Pope Alexander VII decided that the rector should be appointed by the protectors of the college.
He completed the stucco decoration of San Tomaso di Villanova in Castel Gandolfo (1660-1), the stucco decoration of Bernini's Sant'Andrea 1662-1665), the statues of Saint Bernardino and Pope Alexander VII Chigi for Duomo di Siena and the Virgin and Child in Saint Joseph des Carmes in Paris (1650–51).
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Recently discovered documentation shows that he provided the kneeling figure of Saint Bernardino of Siena (1656–57) in Alexander VII's chapel at Santa Maria della Pace, and the two pairs of putti holding portrait medallions on the façade.
Sante Bartoli's memoirs record that when Alexander VII was building the left wing of Bernini's colonnade and the lefthand fountain, a tomb was discovered with a bas-relief above the door representing a marriage-scene ("vi era un bellissimo bassorilievo di un matrimonio antico").
Pope Alexander VII confirmed his appointment on June 3, 1658 and he was consecrated as a bishop by Pierre de Marca, Archbishop of Toulouse, on September 8, 1658.
The popes sent him on various honorable missions, such as bearing the cardinal's hat to the nuncio at Warsaw in 1629, and Alexander VII sent him to Innsbruck to receive abjuration of Protestantism by the mercurial and tiresome Christina, former Queen of Sweden.
The French Jansenists professed that the propositions condemned in 1653 were not in fact to be found in Augustinus, written by Cornelius Jansen.
In 1658, the Church would establish an Apostolic Vicariate by Pope Alexander VII, 124 years since the first voyage of Jacques Cartier in 1534.
Six Franciscans sent by Pope Alexander VII to succeed in converting Ethiopia to Catholicism where the Jesuits had failed 30 years before, were executed during his reign.
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Under Claude Vaussin, General of the Cistercians (in the middle of the seventeenth century), several reforms were made in the liturgical books of the order, and were approved by Pope Alexander VII, Pope Clement IX and Pope Clement XIII.