Correlated low temperature states of YFe2Ge2 and pressure metallised NiS2

While the free electron model can often be surprisingly successful in describing properties of solids, there are plenty of materials in which interactions between electrons are too significant to be neglected. These strongly correlated systems sometimes exhibit rather unexpected, unusual and useful phenomena, understanding of which is one of the aims of condensed matter physics. Heat capacity measurements of paramagnetic YFe$_{2}$Ge$_{2}$ give a Sommerfeld coefficient of about 100 mJ mol$^{−1}$ K$^{−2}$, which is about an order of magnitude higher than the value predicted by band structure calculations.This suggests the existence of strong electronic correlations in the compound, potentially due to proximity to an antiferromagnetic quantum critical point (QCP). Existence of the latter is also indicated by the non-Fermi liquid T$^{3/2}$ behaviour of the low temperature resistivity. Below 1.8 K a superconducting phase develops in the material, making it a rare case of a non-pnictide and non-chalcogenide iron based superconductor with the 1-2-2 structure. This thesis describes growth and study of a new generation of high quality YFe$_{2}$Ge$_{2}$ samples with residual resistance ratios reaching 200. Measurements of resistivity, heat capacity and magnetic susceptibility confirm the intrinsic and bulk character of the superconductivity, which is also argued to be of an unconventional nature. In order to test the hypothesis of the nearby QCP, resistance measurements under high pressure of up to 35 kbar have been conducted. Pressure dependence of the critical temperature of the superconductivity has been found to be rather weak. μSR measurements have been performed, but provided limited information due to sample inhomogeneity resulting in a broad distribution of the critical temperature. While the superconductivity is the result of an effective attraction between electrons, under different circumstances the electronic properties of a system can instead be dictated by the Coulomb repulsion. This is the case for another transition metal based compound NiS$_{2}$, which is a Mott insulator. Applying hydrostatic pressure of about 30 kbar brings the material across the Mott metal-insulator transition (MIT) into the metallic phase. We have used the tunnel diode oscillator (TDO) technique to measure quantum oscillations in the metallised state of NiS$_{2}$, making it possible to track the evolution of the principal Fermi surface and the associated effective mass as a function of pressure. New results are presented which access a wider pressure range than previous studies and provide strong evidence that the effective carrier mass diverges close to the Mott MIT, as expected within the Brinkman-Rice scenario and predicted in dynamical mean field theory calculations. Quantum oscillations have been measured at pressures as close to the insulating phase as 33 kbar and as high as 97 kbar. In addition to providing a valuable insight into the mechanism of the Mott MIT, this study has also demonstrated the potential of the TDO technique for studying materials at high pressures.EPSRC DTA studentshi

Strong coupling superconductivity in a quasiperiodic host-guest structure.

We examine the low-temperature states supported by the quasiperiodic host-guest structure of elemental bismuth at high pressure, Bi-III. Our electronic transport and magnetization experiments establish Bi-III as a rare example of type II superconductivity in an element, with a record upper critical field of ~ 2.5 T, unusually strong electron-phonon coupling, and an anomalously large, linear temperature dependence of the electrical resistivity in the normal state. These properties may be attributed to the peculiar phonon spectrum of incommensurate host-guest structures, which exhibit additional quasi-acoustic sliding modes, suggesting a pathway toward strong coupling superconductivity with the potential for enhanced transition temperatures and high critical fields

Pressure-tuned quantum criticality in the locally non-centrosymmetric superconductor CeRh2_2As2_2

The unconventional superconductor CeRh$_2$As$_2$ (critical temperature $T_{\mathrm{c}}\approx0.4\,\mathrm{K}$) displays an exceptionally rare magnetic-field-induced transition between two distinct superconducting (SC) phases, proposed to be states of even and odd parity of the SC order parameter, enabled by a locally non-centrosymmetric structure. The SC state exhibits signatures of antiferromagnetism and is preceded by a phase transition of unknown origin at $T_{0}\approx0.5\,\mathrm{K}$. Electronic low-temperature properties of CeRh$_2$As$_2$ show pronounced non-Fermi-liquid behavior, indicative of a proximity to a quantum critical point (QCP). The role of quantum fluctuations and normal state orders for the superconductivity in a system with staggered Rashba interaction is currently an open question, pertinent to explaining the occurrence of two-phase superconductivity. In this work, using measurements of resistivity and specific heat under hydrostatic pressure, we show that the $T_{0}$ order vanishes completely at a modest pressure of $P_{0}=0.5-0.7\,\mathrm{GPa}$, revealing a QCP. The linear temperature dependence of the resistivity at $P_{0}$ evolves into a Fermi-liquid quadratic dependence as the quantum criticality is suppressed by increasing pressure. The dome-like behavior of $T_{\mathrm{c}}$ around $P_{0}$ suggests that the fluctuations of the $T_{0}$ order are involved in the SC pairing mechanism. These results set the scene for further investigations into the fate of the multi-phase superconductivity across this phase diagram.Comment: Submitted simultaneously with the follow-up preprint 2312.0972

Unconventional Superconductivity in the Layered Iron Germanide YFe(2)Ge(2).

The iron-based intermetallic YFe_{2}Ge_{2} stands out among transition metal compounds for its high Sommerfeld coefficient of the order of 100  mJ/(mol K^{2}), which signals strong electronic correlations. A new generation of high quality samples of YFe_{2}Ge_{2} show superconducting transition anomalies below 1.8 K in thermodynamic, magnetic, and transport measurements, establishing that superconductivity is intrinsic in this layered iron compound outside the known superconducting iron pnictide or chalcogenide families. The Fermi surface geometry of YFe_{2}Ge_{2} resembles that of KFe_{2}As_{2} in the high pressure collapsed tetragonal phase, in which superconductivity at temperatures as high as 10 K has recently been reported, suggesting an underlying connection between the two systems.The work was supported by the EPSRC of the UK and by Trinity College. Supporting data can be found at https://www.repository.cam.ac.uk/handle/1810/253875.This is the author accepted manuscript. The final version is available from the American Physical Society via http://dx.doi.org/10.1103/PhysRevLett.116.12700

Truncated mass divergence in a Mott metal

The Mott metal–insulator transition represents one of the most fundamental phenomena in condensed matter physics. Yet, basic tenets of the canonical Brinkman-Rice picture of Mott localization remain to be tested experimentally by quantum oscillation measurements that directly probe the quasiparticle Fermi surface and effective mass. By extending this technique to high pressure, we have examined the metallic state on the threshold of Mott localization in clean, undoped crystals of NiS2. We find that i) on approaching Mott localization, the quasiparticle mass is strongly enhanced, whereas the Fermi surface remains essentially unchanged; ii) the quasiparticle mass closely follows the divergent form predicted theoretically, establishing charge carrier slowdown as the driver for the metal–insulator transition; iii) this mass divergence is truncated by the metal–insulator transition, placing the Mott critical point inside the insulating section of the phase diagram. The inaccessibility of the Mott critical point in NiS2 parallels findings at the threshold of ferromagnetism in clean metallic systems, in which criticality at low temperature is almost universally interrupted by first-order transitions or novel emergent phases such as incommensurate magnetic order or unconventional superconductivity

Supporting data for "Composition dependence of bulk superconductivity in YFe2Ge2"

Data underlying the figures shown in the publication 'Composition dependence of bulk superconductivity in YFe2Ge2', including resistivity and heat capacity versus temperature for different sample qualities, in zero and 2.5 T applied field, resistive transition temperature vs. residual resistivity for a large number of samples, transition temperature and residual resistance ratio vs. nominal composition, lattice parameters vs. nominal composition, and EDS-derived phase content of polycrystalline ingots from with varying nominal composition

Effect of Thermal Cycling on the Structural Evolution of Methylammonium Lead Iodide Monitored around the Phase Transition Temperatures

Optoelectronic devices and solar cells based on organometallic hybrid perovskites have to operate over a broad temperature range, which may contain their structural phase transitions. For instance, the temperature of 330 K, associated with the tetragonal-cubic transformation, may be crossed every day during the operation of solar cells. Therefore, the analysis of thermal cycling effects on structural and electronic properties is of significant importance. This issue is addressed in the case of methylammonium lead iodide (CH3NH3PbI3) across both structural phase transitions (at 160 and 330 K). In situ synchrotron radiation X-ray diffraction (XRD) data recorded between 140 and 180 K show the emergence of a boundary phase between the orthorhombic and tetragonal phases, which becomes more abundant with successive thermal cycles. At high temperatures, around 330 K, an incommensurately modulated tetragonal phase is formed upon repeated crossings of the phase boundary between tetragonal and cubic phases. These alterations, which indicate a gradual evolution of the material under operating conditions of photovoltaic devices, are further documented by electrical resistivity and heat capacity measurements

Research data supporting "Unconventional superconductivity in the layered iron germanide YFe2Ge2"

Data is grouped according to the figures in the publication which it supports. Fig. 1 shows resistivity vs. temperature at various applied magnetic fields in YFe2Ge2, and the .txt datasets give the data underlying this diagram. Fig. 2 shows how resistive superconducting transition temperatures depend on sample quality, as measured by the residual resistance ratio, and the .txt dataset gives the underlying table of data. Fig. 3 shows heat capacity and magnetisation data taken at low temperature, and the .txt datasets give the underlying data, as well as giving the data underlying the theoretical extrapolation curves for temperatures less than 0.4 K. The inset to Fig. 3 shows the dependence of the critical field on temperature, as extracted from resistivity and heat capacity measurements, and the .txt datasets give the underlying data. Figure 1 in the Supplemental Material uses some of the same data as Fig. 3. Methods are described further in the publication.This research data supports “Unconventional superconductivity in the layered iron germanide YFe2Ge2” published in “Physical Review Letters” 116, 127001. Accepted version available at https://www.repository.cam.ac.uk/handle/1810/25399610.1103/PhysRevLett.116.127001This work was supported by the EPSRC [grant number EP/K012894/1]