Sounds like you'll have to go into some special debugging to figure out what's wrong with your SMTP Server's operation.
If you're testing emails sent by the storefront, put the following contents into a new file: /includes/extra_datafiles/email_debugging_on.php
Code:
<?php define('EMAIL_SYSTEM_DEBUG','1');
Then use the create-account option again, and see what information is displayed ... it will output all kinds of status response info from the SMTP connection handshaking. Paste it here ... hiding the actual email addresses of course.
If you're testing sending emails from the admin, put that file into the /your-renamed-admin-foldername/includes/extra_datafiles/ folder instead.
Naturally, you'll delete that file once you're done with email testing, since you don't want that information displayed to visitors.
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