Mixed Quantum Classical Simulations of Charge-Transfer Dynamics in a Model Light-Harvesting Complex. II. Transient Vibrational Analysis

Patel, Kush; Bittner, Eric R.

doi:10.1021/acs.jpcb.0c00203

Cited by 3 publications

(4 citation statements)

References 38 publications

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“…PICT is one of the central reactions that drives solar energy conversion in natural photosynthesis, where the charge-separated state is achieved through multiphoton absorption and involves multiple energy-conversion steps. − Like the natural process, there are many artificial systems in which the photoinduced charge transfer plays a crucial role. − Examples include PICT in dye-sensitized solar cells, − ,− ultrafast charge-transfer in organic photovoltaic systems, − ,,− photocatalytic electron/hole transfer in “colloidal quantum dot-organic molecule complex” interfaces, − and photoinduced proton-coupled electron transfer. − Understanding the detailed charge transfer dynamics will provide valuable mechanistic insights and design principles for next-generation photocatalytic devices and profoundly impact energy production and catalysis.…”

Section: Introductionmentioning

confidence: 99%

“…Our approach uses the fewest switches surface hopping algorithm , to capture the influence of nuclear vibrations on the electronic nonadiabatic transitions, and the single-particle time-dependent Kohn–Sham (TDKS) approach ,, to describe the quantum mechanical state of the transferring electron. With this approach, we investigate the nonadiabatic PICT dynamics in the phthalocyanine dimer/fullerene system ,, and the carotenoid–porphyrin–C 60 (CPC) triad system, ,,,,− which are model systems for understanding the CT dynamics in organic photovoltaics. Our results are in excellent agreement with both experimental measurements and high-level (yet expensive) theoretical calculations.…”

Section: Introductionmentioning

confidence: 99%

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Direct Nonadiabatic Simulations of the Photoinduced Charge Transfer Dynamics

Yamijala

Huo

2021

J. Phys. Chem. A

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We apply direct nonadiabatic dynamics simulations to investigate photoinduced charge transfer reactions. Our approach is based on the mixed quantum-classical fewest switches surface hopping (FSSH) method that treats the transferring electron through time-dependent density functional theory and the nuclei classically. The photoinduced excited state is modeled as a transferring single-electron that initially occupies the LUMO of the donor molecule/moiety. This single-particle electronic wave function is then propagated quantum mechanically by solving the time-dependent Schrodinger equation in the basis of the instantaneous molecular orbitals (MOs) of the entire system. The nonadiabatic transitions among electronic states are modeled using the FSSH approach within the classical-path approximation. We apply this approach to simulate the photoinduced charge transfer dynamics in a few well-characterized molecular systems. Our results are in excellent agreement with both the experimental measurements and high-level (yet expensive) theoretical results.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Direct Nonadiabatic Simulations of the Photoinduced Charge Transfer Dynamics

Yamijala

Huo

2021

J. Phys. Chem. A

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“…[5][6][7] Like the natural process, there are many artificial systems in which the photoinduced charge transfer plays a crucial role. [8][9][10][11][12][13][14][15] Examples include PICT in dye-sensitized solar cells, [8][9][10][11][15][16][17] ultra-fast charge-transfer in organic photovoltaic systems, [12][13][14]18,[18][19][20][21][22][23][24][25] photocatalytic electron/hole transfer in "colloidal quantum dot-organic molecule complex" interfaces, [26][27][28] and photoinduced proton-coupled electron transfer. [29][30][31] Understanding the detailed charge transfer dynamics will provide valuable mechanistic insights and design principles for next-generation photocatalytic devices, and profoundly impact energy production and catalysis.…”

Section: Introductionmentioning

confidence: 99%

“…Our approach uses the fewest switches surface hopping algorithm 32,33 to capture the influence of nuclear vibrations on the electronic nonadiabatic transitions, and the single-particle timedependent Kohn-Sham (TDKS) approach 8,34,35 to describe the quantum mechanical state of the transferring electron. With this approach, we investigate the non-adiabatic PICT dynamics in phthalocyanine dimer/fullerene system 12,18,36 and Carotenoid-Porphyrin-C 60 (CPC) triad system, 13,19,22,23,[37][38][39] which are model systems for understanding the CT dynamics in organic photovoltaics. Our results are in excellent agreement with both experimental measurements and highlevel (yet expensive) theoretical calculations.…”

Section: Introductionmentioning

confidence: 99%

Direct Non-adiabatic Simulations of the Photoinduced Charge Transfer Dynamics

Yamijala¹,

Huo²

2020

Preprint

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We apply direct non-adiabatic dynamics simulations to investigate photoinduced charge transfer reactions. Our approach is based on the mixed quantum-classical fewest switches surface hopping (FSSH) method that treats the transferring electron through time-dependent density functional theory and the nuclei classically. The photoinduced excited state is modeled as a transferring single-electron that initially occupies the LUMO of the donor molecule/moiety. This single-particle electronic wavefunction is then propagated quantum mechanically by solving the time-dependent Schr\"odinger equation in the basis of the instantaneous molecular orbitals (MOs) of the entire system. The non-adiabatic transitions among electronic states are modeled using the FSSH approach within the classical-path approximation. We apply this approach to simulate the photoinduced charge transfer dynamics in a few well-characterized molecular systems. Our results are in excellent agreement with both the experimental measurements and high-level (yet expensive) theoretical results.

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Non-Ionic Surfactants as Boosters for FR Hydration in Brines

Kelley¹,

Fontenot²,

Becktold³

et al. 2023

Day 1 Wed, June 28, 2023

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A theoretical model of polyacrylamide polymers (PAM and PHPA) hydration dynamics is explored, with emphasis on the effect pf salinity on the hydration dynamics of traditional PAM and PHPA polymers. By understanding the interactions at a molecular level between the polymer and the solvent system it is expected that the polymer’s usability as a viscosifying agent can be extended into brackish and possibly produced water. In this study, viscosity vs. time plots are used to find the hydration rates for PAM and PHPA emulsions in fresh water and various brines. Special brines were designed, including one with Fe(III) among components. The study is done by using common, commercial viscometers, utilizing an R1 B1 bob configuration with heated cup. The overall mixing shear generated is low and kept constant throughout the runs. The temperature and length of runs are also kept constant. This allows the determination of the rate limiting hydration step, maximum viscosity and the hydration rates of a wide variety of nonionic surfactants to be explored. By comparing the PAM and PHPA hydration rates for the neat brine, tap water and brine with non-ionic surfactant it is shown that by choosing the correct nonionic surfactant the hydration rates can be increased by over 3500% from the brine solution and more than 10-50% from tap water. It is also shown that the maximum viscosity can be increased by over 700% from the brine solution and 27% from tap water. This trend was also shown to be true using Nano pure water. The results support the theoretical hydration dynamics we propose, showing the effect the nonionic surfactants have on the rate limiting hydration step and transitions between different hydration steps. The data is strong proof that by understanding the processes of polymer hydration, brackish and possibly produced water in a wide range of TDS can be used to successfully hydrate the polymer. The novelty of this testing is that it provides further examples of how non-ionic surfactants can be used successfully to allow PAM and PHPA polymers to be hydrated in brine waters of various compositions with no damage to performance. Care was taken to utilize very common instrumentation and to develop simple and clear procedures for testing, to make the method easy and reliable to use by field labs that may not necessarily have state-of-the-art equipment available.

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Mixed Quantum Classical Simulations of Charge-Transfer Dynamics in a Model Light-Harvesting Complex. II. Transient Vibrational Analysis

Cited by 3 publications

References 38 publications

Direct Nonadiabatic Simulations of the Photoinduced Charge Transfer Dynamics

Direct Nonadiabatic Simulations of the Photoinduced Charge Transfer Dynamics

Direct Non-adiabatic Simulations of the Photoinduced Charge Transfer Dynamics

Non-Ionic Surfactants as Boosters for FR Hydration in Brines

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