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In an online dictionary for 単独, 単独 is used seemingly as an adverb in two example sentences, but with different particles:

「単独で登頂する」 「単独に存在する」

99% of other 単独 examples online use で. Since this is a very reliable online dictionary in my experience, what is the grammar of using 単独に here? Is 単独 treated as a different part of speech in 単独に versus 単独で?

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There's definitely some freedom of choice, but で suggests agency (by whatever is "independent"), whereas に suggests passivity/staticity. It's not by chance that 単独で is used with 登頂する, and 単独に is used with 存在する.

Other examples I found on the Shonagon corpus:

『幻想交響曲』のみが 単独に コンサートで演奏される

に feels best here, since 幻想交響曲, which is what is played independently, is the object of action. (The passive structure here is irrelevant, I would still use に in 『幻想交響曲』を単独に演奏する.) 『幻想交響曲』を単独演奏する, on the other hand, sounds a bit more like "[someone] is playing it by themselves", although to me, both interpretations are valid.

夫が 単独で 移住するケース

で sounds better here, since the independence describes the agent, 夫.

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