AI Article Synopsis
- The study investigates how the orientation of donor-acceptor pairs affects the solvent-dependent three-photon transition probabilities (δ(3PA)) in through-space charge-transfer systems, particularly with [2,2]-paracyclophane derivatives.
- The calculations reveal that δ(3PA) can reach values as high as 10^6 a.u., which can be enhanced by optimizing the orientation of the donor and acceptor groups.
- The findings highlight that only a few tensor components contribute significantly to δ(3PA), with the primary influence stemming from the large dipole moment difference between the ground and excited states, emphasizing the interplay between π-conjugation and charge transfer.
Article Abstract
We study the effect of donor-acceptor orientation on solvent-dependent three-photon transition probabilities (δ(3PA)) of representative through-space charge-transfer (TSCT) systems, namely, doubly positively charged [2,2]-paracyclophane derivatives. Our cubic response calculations reveal that the value of δ(3PA) may be as high as 10(6) a.u., which can further be increased by a specific orientation of the donor-acceptor moieties. To explain the origin of the solvent cum orientation dependency of δ(3PA), we have calculated different three-photon tensor components using a two-state model, noting that only a few tensor elements contribute significantly to the overall δ(3PA) value. We show that this dependence is due to the large dipole moment difference between the ground and excited states of the systems. The dominance of a few tensor elements indicates a synergistic involvement of π-conjugation and TSCT in the large δ(3PA) of these systems.
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| http://dx.doi.org/10.1039/c3cp52696h | DOI Listing |
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