extra-keyboards-for-chrome-os
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Use Caps Lock Key as Compose
There doesn't seem to be a way to set the caps lock key to the compose key in these settings. Without that mapping, this extension doesn't provide any value.
If I recall correctly, the ChromeOS IME API doesn't provide a way to cancel Caps Lock events, so there isn't a good way to do this directly in the extension.
However, you can work around it somewhat. In the ChromeOS “Settings” app, go to the “Keyboard” section and remap Caps Lock to either Control or Alt. Then select the corresponding “Left Control” or “Left Alt” key in the ComposeKey settings.
Similar to https://bugs.chromium.org/p/chromium/issues/detail?id=914221&q=Caps%20lock&can=2