2023
DOI: 10.1021/acs.jpclett.2c03413
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Revealing Intermolecular Electronic and Vibronic Coherence with Polarization-Dependent Two-Dimensional Beating Maps

Abstract: Two-dimensional electronic spectroscopy (2DES) has been widely employed as an efficient tool to reveal the impact of intermolecular electronic and/ or vibronic quantum coherence on excitation energy transfer in light-harvesting complexes. However, intramolecular vibrational coherence would also contribute to oscillating signals in 2D spectra, along with the intermolecular coherence signals that are directly related to energy transfer. In this work, the possibility of screening the vibrational coherence signals… Show more

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Cited by 3 publications
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“…As stated above, we incorporate the static disorder over site energies into the HEOM, and use the following scheme for averaging over different (random) orientations of the LH2 complex. The relation between the orientationally averaged third order response function and the molecular frame response functions is given by , false⟨ R total ori = false m 1 m 2 m 3 m 4 C m 1 m 2 m 3 m 4 R m 1 m 2 m 3 m 4 mol where m⃗ k are the molecular axes m⃗ k ∈ { x⃗ , y⃗ , z⃗ } in the molecular frame. The transformation coefficients C m 1 m 2 m 3 m 4 take the form of C m 1 m 2 m 3 m 4 = 1 15 false( δ m 1 m 2 δ m 3 m 4 + δ m 1 m 3 δ m 2 m 4 + δ m 1 m 4 δ m 2 m 3 false) For convenience, all the 21 nonzero coefficients are listed in Table .…”
Section: Resultssupporting
confidence: 91%
“…As stated above, we incorporate the static disorder over site energies into the HEOM, and use the following scheme for averaging over different (random) orientations of the LH2 complex. The relation between the orientationally averaged third order response function and the molecular frame response functions is given by , false⟨ R total ori = false m 1 m 2 m 3 m 4 C m 1 m 2 m 3 m 4 R m 1 m 2 m 3 m 4 mol where m⃗ k are the molecular axes m⃗ k ∈ { x⃗ , y⃗ , z⃗ } in the molecular frame. The transformation coefficients C m 1 m 2 m 3 m 4 take the form of C m 1 m 2 m 3 m 4 = 1 15 false( δ m 1 m 2 δ m 3 m 4 + δ m 1 m 3 δ m 2 m 4 + δ m 1 m 4 δ m 2 m 3 false) For convenience, all the 21 nonzero coefficients are listed in Table .…”
Section: Resultssupporting
confidence: 91%