Professor Robert Taylor

Abstract:

We demonstrate with an experiment how molecules are a natural test bed for probing fundamental quantum thermodynamics. Single-molecule spectroscopy has undergone transformative change in the past decade with the advent of techniques permitting individual molecules to be distinguished and probed. We demonstrate that the quantum Jarzynski equality for heat is satisfied in this set-up by considering the time-resolved emission spectrum of organic molecules as arising from quantum jumps between states. This relates the heat dissipated into the environment to the free energy difference between the initial and final state. We demonstrate also how utilizing the quantum Jarzynski equality allows for the detection of energy shifts within a molecule, beyond the relative shift.

Abstract:

Photosynthetic organisms rely on a series of self-assembled nanostructures with tuned electronic energy levels in order to transport energy from where it is collected by photon absorption, to reaction centers where the energy is used to drive chemical reactions. In the photosynthetic bacteria Chlorobaculum tepidum, a member of the green sulfur bacteria family, light is absorbed by large antenna complexes called chlorosomes to create an exciton. The exciton is transferred to a protein baseplate attached to the chlorosome, before migrating through the Fenna-Matthews-Olson complex to the reaction center. Here, it is shown that by placing living Chlorobaculum tepidum bacteria within a photonic microcavity, the strong exciton-photon coupling regime between a confined cavity mode and exciton states of the chlorosome can be accessed, whereby a coherent exchange of energy between the bacteria and cavity mode results in the formation of polariton states. The polaritons have energy distinct from that of the exciton which can be tuned by modifying the energy of the optical modes of the microcavity. It is believed that this is the first demonstration of the modification of energy levels within living biological systems using a photonic structure.

Abstract:

Due to its unique layer-number dependent electronic band structure and strong excitonic features, atomically thin MoS2 is an ideal 2D system where intriguing photoexcited-carrier-induced phenomena can be detected in excitonic luminescence. We perform micro-photoluminescence (PL) measurements and observe that the PL peak redshifts nonlinearly in mono- and bi-layer MoS2 as the excitation power is increased. The excited carrier-induced optical bandgap shrinkage is found to be proportional to n4/3, where n is the optically-induced free carrier density. The large exponent value of 4/3 is explicitly distinguished from a typical value of 1/3 in various semiconductor quantum well systems. The peculiar n4/3 dependent optical bandgap redshift may be due to the interplay between bandgap renormalization and reduced exciton binding energy.