Efficiency Limits of Solar Energy Harvesting via Internal Photoemission in Carbon Materials

We describe strategies to estimate the upper limits of the efficiency of photon energy harvesting via hot electron extraction from gapless absorbers. Gapless materials such as noble metals can be used for harvesting the whole solar spectrum, including visible and near-infrared light. The energy of photo-generated non-equilibrium or hot charge carriers can be harvested before they thermalize with the crystal lattice via the process of their internal photo-emission (IPE) through the rectifying Schottky junction with a semiconductor. However, the low efficiency and the high cost of noble metals necessitates the search for cheaper abundant alternative materials, and we show here that carbon can serve as a promising IPE material candidate. We compare the upper limits of performance of IPE photon energy-harvesting platforms, which incorporate either gold or carbon as the photoactive material where hot electrons are generated. Through a combination of density functional theory, joint electron density of states calculations, and Schottky diode efficiency modeling, we show that the material electron band structure imposes a strict upper limit on the achievable efficiency of the IPE devices. Our calculations reveal that graphite is a good material candidate for the IPE absorber for harvesting visible and near-infrared photons. Graphite electron density of states yields a sizeable population of hot electrons with energies high enough to be collected across the potential barrier. We also discuss the mechanisms that prevent the IPE device efficiency from reaching the upper limits imposed by their material electron band structures. The proposed approach is general and allows for efficient pre-screening of materials for their potential use in IPE energy converters and photodetectors within application-specific spectral windows.

Micro/nanoscale thermal transport by phonons beyond the relaxation time approximation: Greens function with the full scattering matrix

The phonon Boltzmann transport equation (BTE) has been widely utilized to study thermal transport in materials within the relaxation time approximation (RTA). However, the RTA limits the study to materials for which this mean field scattering assumption is a valid approximation, preventing the study of a wider class of materials, including graphene and diamond. Here we develop a Greens function solution of the linearized BTE for an arbitrary distribution of heat sources in an unbounded medium, which includes the full scattering matrix, and provide an analytical expression for the temperature distribution. We provide a condition on the scattering matrix to satisfy energy conservation simply in terms of the phonon frequencies, group velocities, and mode specific heat. We provide numerical calculations for graphene for the particular geometry of a spatially sinusoidal heating profile to highlight the importance of using the full scattering matrix compared to the RTA.

Phonon Hydrodynamic Heat Conduction and Knudsen Minimum in Graphite

In the hydrodynamic regime, phonons drift with a nonzero collective velocity under a temperature gradient, reminiscent of viscous gas and fluid flow. The study of hydrodynamic phonon transport has spanned over half a century but has been mostly limited to cryogenic temperatures (~1 K) and more recently to low-dimensional materials. Here, we identify graphite as a three-dimensional material that supports phonon hydrodynamics at significantly higher temperatures (~100 K) based on first-principles calculations. In particular, by solving the Boltzmann equation for phonon transport in graphite ribbons, we predict that phonon Poiseuille flow and Knudsen minimum can be experimentally observed above liquid nitrogen temperature. Further, we reveal the microscopic origin of these intriguing phenomena in terms of the dependence of the effective boundary scattering rate on momentum-conserving phonon-phonon scattering processes and the collective motion of phonons. The significant hydrodynamic nature of phonon transport in graphite is attributed to its strong intralayer sp2 hybrid bonding and weak van der Waals interlayer interactions. As a boundary-sensitive transport regime, phonon hydrodynamics opens up new possibilities for thermal management and energy conversion.

The Non-Perturbative Quantum Nature of the Dislocation-Phonon Interaction

Despite the long history of dislocation-phonon interaction studies, there are many problems that have not been fully resolved during this development. These include an incompatibility between a perturbative approach and the long-range nature of a dislocation, the relation between static and dynamic scattering, and the nature of dislocation-phonon resonance. Here by introducing a fully quantized dislocation field, the dislon[1], a phonon is renormalized as a quasi-phonon, with shifted quasi-phonon energy, and accompanied by a finite quasi-phonon lifetime that is reducible to classical results. A series of outstanding legacy issues including those above can be directly explained within this unified phonon renormalization approach. In particular, a renormalized phonon naturally resolves the decades-long debate between dynamic and static dislocation-phonon scattering approaches.