Natural light-harvesting systems spatially organize densely packed dyes in different configurations to either transport excitons or convert them into charge photoproducts, with high efficiency. In contrast, artificial photosystems like organic solar cells and light-emitting diodes lack this fine structural control, limiting their efficiency. Thus, biomimetic multi-dye systems are needed to organize dyes with the sub-nanometer spatial control required to sculpt resulting photoproducts.
View Article and Find Full Text PDFStrongly-coupled multichromophoric assemblies orchestrate the absorption, transport, and conversion of photonic energy in natural and synthetic systems. Programming these functionalities involves the production of materials in which chromophore placement is precisely controlled. DNA nanomaterials have emerged as a programmable scaffold that introduces the control necessary to select desired excitonic properties.
View Article and Find Full Text PDFIn this manuscript, we examine design strategies for the development of excitonic circuits that are capable of performing simple 2-qubit multi-step quantum algorithms. Specifically, we compare two different strategies for designing dye-based systems that prescribe exciton evolution encoding a particular quantum algorithm. A serial strategy implements the computation as a step-by-step series of circuits, with each carrying out a single operation of the quantum algorithm, and a combined strategy implements the entire computation in a single circuit.
View Article and Find Full Text PDFPhys Chem Chem Phys
February 2020
This manuscript presents a strategy for controlling the transformation of excitonic states through the design of circuits made up of coupled organic dye molecules. Specifically, we show how unitary transformation matrices can be mapped to the Hamiltonians of physical systems of dye molecules with specified geometric and chemical properties. The evolution of these systems over specific time scales encodes the action of the unitary transformation.
View Article and Find Full Text PDFWe proposed a methodology that allows to maximize the population transfer from a high vibrational state of the Σ triplet state to the vibrational ground state of the Σ singlet state though the optimization of one pump and one dump laser pulses. The pump pulse is optimized using a fitness function, heuristically improved, that includes the effect of the spin-orbit coupling of the KRb [b-A]-scheme. The dump pulse is optimized to maximize the population transfer to the ground state.
View Article and Find Full Text PDFWe apply a real-time path-integral approach to investigate the charge-transfer (CT)-mediated singlet fission quantum dynamics in a model pentacene dimer. Our path-integral method gives reliable fission dynamics across various reaction regimes as well as a broad range of reorganization energies and temperatures. With this method, we investigated the destructive interference between the two CT-mediated fission pathways and discovered two mechanisms that can suppress this deleterious effect.
View Article and Find Full Text PDFPurpose: To evaluate ocular outcome in premature infants treated with intravitreal ranibizumab injections for retinopathy of prematurity (ROP) over a period of 3 years.
Methods: An interventional case series. Premature infants with high-risk prethreshold or threshold ROP with plus disease received an off label monotherapy with intravitreal injections of ranibizumab.
Purpose: To evaluate the physiological and behavioral pain response in premature infants receiving intravitreal bevacizumab injection (IVB) for retinopathy of prematurity (ROP) under topical anesthesia.
Methods: A prospective interventional non-comparative case series. Premature infants with high-risk prethreshold or threshold ROP received IVB using topical anesthesia with tetracaine eye drops.