Dr Joseph Prentice

Abstract:

When calculating the optical absorption spectra of molecular crystals from first principles, the influence of the crystalline environment on the excitations is of significant importance. For such systems, however, methods to describe the excitations accurately can be computationally prohibitive due to the relatively large system sizes involved. In this work, we demonstrate a method that allows optical absorption spectra to be computed both efficiently and at high accuracy. Our approach is based on the spectral warping method successfully applied to molecules in solvent. It involves calculating the absorption spectrum of a supercell of the full molecular crystal using semi-local time-dependent density functional theory (TDDFT), before warping the spectrum using a transformation derived from smaller-scale semi-local and hybrid TDDFT calculations on isolated dimers. We demonstrate the power of this method on three polymorphs of the well-known color polymorphic compound ROY and find that it outperforms both small-scale hybrid TDDFT dimer calculations and large-scale semi-local TDDFT supercell calculations, when compared to the experiment.

Abstract:

Strain is a powerful experimental tool to explore new electronic states and understand unconventional superconductivity. Here, we investigate the effect of uniaxial strain on the nematic and superconducting phase of single crystal FeSe using magnetotransport measurements. We find that the resistivity response to the strain is strongly temperature dependent and it correlates with the sign change in the Hall coefficient being driven by scattering, coupling with the lattice and multiband phenomena. Band structure calculations suggest that under strain the electron pockets develop a large in-plane anisotropy as compared with the hole pocket. Magnetotransport studies at low temperatures indicate that the mobility of the dominant carriers increases with tensile strain. Close to the critical temperature, all resistivity curves at constant strain cross in a single point, indicating a universal critical exponent linked to a strain-induced phase transition. Our results indicate that the superconducting state is enhanced under compressive strain and suppressed under tensile strain, in agreement with the trends observed in FeSe thin films and overdoped pnictides, whereas the nematic phase seems to be affected in the opposite way by the uniaxial strain. By comparing the enhanced superconductivity under strain of different systems, our results suggest that strain on its own cannot account for the enhanced high $T_c$ superconductivity of FeSe systems.