abstract: This research focused on the structure-property relationships of a rejuvenator to understand the comprehensive rejuvenation mechanism of aged asphalt binder. Aged asphalt such as recycled asphalt shingles (RAS) and reclaimed asphalt pavement (RAP) contain various amounts of asphalt binder. However, the asphalt binder in RAS and RAP is severely aged and inferior in properties compared to a virgin binder. To address this issue, liquid additives have been used under the general title of rejuvenators. That poses an additional challenge associated with the lack of clear metrics to differentiate between softeners and rejuvenators. Therefore, there is a need for a thorough study of rejuvenators. In this study, diverse-sourced rejuvenators have been used in RAS and RAP-modified binders as well as laboratory-prepared aged binders. The properties of the rejuvenated aged binder were characterized at a macro-level and molecular level. The study showed that the performance of the RAS-modified binder was significantly improved after bio-modification by a bio-rejuvenator. This study further evaluated laboratory-prepared aged asphalt rejuvenated with different rejuvenators. The results found that oxidized bitumen became soft after adding rejuvenators, regardless of their source. Molecular dynamics simulation showed that the effective rejuvenator restored the molecular conformation and reduced the size of asphaltene nanoaggregates. The study results showed that due to the specific chemical composition of certain rejuvenators, they may negatively impact the durability of the mixture, especially about its resistance to moisture damage and aging. Computational analysis showed that while the restoration capacity of rejuvenators is related to their penetration into and peptizing of asphaltene nanoaggregates, the durability of the restored aged asphalt is mainly related to the polarizability values of the rejuvenator. Rejuvenators with lower polarizability showed better resistance to aging and moisture damage. In summary, this study develops the rheology-based indicators which relate to the molecular level phenomenon in the rejuvenation mechanism. The rheology-based indicators, for instance, crossover modulus and crossover frequency differentiated the rejuvenators from recycling agents. Moreover, the study found that rejuvenation efficiency and durability are depended on the chemistry of rejuvenators. Finally, based on the learning of chemistry, a chemically balanced rejuvenator is synthesized with superior rejuvenation properties. / Dissertation/Thesis / Doctoral Dissertation Civil, Environmental and Sustainable Engineering 2020