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Electronic State-Resolved Electron–Phonon Coupling in an Organic Charge Transfer Material from Broadband Quantum Beat Spectroscopy
journal contribution
posted on 2015-12-17, 09:43 authored by Aaron S. Rury, Shayne Sorenson, Eric Driscoll, Jahan M. DawlatyThe coupling of electron and lattice
phonon motion plays a fundamental
role in the properties of functional organic charge-transfer materials.
In this Letter we extend the use of ultrafast vibrational quantum
beat spectroscopy to directly elucidate electron–phonon coupling
in an organic charge-transfer material. As a case study, we compare
the oscillatory components of the transient reflection (TR) of a broadband
probe pulse from single crystals of quinhydrone, a 1:1 cocrystal of
hydroquinone and p-benzoquinone, after exciting nonresonant impulsive
stimulated Raman scattering and resonant electronic transitions using
ultrafast pulses. Spontaneous resonance Raman spectra confirm the
assignment of these oscillations as coherent lattice phonon excitations.
Fourier transforms of the vibrational quantum beats in our broadband
TR measurements allow construction of spectra that we show report
the ability of these phonons to directly modulate the electronic structure
of quinhydrone. These results demonstrate how coherent ultrafast processes
can characterize the complex interplay of charge transfer and lattice
motion in materials of fundamental relevance to chemistry, materials
sciences, and condensed matter physics.
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Organic Charge Transfer Materiallattice phonon excitationscase studycharge transferelectronlattice motionultrafast vibrational quantummaterials sciencesbroadband probe pulseshow reportvibrational quantumlattice phonon motionBroadband Quantum Beat SpectroscopyThebroadband TR measurementsSpontaneous resonance Raman spectraoscillatory componentsquinhydroneultrafast processesmatter physicsultrafast pulses
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