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Your search keyword '"Paisley, Nathan R."' showing total 23 results
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23 results on '"Paisley, Nathan R."'

1. Estimating Phosphorescent Emission Energies in Ir(III) Complexes using Large-Scale Quantum Computing Simulations

Author

Genin, Scott N., Ryabinkin, Ilya G., Paisley, Nathan R., Whelan, Sarah O., Helander, Michael G., and Hudson, Zachary M.

Subjects
Quantum Physics, Physics - Chemical Physics
Abstract

Quantum chemistry simulations that accurately predict the properties of materials are among the most highly anticipated applications of quantum computing. It is widely believed that simulations running on quantum computers will allow for higher accuracy, but there has not yet been a convincing demonstration that quantum methods are competitive with existing classical methods at scale. Here we apply the iterative qubit coupled cluster (iQCC) method on classical hardware to the calculation of the $T_1 \to S_0$ transition energies in nine phosphorescent iridium complexes, to determine if quantum simulations have any advantage over traditional computing methods. Phosphorescent iridium complexes are integral to the widespread commercialization of organic light-emitting diode (OLED) technology, yet accurate computational prediction of their emission energies remains a challenge. Our simulations would require a gate-based quantum computer with a minimum of 72 fully-connected and error-corrected logical qubits. Since such devices do not yet exist, we demonstrate the iQCC quantum method using a special purpose quantum simulator on classical hardware. The results are compared to a selection of common density-functional theory (DFT) functionals (B3LYP, CAM-B3LYP, LC-wHPBE), ab initio methods (HF and MP2), and experimental data. The iQCC quantum method is found to match the accuracy of the fine-tuned DFT functionals, has a better Pearson correlation coefficient, and still has considerable potential for systematic improvement. Based on these results, we anticipate that the iQCC quantum method will have the required accuracy to design organometallic complexes when deployed on emerging quantum hardware., Comment: Supplementary is added

Published
2021
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5. Red and near-infrared luminescent materials for biological imaging

Author

Paisley, Nathan R.

Abstract

Fluorescence imaging is a critical tool for visualizing cellular structures and complex biological processes; however, background autofluorescence from molecules and structures within the cell can severely reduce the signal-to-noise ratio (SNR) and imaging quality. Time-resolved imaging (TRI) and two-photon excited fluorescence (2PEF) microscopy are two techniques that can be used to remove background autofluorescence and improve SNR. Imaging probes with long lifetime emission are required to utilize TRI techniques. Purely organic materials with properties such as thermally activated delayed fluorescence (TADF) exhibit long lifetime photoluminescence. Additionally, to image living samples, luminescent imaging probes should ideally absorb and emit within the biological transparency window (650���1350 nm), but efficient TADF emission within this range is rare. Work described in this thesis uses materials exhibiting TADF or 2PEF to develop biological imaging probes with emission within the biological transparency window. These materials were synthesized as small molecules or polymerized with a semiconductor host and formed into polymer nanoparticles called polymer dots (Pdots) that retain the photophysical properties required for TRI or 2PEF microscopy. New deep-red/near-infrared (NIR) emissive TADF monomers were synthesized and the mechanism behind TADF was explored using density functional theory (DFT). Pdots with a cell-penetrating peptide mimic shell were demonstrated to efficiently enter multiple cell lines in under 30 minutes while retaining high cell viability. Proof-of-concept experiments for the use of these Pdots in TRI demonstrated that the TADF emission can be separated from background fluorescence. This work represents some of the first demonstrations of Pdots containing red to NIR emissive TADF polymers for cellular imaging. For materials exhibiting 2PEF, it was shown that the electron donor moieties effect on planarity directly correlates to the relative strength of 2PEF within a series. Additionally, in the closely related field of semiconductor polymers, reactive semifluorinated polymers were investigated for the efficient synthesis of a series of polymers based on p-type and n-type semiconductor motifs commonly found in organic light-emitting diodes (OLEDs), organic thin-film transistors (OTFTs), and organic photovoltaics (OPVs). Experiments demonstrating that semifluorinated polymers can provide a useful building block in the synthesis of organic electronic materials were conducted.

Published
2022
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13. Estimating Phosphorescent Emission Energies in IrIII Complexes Using Large‐Scale Quantum Computing Simulations**.

Author

Genin, Scott N., Ryabinkin, Ilya G., Paisley, Nathan R., Whelan, Sarah O., Helander, Michael G., and Hudson, Zachary M.

Subjects
QUANTUM computing, PHOSPHORESCENCE, QUANTUM computers, QUBITS, FUNCTIONALS, LIGHT emitting diodes, QUANTUM gates
Abstract

Here we calculate T1→S0 transition energies in nine phosphorescent iridium complexes using the iterative qubit coupled cluster (iQCC) method to determine if quantum simulations have any advantages over classical methods. These simulations would require a gate‐based quantum computer with at least 72 fully‐connected logical qubits. Since such devices do not yet exist, we demonstrate the iQCC method using a purpose‐built quantum simulator on classical hardware. The results are compared to a selection of common DFT functionals, ab initio methods, and empirical data. iQCC is found to match the accuracy of the best DFT functionals, but with a better correlation coefficient, demonstrating that it is better at predicting the structure–property relationship. Results indicate that the iQCC method has the required accuracy to design organometallic complexes when deployed on emerging quantum hardware and sets an industrially relevant target for demonstrating quantum advantage. [ABSTRACT FROM AUTHOR]

Published
2022
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