Sum-frequency generation spectra of a Langmuir monolayer on water surface at varying surface areas were studied with two-dimensional correlation analysis. Upon enlarging the area/molecule of the Langmuir monolayer, the sum-frequency spectra changed reflecting the conformation change of the alkyl chains of the molecules in the monolayer. These changes stood out more clearly by employing two-dimensional correlation analysis of the above sum-frequency spectra. Features not very pronounced in the original spectra such as closely-spaced spectral bands can also be easily distinguished in the two-dimensional correlation spectra.
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