The ability of the Q/s method to align with experimental observations is limited by the extent of its conformational search. While an exhaustive search could yield results closer to those of C/d, non-bonded aggregates exhibit high configurational entropy, imposing practical limits on systematic search-based approaches. Aggregates with such loosely bound, flexible structures inherently challenge even sophisticated automated search techniques, as capturing their full entropy becomes infeasible. Our findings thus indicate that the C/d approach provides a more reliable representation of aggregate populations in this system, as demonstrated by its superior performance in simulating IR spectral regions sensitive to non-bonded interactions, such as the broad OH stretching band.