At age twenty, he joined an expedition of naturalists into then-remote and largely uncharted Chaco Province, publishing his observations in Buenos Aires by a pseudonym, Tomás Bathata.
Ambrosetti's reputation in his field was first earned with his publication of studies on the ethnomusicology and cemeteries of the native peoples of Misiones Province, in 1893-95, and with The Megaliths of Tafí del Valle (1896).
[1] His expeditions in the Argentine Northwest led Ambrosetti to the Quebrada de Humahuaca, a scenic gorge in Jujuy Province, where in 1908, he discovered the ruins of the Tilcara, an Omaguaca people long since vanished.
Built on a strategic site as a fort along the storied Inca road system, the Pucará de Tilcara was estimated by Ambrosetti to have been established in the 11th century.
The effort earned Ambrosetti a Doctorate honoris causa from his alma mater in 1910, following which he left responsibility for the project to his student, Salvador Debenedetti; the Quebrada de Humahuaca, including the ruins, was declared a UNESCO World Heritage Site in 2003.