I would use yearning to convey that sort of exquisite pain. It means a passionate longing for something. It doesn't specifically apply to unrequited love, but usually refers to something you are not going to get.
yearn·ing [yur-ning]
noun
deep longing, especially when accompanied by tenderness or sadness: a widower's yearning for his wife.
an instance of such longing.
That source also mentions a few synonyms for yearning (or rather for yearn) and discusses their differences:
Synonyms
1. Yᴇᴀʀɴ, ʟᴏɴɢ, ʜᴀɴᴋᴇʀ, ᴘɪɴᴇ all mean to feel a powerful desire for something. Yᴇᴀʀɴ stresses the depth and passionateness of a desire: to yearn to get away and begin a new life; to yearn desperately for recognition. Lᴏɴɢ implies a wholehearted desire for something that is or seems unattainable: to long to relive one's childhood; to long for the warmth of summer. Hᴀɴᴋᴇʀ suggests a restless or incessant craving to fulfill some urge or desire: to hanker for a promotion; to hanker after fame and fortune. Pɪɴᴇ adds the notion of physical or emotional suffering as a result of the real or apparent hopelessness of one's desire: to pine for one's native land; to pine for a lost love.
I wouldn't recommend using hankering to describe unrequited love, because it tends to be applied to things rather than people. I think pine usually refers to something you once had but no longer do (plus pining as a noun is not so common as the other three), so I think yearning or longing are your best bets.
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