The study aimed to investigate the molecular structure of indomethacin-PVP amorphous solid dispersions and identify specific interactions between the components using vibrational spectroscopy. Solid dispersions were prepared using a solvent evaporation technique, and IR and FT-Raman spectra were obtained. The results showed that amorphous indomethacin predominantly exists as dimers, while the addition of PVP increased the intensity of the non-hydrogen-bonded carbonyl band in the infrared spectrum and shifted the PVP carbonyl stretch to a lower wavenumber, indicating hydrogen bonding. Model solvent systems aided spectral interpretation, and the magnitude of spectral changes was similar for solid dispersions and solutions. The study concluded that indomethacin interacts with PVP through hydrogen bonds, disrupting indomethacin dimers and potentially influencing crystallization kinetics by preventing self-association of indomethacin molecules. The similarity in results for solid dispersions and solutions highlights the "solution" nature of this binary amorphous state.The study aimed to investigate the molecular structure of indomethacin-PVP amorphous solid dispersions and identify specific interactions between the components using vibrational spectroscopy. Solid dispersions were prepared using a solvent evaporation technique, and IR and FT-Raman spectra were obtained. The results showed that amorphous indomethacin predominantly exists as dimers, while the addition of PVP increased the intensity of the non-hydrogen-bonded carbonyl band in the infrared spectrum and shifted the PVP carbonyl stretch to a lower wavenumber, indicating hydrogen bonding. Model solvent systems aided spectral interpretation, and the magnitude of spectral changes was similar for solid dispersions and solutions. The study concluded that indomethacin interacts with PVP through hydrogen bonds, disrupting indomethacin dimers and potentially influencing crystallization kinetics by preventing self-association of indomethacin molecules. The similarity in results for solid dispersions and solutions highlights the "solution" nature of this binary amorphous state.