An automated quantum chemistry-driven, experimental characterization for high PCE donor–π–acceptor NIR molecular dyes

Santaloci, Taylor J.; Meador, William E.; Wallace, Austin M.; Valencia, E.; Rogers, Blake N.; Delcamp, Jared H.; Fortenberry, Ryan C.

doi:10.1039/d3dd00023k

Cited by 2 publications

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References 100 publications

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“…The PESs needed to provide bases for anharmonic vibrational frequency computations or rotational constant generation are coarsely parallel computations that can be spread over as many compute nodes as available. , Hence, reasonable molecular selections each containing 10 or so atoms can have their anharmonic fundamental vibrational frequencies computed to the accuracies listed above (∼<2%; enough for experimental comparison) in a matter of days with a modest high-performance computing cluster . The software needed to create the PES, run the computations, and analyze the results independently of a human user has also been developed and is available for utilization. ,, Furthermore, recent work in the area of energy science has established a means of automating molecular structure generation from combinations of predetermined ligands and backbones . As such, full automation and even prediction for whole classes of molecules of astrochemical interest is on the horizon.…”

Section: The Future Of Quantum Chemistry In Astrochemistrymentioning

confidence: 99%

Quantum Chemistry and Astrochemistry: A Match Made in the Heavens

Fortenberry

2024

J. Phys. Chem. A

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Quantum chemistry can uniquely answer astrochemical questions that no other technique can provide. Computations can be parallelized, automated, and left to run continuously providing exceptional molecular throughput that cannot be done through experimentation. Additionally, the granularity of the individual computations that are required of potential energy surfaces, reaction mechanism pathways, or other quantum chemically derived observables produces a unique mosaic that make up the larger whole. These pieces can be dissected for their individual contributions or evaluated in an ad hoc fashion for each of their roles in generating the larger whole. No other scientific approach is capable of reporting such fine-grained insights. Quantum chemistry also works from a bottom-up approach in providing properties directly from the desired molecule instead of a top-down perspective as required of experiment where molecules have to be linked to observed phenomena. Furthermore, modern quantum chemistry is well within the range of "chemical accuracy" and is approaching "spectroscopic accuracy." As such, the seemingly difficult questions asked by astrochemistry that would not be asked initially for any other application require quantum chemical reference data. While the results of quantum chemical computations are needed to interpret astrochemical observation, modeling, or laboratory experimentation, such hard questions, regardless of the original need to answer them, produce unique solutions. While questions in astrochemistry often require novel developments in and implementations of quantum chemistry as outlined herein, the applications of these solutions will stretch beyond astrochemistry and may yet impact fields much closer to Earth.

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Section: The Future Of Quantum Chemistry In Astrochemistrymentioning

confidence: 99%

Quantum Chemistry and Astrochemistry: A Match Made in the Heavens

Fortenberry

2024

J. Phys. Chem. A

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“…Again, as hardware like GPUs and even quantum computing technology develops, dedicated, stochastic approaches could “brute force” their way through thousands of molecules in a similar fashion especially though the use of dedicated backbones and functional groups linked together with SMILES strings which can construct molecules with single-line computational syntax. Of course, larger molecules like PAHs will require even lower-levels of theory than DFT can provide in order to reach the needed level of throughput for scratching the surface of JWST (much less LUVOIR) data, and ongoing work is parametrizing semiempirical methods to this effect through automated, explicitly anharmonic computations trying to solve the future problem of PAHs as alluded to previously. − …”

Section: The 2050 Horizonmentioning

confidence: 99%

A Vision for the Future of Astrochemistry in the Interstellar Medium by 2050

Fortenberry

2023

ACS Phys. Chem Au

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By 2050, many, but not nearly all, unattributed astronomical spectral features will be conclusively linked to molecular carriers (as opposed to nearly none today in the visible and IR); amino acids will have been observed remotely beyond our solar system; the largest observatories ever constructed on the surface of the Earth or launched beyond it will be operational; high-throughput computation either from brute force or machine learning will provide unprecedented amounts of reference spectral and chemical reaction data; and the chemical fingerprints of the universe delivered by those of us who call ourselves astrochemists will provide astrophysicists with unprecedented resolution for determining how the stars evolve, planets form, and molecules that lead to life originate. Astrochemistry is a relatively young field, but with the entire universe as its playground, the discipline promises to persist as long as telescopic observations are made that require reference data and complementary chemical modeling. While the recent commissionings of the James Webb Space Telescope and Atacama Large Millimeter Array are ushering in the second "golden age" of astrochemistry (with the first being the radio telescopic boom period of the 1970s), this current period of discovery should facilitate unprecedented advances within the next 25 years. Astrochemistry forces the asking of hard questions beyond the physical conditions of our "pale blue dot", and such questions require creative solutions that are influential beyond astrophysics. By 2050, more creative solutions will have been provided, but even more will be needed to answer the continuing question of our astrochemical ignorance.

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An automated quantum chemistry-driven, experimental characterization for high PCE donor–π–acceptor NIR molecular dyes

Abstract: A readily accessible (less than four synthetic steps) dye molecule with potential properties well-beyond the current state-of-the-art for use in dye-sensitized solar cells (DSCs) is realized from extensive quantum chemical...

Cited by 2 publications

References 100 publications

Quantum Chemistry and Astrochemistry: A Match Made in the Heavens

Quantum Chemistry and Astrochemistry: A Match Made in the Heavens

A Vision for the Future of Astrochemistry in the Interstellar Medium by 2050

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