Ballistic Energy Transport via Long Alkyl Chains: A New Initiation Mechanism
arxiv(2024)
Abstract
In an effort to increase the speed and efficiency of ballistic energy
transport via oligomeric chains, we performed measurements of the transport in
compounds featuring long alkyl chains of up to 37 methylene units. Compounds of
the N3-(CH2)n-COOMe type (denoted as aznME) were synthesized with n = 5, 10,
15, 19, 28, 37 and studied using relaxation-assisted two-dimensional infrared
spectroscopy. The speed of the ballistic transport, initiated by the N3 tag
excitation, increased ca. 3-fold for the longer chains (n = 19-37) compared to
the shorter chains, from 14.7 Å/ps to 48 Å/ps, in line with an earlier
prediction (Nawagamuwage et al. 2021, J. Phys. Chem. B, 125, 7546). Modeling,
based on solving numerically the Liouville equation, was capable of reproducing
the experimental data only if three wavepackets are included, involving CH2
twisting (Tw), wagging (W), and rocking (Ro) chain bands. The approaches for
designing molecular systems featuring higher speed and efficiency of energy
transport are discussed.
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