So the ties between Carlos and the Spanish royal family continued after the death of his first wife: King Alfonso XIII even sent his former brother-in-law to represent him at the funeral in 1912 of Prince Regent Luitpold. If nothing else, Luitpold's granddaughter Maria Ludwig was married to Carlos' older brother, the Duke of Calabria.
If it came to that, Infanta Amalia of Spain (1834-1905), whose marriage in 1856 to Prince Adalbert of Bavaria (1828-1875) established the Spanish branch of the Wittelsbachs, was herself a direct descendant of the Bourbon kings of the Two Sicilies.
So you had an interesting situation where Prince Ludwig Ferdinand of Bavaria (1859-1949) was a cousin of all the Spanish Bourbons, a brother-in-law to King Alfonso XII and Infanta Eulalia, an uncle by marriage to their children, and finally the father-in-law of Infanta Maria Teresa.
So, answering your question, no, she was never considered to be Carlos’s second wife.
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