When a semiconductor absorbs light, the resulting electron-hole superposition amounts to a uncontrolled quantum ripple that eventually degenerates into diffusion. If the conformation of these excitonic superpositions could be engineered, though, they would constitute a new means of transporting information and energy. We show that properly designed laser pulses can be used to create such excitonic wave packets. They can be formed with a prescribed speed, direction and spectral make-up that allows them to be selectively passed, rejected or even dissociated using superlattices. Their coherence also provides a handle for manipulation using active, external controls. Energy and information can be conveniently processed and subsequently removed at a distant site by reversing the original procedure to produce a stimulated emission. The ability to create, manage and remove structured excitons comprises the foundation for opto-excitonic circuits with application to a wide range of quantum information, energy and light-flow technologies. The paradigm is demonstrated using both Tight-Binding and Time-Domain Density Functional Theory simulations.

A first principles, excited state analysis is carried out to identify ways of producing silicon quantum dots with low excitonic reorganization energy. These focus on the general strategy of either reducing or constraining exciton-phonon coupling, and four approaches are explored. The results can be implemented in quantum dot solids to mitigate polaronic effects and increase the lifetime of coherent excitonic superpositions. It is demonstrated that such designs can also be used to alter the shape of the spectral density for reorganization so as to reduce the rates of both decoherence and dissipation. The results suggest that it may be possible to design quantum dot solids that support partially coherent exciton transport.

Molecules with C N or C N h symmetry can absorb quanta of optical angular momentum to generate twisted excitons with well-defined quasi-angular momenta of their own. Angular momentum is conserved in such interactions at the level of a paraxial approximation for the light beam. A sequence of absorption events can thus be used to create a range of excitonic angular momenta.Subsequent decay can produce radiation with a single angular momentum equal to that accumulated. Such molecules can thus be viewed as mediators for changing the angular momentum of light. This sidesteps the need to exploit nonlinear light-matter interactions based on higher-order susceptibilities. A tight-binding paradigm is used to verify angular momentum conservation and demonstrate how it can be exploited to change the angular momentum of light. The approach is then extended to a time-dependent density functional theory setting where the key results are shown to hold in a many-body, multi-level setting.

Topological phases of matter are conventionally characterized by the bulk-boundary correspondence in Hermitian systems. The topological invariant of the bulk in d dimensions corresponds to the number of (d − 1) -dimensional boundary states. By extension, higher-order topological insulators reveal a bulk-edge-corner correspondence, such that nth order topological phases feature (d − n)-dimensional boundary states. The advent of non-Hermitian topological systems sheds new light on the emergence of the non-Hermitian skin effect (NHSE) with an extensive number of boundary modes under open boundary conditions. Still, the higher-order NHSE remains largely unexplored, particularly in the experiment. An unsupervised approach-physics-graph-informed machine learning (PGIML)-to enhance the data mining ability of machine learning with limited domain knowledge is introduced. Through PGIML, the second-order NHSE in a 2D non-Hermitian topoelectrical circuit is experimentally demonstrated. The admittance spectra of the circuit exhibit an extensive number of corner skin modes and extreme sensitivity of the spectral flow to the boundary conditions. The violation of the conventional bulk-boundary correspondence in the second-order NHSE implies that modification of the topological band theory is inevitable in higher dimensional non-Hermitian systems.

Peripheral surface functionalization of hydrideterminated silicon quantum dots (SiQD) is necessary in order to minimize their oxidation/aggregation and allow for solution processability. Historically thermal hydrosilylation addition of alkenes and alkynes across the Si−H surface to form Si−C bonds has been the primary method to achieve this. Here we demonstrate a mild alternative approach to functionalize hydride-terminated SiQDs using bulky silanols in the presence of free-radical initiators to form stable siloxane (∼Si−O−SiR 3 ) surfaces with hydrogen gas as a byproduct. This offers an alternative to existing methods of forming siloxane surfaces that require corrosive Si−Cl based chemistry with HCl byproducts. A 52 nm blue shift in the photoluminescent spectra of siloxane versus alkyl-functionalized SiQDs is observed that we explain using computational theory. Model compound synthesis of silane and silsesquioxane analogues is used to optimize surface chemistry and elucidate reaction mechanisms. Thorough characterization on the extent of siloxane surface coverage is provided using FTIR and XPS. TEM is used to demonstrate SiQD size and integrity after surface chemistry and product isolation.