The detection of analyte-binding events by receptors is drawing together the fields of Raman spectroscopy and supramolecular chemistry. This study is intended to facilitate this cohering by examining a model system in the solution phase, The resonance Raman scattering (RRS) spectra of the complexation between tetrathiafulvalene (TTF) and cyclobis(paraquat-p-phenylene) (CBPQT(4+)) has been used as the model to characterize the binding event of a host-guest system. RRS spectra are generated by excitation (lambda(exc) = 785 nm) within the lowest-energy charge-transfer (CT) transition (lambda(max) = 865 nm) of the TTF subset of CBPQT(4+) complex. The paired binding curves from the RRS and UV-vis-NIR titration data agrees with prior work. and a Delta G of -5.7 +/- 0.6 kcal mol(-1) (MeCN, 298 K) was obtained for the complexation of TTF with CBPQT(4+). Computations on the complex and its components reproduce the energy shifts and resonance enhancements of the Raman band intensities, providing a basis to identify the structural and vibrational changes Occurring upon complexation. The changes in bond lengths coincide with partial depopulation of a TTF-based HOMO and population of a CBPQT(4+)-based LUMO through CT mixing in the ground state of 0.46e(-). The structural changes upon complexation generally lead to lower wavenumber vibrations and to changes in the normal mode descriptions.