Center for Functional Nanomaterials Seminar

We present electronic structure calculations of Pu using density functional theory in conjunction with the dynamical mean-field theory (DMFT). The newly developed continuous time quantum Monte-Carlo technique is used to solve DMFT impurity problem without approximation, including the full rotationally invariant exchange interaction. We predict various properties, such as the photoemission spectra, heat capacity, and magnetic susceptibility, as a function of temperature, pressure, and crystal structure. The sensitivity of the results to the on-site exchange interaction and the number of electrons in the f-shell is explored. We predict that delta-Pu has a Pauli-like magnetic susceptibility near ambient temperature, as in experiment, indicating that electronic coherence causes the absence of local moments. Additionally, we show that volume expansion causes a crossover from incoherent to coherent electronic behavior at increasingly lower temperatures.