arXiv subjects

Jonathan Tollerud

Publications and source records attributed to Jonathan Tollerud.

3 recordsLinked to original sources

arXiv2021

Direct Measurement of Biexcitons in Monolayer WS2

The optical properties of atomically thin transition metal dichalcogenides (TMDCs) are dominated by Coulomb bound quasi-particles, such as excitons, trions, and biexcitons. Due to the number and density of possible states, attributing different spectral peaks to the specific origin can be difficult. In particular, there has been much conjecture around the presence, binding energy and/or nature of biexcitons in these materials. In this work, we remove any ambiguity in identifying and separating the optically excited biexciton in monolayer WS2 using two-quantum multidimensional coherent spectroscopy (2Q-MDCS), a technique that directly and selectively probes doubly-excited states, such as biexcitons. The energy difference between the unbound two-exciton state and the biexciton is the fundamental definition of biexciton binding energy and is measured to be 26 \pm 2 meV. Furthermore, resolving the biexciton peaks in 2Q-MDCS allows us to identify that the biexciton observed here is composed of two bright excitons in opposite valleys.

cond-mat.mes-hall↗

arXiv2017

Time-domain THz spectroscopy reveals coupled protein-hydration dielectric response in solutions of native and fibrils of human lyso-zyme

Here we reveal details of the interaction between human lysozyme proteins, both native and fibrils, and their water environment by intense terahertz time domain spectroscopy. With the aid of a rigorous dielectric model, we determine the amplitude and phase of the oscillating dipole induced by the THz field in the volume containing the protein and its hydration water. At low concentrations, the amplitude of this induced dipolar response decreases with increasing concentration. Beyond a certain threshold, marking the onset of the interactions between the extended hydration shells, the amplitude remains fixed but the phase of the induced dipolar response, which is initially in phase with the applied THz field, begins to change. The changes observed in the THz response reveal protein-protein interactions me-diated by extended hydration layers, which may control fibril formation and may have an important role in chemical recognition phenomena.

physics.bio-ph↗

arXiv2017

Separating Pathways in Double-Quantum Optical Spectroscopy Reveals Excitonic Interactions

Techniques for coherent multidimensional optical spectroscopy have been developed and utilised to understand many different processes, including energy transfer in photosynthesis and many-body effects in semiconductor nanostructures. Double-quantum 2D spectroscopy is one variation that has been particularly useful for understanding many-body effects. In condensed matter systems, however, there are often many competing signal pathways, which can make it difficult to isolate different contributions and retrieve quantitative information. Here, a means of separating overlapping pathways while maintaining the fidelity of the relevant peak/s is demonstrated. This selective approach is used to isolate the double-quantum signal from a mixed two exciton state in a semiconductor quantum well. The removal of overlapping peaks allows analysis of the relevant peak-shape and thus details of interactions with the environment and other carriers to be revealed. An alternative pulse ordering identifies a double-quantum state associated only with GaAs defects, the signature of which has previously been confused with other interaction induced effects. The experimental approach described here provides access to otherwise hidden details of excitonic interactions and demonstrates that the manner in which the double-quantum coherence is generated can be important and provide an additional control to help understand the many-body physics in complex systems.

physics.optics↗