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                <term xml:lang="en">Nitrogen oxides</term>
                <term xml:lang="en">Absorption spectroscopy</term>
                <term xml:lang="en">Charge transfer</term>
                <term xml:lang="en">Chromophores</term>
                <term xml:lang="en">Ground state</term>
                <term xml:lang="en">Light absorption</term>
                <term xml:lang="en">Phenyleneethynylene</term>
                <term xml:lang="en">Charge transfer process</term>
                <term xml:lang="en">DFT calculation</term>
                <term xml:lang="en">Donor and acceptor</term>
                <term xml:lang="en">Donor-acceptor dyads</term>
                <term xml:lang="en">Excited states</term>
                <term xml:lang="en">Time-resolved infrared absorption spectroscopy</term>
                <term xml:lang="en">Push-pull chromophores</term>
                <term xml:lang="en">Photophysical behavior</term>
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              <p>The D-π-A dyads [(n-Hex)2N(1,4-C6H4)]CC[(1,4-C6H4)NO2] (1) and [(n-Hex)2N(1,4-C6H4)]CC(1,4-C6H4)CC[(1,4-C6H4)NO2] (2) have been studied by ultrafast time-resolved infrared absorption spectroscopy. After excitation into their singlet charge-transfer (1CT) state, a fast decay (ca. 6 ps for 1 and 1 ps for 2) of the initially populated singlet state into a ground state (major pathway) and a longer lived excited state (possibly the triplet state) is observed. The nitro and alkyne groups were used as vibrational reporters to probe the changes induced by the charge-transfer process. For the first time, we confirm experimentally that these changes are consistent with expectations based on the traditional valence-bond representations of the CT states of these push-pull chromophores. An almost identical charge transfer takes place in the two dyads, despite π-bridges of different lengths between the donor and acceptor groups. Complementary DFT calculations support the experimental assignments and have helped clarify the photophysical behavior of 1 and 2.</p>
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