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Discover Ludwig"most unexpected" is correct and can be used in written English.
You can use it when something happens that is totally beyond what you have expected to happen. For example, "I received a phone call from my long-lost friend, which was most unexpected."
Exact(60)
Most unexpected?
The result was most unexpected.
A most unexpected work.
Most unexpected entry: Unknown, as Moby-Duck.
What's the most unexpected thing you found?
Anyway, this is all most unexpected.
Transcendence: 2014's most unexpected turkey?
Those physical insights often come from the most unexpected places.
Encouragement often comes from the most unexpected sources.
If so, what are your most unexpected sources of influence?
What was the most unexpected turn it took?
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Since I tried Ludwig back in 2017, I have been constantly using it in both editing and translation. Ever since, I suggest it to my translators at ProSciEditing.

Justyna Jupowicz-Kozak
CEO of Professional Science Editing for Scientists @ prosciediting.com