The use of a novel spectral interconversion scheme to probe weak molecular interactions of a polymer system is reported. Based on the multivariate regression model using partial least squares (PLS), the thermally induced changes in the weak interaction of poly(<i>n</i>-isopropylacrylamide) (PNiPA) film was studied by the interconversion between mid-infrared (MIR) and near-infrared (NIR) spectra measured at temperatures between 40 and 220 °C. It was demonstrated that not only NIR spectra but also well-resolved MIR spectra of PNiPA film, either in narrow or wide spectral ranges, can be predicted from each other based on the proposed scheme. The thermally induced weak interaction changes of PNiPA, expressed as either the band shift or intensity changes at a specific region, can be probed properly. Meanwhile, the effect of several important factors such as the selected spectral range, correlation between the specific bands, and especially the multiple scattering corrections (MSC) on the accuracy of the spectral prediction were also investigated in detail. This study provides a novel method for the analysis of weak interactions in complex systems.

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