Atmospheric aerosols deteriorate visibility and pose a significant risk to human health. The global fluxes of secondary organic aerosols (SOA) that form in the atmosphere from aromatic hydrocarbons are poorly constrained and highly uncertain. The lack of molecular tracers to quantify anthropogenic SOA (ASOA) in part limits the understanding of its abundance and variability, and results in a systematic underestimation of the role of ASOA in the atmosphere. The research presented in this thesis advances the knowledge about ASOA through the i) development of new and advanced methods to quantify potential ASOA tracers, ii) evaluation of their suitability as tracers for ASOA, and iii) application of the validated tracers to assess the spatial, diurnal and seasonal variation of ASOA in three urban environments. In this research, a greater understanding of the role of ASOA is gained through the expansion of tracers for SOA from aromatic hydrocarbons. An analytical method to quantify furandiones, which are produced in high yields from the photooxidation of aromatic hydrocarbons, was developed and enabled the first ambient measurements of furandiones. The optimized method allows for the simultaneous extraction of primary source tracers (e.g., polycyclic aromatic hydrocarbons, hopanes, levoglucosan) and other potential ASOA tracers (e.g., 2,3-dihydroxy-4-oxopentanoic acid [DHOPA], benzene dicarboxylic acids, and nitromonoaromatics). The systematic evaluation of potential ASOA tracers by their detectability, gas-particle partitioning, and specificity revealed that DHOPA, phthalic acid, 4-methylphthalic acids, and some nitromonoaromatics are good ASOA tracers because they are specific to aromatic hydrocarbon photooxidation, readily detected in ambient air, and substantially partition to the particle phase under ambient conditions. These tracers are thus recommended for use in field studies to estimate ASOA contributions to atmospheric aerosol relative to other sources. ASOA was determined to be a significant contributor to PM2.5 organic carbon (OC) in three urban environments. In the industrial Houston Ship Channel area in Houston, TX, ASOA contributed 28% of OC, while biogenic SOA (BSOA) contributed 11%. Diurnally, ASOA peaked during daytime and was largely associated with motor vehicle emissions. In Shenzhen, a megacity in China, 13-23% of OC mass was attributed to ASOA, three folds higher than BSOA. When China controlled the emissions from fossil fuel-related sources, the ASOA contribution to OC reduced by 42-75% and visibility remarkably improved. In downtown Atlanta, GA, ASOA contributed 29% and 16% of OC during summer and winter, respectively. ASOA dominates over BSOA during winter, while high biogenic VOC fluxes made BSOA the major SOA source in Atlanta, GA during summertime. These results indicate the high abundance of ASOA in urban air that has potential to be reduced by modification of anthropogenic activities. Overall, the work presented in this dissertation advances the knowledge about the abundance and variation of ASOA in urban atmospheres through the development of quantification methods and expansion of ASOA tracers. These tracers improve source apportionment of ASOA in receptor based models, which can ultimately aid in developing and implementing effective strategies for air quality management.