I am attempting to Impersonate an administrator account from a LocalSystem Service in order to get data from administrators HKEY CURRENT USER registry - in order to impersonate
By default the HKEY_CURRENT_USER handle is cached on a process wide basis. So when you impersonate a user and then access the current user hive you will be accessing the hive of the user that started the process not the user being impersonated. This is true for all Win32 processes not just .Net. If you wish to disable this caching so that all current user calls go to the correct user hive under HKEY_USERS then you must call RegDisablePredefinedCache via pInvoke.
Be warned that if the user being impersonated has not had their profile loaded then any CurrentUser requests will be forwarded to the .DEFAULT user. So you may also need to call LoadUserProfile.
Disabling the handle caching will also cause a slight slowdown in all CurrentUser requests.