Ancient Roman architecture
Although concrete had been used on a minor scale in Mesopotamia, Roman architects perfected Roman concrete and used it in buildings where it could stand on its own and support a great deal of weight. The first use of concrete by the Romans was in the town of Cosa sometime after 273 BC. Ancient Roman concrete was a mixture of lime mortar, aggregate, pozzolana, water, and stones, and was stronger than previously-used concretes. The ancient builders placed these ingredients in wooden frames where they hardened and bonded to a facing of stones or (more frequently) bricks. The aggregates used were often much larger than in modern concrete, amounting to rubble.
Mortar (masonry)
Historically, building with concrete and mortar next appeared in Greece. The excavation of the underground aqueduct of Megara revealed that a reservoir was coated with a pozzolanic mortar 12 mm thick. This aqueduct dates back to c. 500 BCE. Pozzolanic mortar is a lime based mortar, but is made with an additive of volcanic ash that allows it to be hardened underwater; thus it is known as hydraulic cement. The Greeks obtained the volcanic ash from the Greek islands Thira and Nisiros, or from the then Greek colony of Dicaearchia (Pozzuoli) near Naples, Italy. The Romans later improved the use and methods of making what became known as pozzolanic mortar and cement. Even later, the Romans used a mortar without pozzolana using crushed  terra cotta, introducing aluminum oxide and silicon dioxide into the mix. This mortar was not as strong as pozzolanic mortar, but, because it was denser, it better resisted penetration by water.