Energetics of photoinduced electron-transfer reactions decided by quantum confinement

Gregory D. Scholes; Marcus Jones; Sandeep Kumar

doi:10.1021/jp0754583

Energetics of photoinduced electron-transfer reactions decided by quantum confinement

Gregory D. Scholes, Marcus Jones, Sandeep Kumar

Research output: Contribution to journal › Article › peer-review

68 Scopus citations

Abstract

The photophysics of linear CdSe-CdTe nanorod heterostructures are reported. Charge-transfer emission and absorption bands are identified. Analysis of these bands reveals the factors governing photoinduced electron transfer from CdTe to CdSe, and it is thereby shown how quantum confinement effects decide the thermodynamic parameters of the Marcus-Hush theory. An important finding is the very small reorganization energy associated with the nuclear degrees of freedom (∼20 meV in toluene), which seems to be a characteristic of these nanoscale donor-acceptor systems and differentiates them from most analogous molecular systems. Therefore Marcus "inverted region" behavior is found to be typical for these systems. By analyzing the mixing between the CdTe exciton and the charge-transfer states for one sample, we find the electronic coupling matrix element that promotes the charge separation to be ∼50 meV.

Original language	English (US)
Pages (from-to)	13777-13785
Number of pages	9
Journal	Journal of Physical Chemistry C
Volume	111
Issue number	37
DOIs	https://doi.org/10.1021/jp0754583
State	Published - Sep 20 2007
Externally published	Yes

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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10.1021/jp0754583

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title = "Energetics of photoinduced electron-transfer reactions decided by quantum confinement",

abstract = "The photophysics of linear CdSe-CdTe nanorod heterostructures are reported. Charge-transfer emission and absorption bands are identified. Analysis of these bands reveals the factors governing photoinduced electron transfer from CdTe to CdSe, and it is thereby shown how quantum confinement effects decide the thermodynamic parameters of the Marcus-Hush theory. An important finding is the very small reorganization energy associated with the nuclear degrees of freedom (∼20 meV in toluene), which seems to be a characteristic of these nanoscale donor-acceptor systems and differentiates them from most analogous molecular systems. Therefore Marcus {"}inverted region{"} behavior is found to be typical for these systems. By analyzing the mixing between the CdTe exciton and the charge-transfer states for one sample, we find the electronic coupling matrix element that promotes the charge separation to be ∼50 meV.",

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T1 - Energetics of photoinduced electron-transfer reactions decided by quantum confinement

AU - Scholes, Gregory D.

AU - Jones, Marcus

AU - Kumar, Sandeep

PY - 2007/9/20

Y1 - 2007/9/20

N2 - The photophysics of linear CdSe-CdTe nanorod heterostructures are reported. Charge-transfer emission and absorption bands are identified. Analysis of these bands reveals the factors governing photoinduced electron transfer from CdTe to CdSe, and it is thereby shown how quantum confinement effects decide the thermodynamic parameters of the Marcus-Hush theory. An important finding is the very small reorganization energy associated with the nuclear degrees of freedom (∼20 meV in toluene), which seems to be a characteristic of these nanoscale donor-acceptor systems and differentiates them from most analogous molecular systems. Therefore Marcus "inverted region" behavior is found to be typical for these systems. By analyzing the mixing between the CdTe exciton and the charge-transfer states for one sample, we find the electronic coupling matrix element that promotes the charge separation to be ∼50 meV.

AB - The photophysics of linear CdSe-CdTe nanorod heterostructures are reported. Charge-transfer emission and absorption bands are identified. Analysis of these bands reveals the factors governing photoinduced electron transfer from CdTe to CdSe, and it is thereby shown how quantum confinement effects decide the thermodynamic parameters of the Marcus-Hush theory. An important finding is the very small reorganization energy associated with the nuclear degrees of freedom (∼20 meV in toluene), which seems to be a characteristic of these nanoscale donor-acceptor systems and differentiates them from most analogous molecular systems. Therefore Marcus "inverted region" behavior is found to be typical for these systems. By analyzing the mixing between the CdTe exciton and the charge-transfer states for one sample, we find the electronic coupling matrix element that promotes the charge separation to be ∼50 meV.

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Energetics of photoinduced electron-transfer reactions decided by quantum confinement

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