Error suggests that it's an authentication issue. Make sure that the Firewall permissions are in place and the credentials used are correct and allowed.
Also, make sure you have configured SMTP configuration in Web.Config:
<system.net>
<mailSettings>
<smtp from="abc@somedomain.com">
<network host="somesmtpserver" port="25" userName="name" password="pass" defaultCredentials="true" />
</smtp>
</mailSettings>
</system.net>
If needed, have a look at this Microsoft Video tutorial:
Use ASP.NET to send Email from Website[
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