Unfortunately, this is not possible: LINQPad relies on the .NET WCF client and EntityClassGenerator in System.Data.Services.Design.dll, which don't really support service operations (as of Framework 4.0).
The workaround at this stage is the same as what you'd do if you were coding in Visual Studio and is described well here.
Hence you could type the following into LINQPad to call the operation GetContacts(string firstName):
this.Execute<Contact> (new Uri ("GetContacts?firstName='John'", UriKind.Relative))
or, if the service returns a sequence of objects:
CreateQuery<Contact>("GetContacts").AddQueryOption("firstName", "'John'")