.

Cu nuclear magnetic resonance study of charge and spin stripe order in La1.875Ba0.125CuO4

In this paper, we present a Cu nuclear magnetic/quadrupole resonance study of the charge stripe ordered phase of LBCO, with detection of previously unobserved (“wiped-out”) signal. We show that spin-spin and spin-lattice relaxation rates are strongly enhanced in the charge ordered phase, explaining the apparent signal decrease in earlier investigations. The enhancement is caused by magnetic, rather than charge fluctuations, conclusively confirming the long-suspected assumption that spin fluctuations are responsible for the wipeout effect. Observation of the full Cu signal enables insight into the spin and charge dynamics of the stripe-ordered phase, and measurements in external magnetic fields provide information on the nature and suppression of spin fluctuations associated with charge order. Lastly, we find glassy spin dynamics, in agreement with previous work, and incommensurate static charge order with charge modulation amplitude similar to other cuprate compounds, suggesting that the amplitude of charge stripes is universal in the cuprates.

Cooperative mercury motion in the ionic conductor Cu2HgI4.

We present the observation of glasslike dynamic correlations of mobile mercury ions in the ionic conductor Cu2HgI4, detected in both NMR and nonlinear conductivity experiments. The results show that dynamic cooperativity appears in systems seemingly unrelated to glassy and soft arrested materials. A simple kinetic two-component model is proposed, which seems to provide a good description of the cooperative ionic dynamics.