Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid

Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of c...

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Veröffentlicht in:The Journal of chemical physics 2016-03, Vol.144 (10), p.104701-104701
Hauptverfasser: Rury, Aaron S., Sorenson, Shayne, Dawlaty, Jahan M.
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creator Rury, Aaron S.
Sorenson, Shayne
Dawlaty, Jahan M.
description Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone, we find sub-cm−1 oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology.
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Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. 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subjects ACOUSTICS
BENZOQUINONES
Charge materials
Charge transfer
Coherence
Coupling (molecular)
ELECTRON DENSITY
ELECTRON TRANSFER
ELECTRON-PHONON COUPLING
EXCITATION
EXPERIMENTAL DATA
Hydrogen bonding
Hydrogen storage
Hydroquinone
Information technology
INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Optical pumping
Organic materials
ORGANIC MATTER
Oxidation
PHONONS
Photonics
Quinones
RAMAN SPECTROSCOPY
RESONANCE
title Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid
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