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filesystem semantics are complicated. Which operations are atomic, what ordering guarantees there are, how fsync works, etc, etc. Network filesystems never get all of them right, in my experience. Trying to do so would make them unusably slow. Whether any particular tradeoff any particular implementation makes will break something calibre relies on, there is no a-priori way to know, you have to test.
And of course, if you have multiple things making modifications to the same library database/files, all bets are off, even without file system implementation issues.
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