Communication: Trapping upconverted energy in neat platinum porphyrin films via an unexpected fusion mechanism

Jonathan A. Hinke; Tom J. Pundsack; Wade A. Luhman; Russell J. Holmes; David A. Blank

doi:10.1063/1.4821164

Communication: Trapping upconverted energy in neat platinum porphyrin films via an unexpected fusion mechanism

Jonathan A. Hinke, Tom J. Pundsack, Wade A. Luhman, Russell J. Holmes, David A. Blank

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Abstract

Direct observation of an unexpected product from excited state fusion of two excited triplet states in platinum octaethylporphyrin is reported. Transient spectroscopy was used to identify the product as a metal centered (d, d) state that decays slowly compared with the rate of fusion. The reaction was demonstrated to be second order with a rate coefficient of k_TTF = (5.4 ± 0.4) × 10^-10 cm³ · s ^-1. The results contrast with the common assumption that fusion proceeds directly to annihilation via rapid non-radiative deactivation of the products. Following visible photo-excitation, the fusion process results in energetic upconversion of the incident photons stored in the higher energy (d, d) state at irradiances below the threshold for multi-photon absorption.

Original language	English (US)
Article number	101102
Journal	Journal of Chemical Physics
Volume	139
Issue number	10
DOIs	https://doi.org/10.1063/1.4821164
State	Published - Sep 14 2013

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abstract = "Direct observation of an unexpected product from excited state fusion of two excited triplet states in platinum octaethylporphyrin is reported. Transient spectroscopy was used to identify the product as a metal centered (d, d) state that decays slowly compared with the rate of fusion. The reaction was demonstrated to be second order with a rate coefficient of kTTF = (5.4 ± 0.4) × 10-10 cm3 · s -1. The results contrast with the common assumption that fusion proceeds directly to annihilation via rapid non-radiative deactivation of the products. Following visible photo-excitation, the fusion process results in energetic upconversion of the incident photons stored in the higher energy (d, d) state at irradiances below the threshold for multi-photon absorption.",

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AU - Luhman, Wade A.

AU - Holmes, Russell J.

AU - Blank, David A.

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AB - Direct observation of an unexpected product from excited state fusion of two excited triplet states in platinum octaethylporphyrin is reported. Transient spectroscopy was used to identify the product as a metal centered (d, d) state that decays slowly compared with the rate of fusion. The reaction was demonstrated to be second order with a rate coefficient of kTTF = (5.4 ± 0.4) × 10-10 cm3 · s -1. The results contrast with the common assumption that fusion proceeds directly to annihilation via rapid non-radiative deactivation of the products. Following visible photo-excitation, the fusion process results in energetic upconversion of the incident photons stored in the higher energy (d, d) state at irradiances below the threshold for multi-photon absorption.

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Communication: Trapping upconverted energy in neat platinum porphyrin films via an unexpected fusion mechanism

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