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The inter- and intramolecular interactions of the carbonyl moieties at the polar interface of a phospholipid membrane are probed by using nonlinear femtosecond infrared spectroscopy. Two-dimensional IR correlation spectra separate homogeneous and inhomogeneous broadenings and show a distinct cross-peak pattern controlled by electrostatic interactions. The inter- and intramolecular electrostatic interactions determine the inhomogeneous character of the optical response. Using molecular dynamics simulation and the nonlinear exciton equations approach, we extract from the spectra short-range structural correlations between carbonyls at the interface.

Electrostatic interactions in phospholipid membranes revealed by coherent 2D IR spectroscopy