specificlee What, exactly, is Google Play Services? What is Google Play Store? What is GmsCompatConfig? I don't mean on Graphene specifically, but generally: what are these things?
Google Play Store is an app store, where you can install apps from, like any other app store. Most proprietary and government issued apps are only available through Google Play Store, as that is the app store that is preinstalled on most devices. But it is not preinstalled on GrapheneOS.
Google Play Services is an app that allows other apps to easily implement interactions with your Google account, and registration for push messages, and much more, without each and every app having to implement all this functionality itself. Thus, some apps that use your Google account or push messages might need Google Play Services to be installed to function properly. Google Play Store also needs Google Play Services installed to function properly. Google Play Services is not preinstalled on GrapheneOS either.
GmsCompat is a layer GrapheneOS has implemented to allow Google Play Services to function on GrapheneOS. Typically, on most Android based operating systems, Google Play Services is part of the operating system itself, and a privileged component, but it is not included in GrapheneOS. If you install Google Play Services, it will be installed as a regular app, in the regular app sandbox, and thus need to function like that too, without any system level privileges. GmsCompat makes that possible. GmsCompat is a built-in part of GrapheneOS, but is only activated once Google Play Services is installed.
Both Google Play and Google Play Services are proprietary and closed source software, and they need a Google account, thus also depending on a proprietary service from a company known to harvest user data for advertisement purposes. GmsCompat is fully open source, and does not interact with Google or any other party by itself.
specificlee What does it mean that there is a "compatibility layer" or that Graphene has "sandboxed" Google Play services? What are the security benefits that result from this?
What this refers to is that Google Play Services is running as a regular app, in the regular app sandbox, without any system level privileges. The benefit is that Google Play Services cannot spy on you or modify your system in any more way than any regular app can, unlike if it was a system component. This means, that unless you give Google Play Services access to your files, it cannot access your files, and unless you give Google Play Services access to your SMS messages, it cannot read your messages, and so on. This is a great benefit, since Google Play Services is a proprietary closed source component outside of GrapheneOS' control.
specificlee What risks, if any, come from using the GrapheneOS versions of these services on a user profile?
What risks, if any, come from using the GrapheneOS versions of these services on the Owner profile?
It is not GrapheneOS versions. It is the Google versions, identical to how they were released by Google. What risks that carry, if any at all, depends on your threat model.
specificlee Google Play Store asks for an e-mail. Assuming I were to install the sandboxed version on one of the user profiles and enter my IRL google account, would this compromise my privacy on any of the other user profiles? Of the entire device?
Google Play Store and Google Play Services runs as regular apps in GrapheneOS. This also means all their app data, including the email address you entered, are stored solely in that specific user profile, and not shared across user profiles in any way. Regular apps cannot communicate across profiles, except for a known security flaw in AOSP and GrapheneOS user isolation exploited by certain few apps, but not by any Google apps as far as I know.