I think I answered my own question...
I simply had to call the ADD method on my PIServers object.
Is this correct?
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As the PIServers object represents the collection of known PI Data Archive servers on the client workstation, you would only need to use the Add method to register a new, previously unknown server (relative to the computer you are connecting from). More likely what you need to do is to specify which server from the collection you want to connect to before calling it's Connect() method:
PIServers piServers = new PIServers(); PIServer piServer; piServer = piServers["MyDAserver"]; piServer.Connect();