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It has been reported that adding polyphosphoric acid (PPA) to bitumen modified with Montmorillonite clay (MMT) makes the bituminous composite less prone to swelling and more resistant to moisture damage, thus improving two major causes of pavement distress. There has been no in-depth study on the underlying mechanism for such a synergistic effect between MMT and PPA. Here, we used laboratory experiments and computational modeling to study how PPA moderates the intermolecular interactions in bitumen modified with MMT. The results showed tha