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On 23 September 1584, she married Robert Sidney, later created Earl of Leicester, at St Donat's Castle, the home of her guardian.
Arnold was personal physician to Robert Sidney, 2nd Earl of Leicester, and subsequently to James Ussher, Archbishop of Armagh; he was also Surgeon General to the Irish Army, and this provided the material for two of his books.
She was backed by Sir Robert Sidney, who considered himself the only legitimate heir of his uncles Leicester and Warwick.
His other grandson, the Viscount De L’isle, was appointed Earl of Leicester in 1618 and it was shortly after this that The Leicester Arms, formerly known as The Porcupine, was renamed in his honour.
Robert Sidney was a patron of musicians, as is proved by his being the dedicatee of Robert Jones’s First Booke of Songes and Ayres (1600) and A Musicall Banquet (1610) compiled by Robert Dowland, son of the composer John Dowland.
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Sold again at Sotheby's and acquired by the British Library in 1975, the autograph is, as its first editor P. J. Croft pointed out, "the largest body of verse to have survived from the Elizabethan period in a text entirely set down by the poet himself".