In the cloister, she suffered much from illness. Early in her sickness, she experienced periods of spiritual ecstasy through the use of the devotional book, Abecedario espiritual, commonly known as the "third" or the "spiritual alphabet". This work, following the example of similar writings of the medieval mystics, consisted of directions for tests of conscience and for spiritual self concentration and inner contemplation, known in mystical nomenclature as oratio recollectionis or oratio meretalis. Besides this, she employed other mystical ascetic works. She professed, in her illness, to rise from the lowest stage, "recollection", to the "devotions of peace" or even to the "devotions of union", which was one of perfect ecstasy. With this was frequently joined a rich "blessing of tears". As the merely outer and void Roman Catholic distinction between mortal and venial sin dawned upon her, she came upon the secret of the awful terror of sinful iniquity, and the inherent nature of original sin. With this was correlated the consciousness of utter natural impotence and the necessity of absolute subjection to God.

George Bataille pointed out in his text On Erotisme that the transgressor needs to know the structures she or he seeks to transgress. Saint Theresa was utterly aware of how dangerous her mystic experiences, which she describes in her poems and that, were widely condemned by the catholic establishment.

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