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Distance dependence of triplet energy transfer in water and organic solvents: A QM/MD study

The possibility to optimize optoelectronic devices, such as organic light-emitting diodes or solar cells, by exploiting the special characteristics of triplet electronic states and their migration ability is attracting increased attention. In this study, we analyze how an intervening solvent modifies the distance dependence of triplet electronic energy transfer (TEET) processes by combining molecular dynamics simulations with quantum chemical calculations of the transfer matrix elements using the Fragment Excitation Difference (FED) method. We determine the β parameter characterizing the exponential distance decay of TEET rates in a stacked perylene dimer in water, chloroform, and benzene solutions. Our results indicate that the solvent dependence of β (β vacuum = 5.14 Å -1 > β water = 3.77 Å -1 > β chloroform = 3.61 Å -1 > β benzene = 3.44 Å -1) can be rationalized adopting the McConnell model of superexchange, where smaller triplet energy differences between the donor and the solvent lead to smaller β constants. We also estimate the decay of hole transfer (HT) and excess electron transfer (EET) processes in the system using the Fragment Charge Difference (FCD) method and find that β TEET can be reasonably well approximated by the sum of β EET and β HT constants

C.C. acknowledges support from the Spanish Ministry of Economy and Competitivity through the Ramon y Cajal program (ref. RYC-2011-08918). A.A.V. acknowledges financial support from MICINN (Ministry of Science and Innovation, Spain) and the FEDER fund (European Fund for Regional Development) provided by grants CTQ2011-26573, UNGI08-4E-003, and UNGI10-4E-801

info:eu-repo/grantAgreement/MICINN//CTQ2011-26573/ES/MODELIZACION QUIMICO CUANTICA DE FOTOQUIMICA Y TRANSFERENCIA ELECTRONICA: SISTEMAS GRANDES, EFECTOS COLECTIVOS Y CONTROL OPTICO/

American Chemical Society (ACS)

Manager: Ministerio de Ciencia e Innovación (Espanya)
Ministerio de Educación y Ciencia (Espanya)
Author: Curutchet, Carles
Voityuk, Alexander A.
Abstract: The possibility to optimize optoelectronic devices, such as organic light-emitting diodes or solar cells, by exploiting the special characteristics of triplet electronic states and their migration ability is attracting increased attention. In this study, we analyze how an intervening solvent modifies the distance dependence of triplet electronic energy transfer (TEET) processes by combining molecular dynamics simulations with quantum chemical calculations of the transfer matrix elements using the Fragment Excitation Difference (FED) method. We determine the β parameter characterizing the exponential distance decay of TEET rates in a stacked perylene dimer in water, chloroform, and benzene solutions. Our results indicate that the solvent dependence of β (β vacuum = 5.14 Å -1 > β water = 3.77 Å -1 > β chloroform = 3.61 Å -1 > β benzene = 3.44 Å -1) can be rationalized adopting the McConnell model of superexchange, where smaller triplet energy differences between the donor and the solvent lead to smaller β constants. We also estimate the decay of hole transfer (HT) and excess electron transfer (EET) processes in the system using the Fragment Charge Difference (FCD) method and find that β TEET can be reasonably well approximated by the sum of β EET and β HT constants
C.C. acknowledges support from the Spanish Ministry of Economy and Competitivity through the Ramon y Cajal program (ref. RYC-2011-08918). A.A.V. acknowledges financial support from MICINN (Ministry of Science and Innovation, Spain) and the FEDER fund (European Fund for Regional Development) provided by grants CTQ2011-26573, UNGI08-4E-003, and UNGI10-4E-801
Format: application/pdf
Document access: http://hdl.handle.net/10256/11480
Language: eng
Publisher: American Chemical Society (ACS)
Collection: info:eu-repo/semantics/altIdentifier/doi/10.1021/jp306280y
info:eu-repo/semantics/altIdentifier/issn/1932-7447
info:eu-repo/semantics/altIdentifier/eissn/1932-7455
info:eu-repo/grantAgreement/MEC//UNGI08-4E-003/ES/Clúster de PCs para cálculo intensivo en química cuántica/
info:eu-repo/grantAgreement/MICINN//UNGI10-4E-801/ES/Clúster de PCs para cálculo intensivo en química cuántica/
Is part of: info:eu-repo/grantAgreement/MICINN//CTQ2011-26573/ES/MODELIZACION QUIMICO CUANTICA DE FOTOQUIMICA Y TRANSFERENCIA ELECTRONICA: SISTEMAS GRANDES, EFECTOS COLECTIVOS Y CONTROL OPTICO/
Rights: Tots els drets reservats
Subject: Transferència d’energia
Transferència d’energia
Dinàmica molecular
Molecular dynamics
Electrònica molecular
Molecular electronics
Química quàntica
Quantum chemistry
Title: Distance dependence of triplet energy transfer in water and organic solvents: A QM/MD study
Type: info:eu-repo/semantics/article
Repository: DUGiDocs

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