I think the fastest way would be to change the DNS zone - if you did want any incoming mail to reach them either.
Otherwise modifying this line in exim.conf would probably do the trick. Just make them not allowed.
Code:
accept hosts = +auth_relay_hosts
endpass
message = $sender_fullhost is currently not permitted to \
relay through this server. Perhaps you \
have not logged into the pop/imap server in the \
last 30 minutes or do not have SMTP Authentication turned on in your email client.
authenticated = *
Add a deny hosts.