The effects of noncovalent interactions, which influence the populations of aggregates, are ultimately manifested in the spectroscopic signals of the system. Infrared (IR) spectra, in particular, contain exquisite information about microscopic characteristics and provide detailed insights into key noncovalent interactions, notably hydrogen bonds . Recent advances have reported simulations of IR and vibrational circular dichroism (VCD) spectra based on aggregate populations for pure solvents and solvent mixtures with various solutes . These approaches involve averaging the spectra of optimized clusters and calculating their populations using either the quantum cluster equilibrium theory or the clusters-in-a-liquid framework . While most studies focus on the fingerprint region, simu-lations of the O H stretching region for hydrogen-bonded aggregates have revealed limitations in addressing the challenging broadband that is observed. The formation of hydrogen bonds significantly affects the vibrational spectrum, shifting the O H stretching bands of the acceptor to lower wavenumbers. Indeed, this band is highly sensitive to the number and arrangement of hydrogen bonds, whether intra-or intermolecular. Consequently, these characteristics make the simulations of such O H stretching region (3100-3800 cm -1 ) a stringent test to compare populations derived from MD and conformational search-based methods.