Just to be sure I understand what you are asking...
You have a volume "Archive_chi", that contains general file data shared out to users via CIFS/NFS.
You have/are trying to create a second volume "ArchiveLUN_chi" which will contain a LUN "ArchiveLUN".
You want to run a command on the controller to copy the files from the original volume into the LUN as a single unit (meaning the LUN is a single unit).
Just want to make sure I have your intent straight.
You can't do this at the NetApp controller itself, which is why your attempts to do this failed. Accesses into a LUN require something to use the appropriate SCSI varient protocol to initiate block level reads and writes. You will have to create the LUN, mount the LUN to a server/workstation as a disk, format the disk appropriately based on the OS of the server/workstation, access the shared files on the original volume, and start a manual copy using the external server as a conduit between the files on a share and the LUN.
In the NetApp WAFL file system, everything (even LUNs) are files. LUNS generally are big files, but just files. Data Ontap itself doesn't interpret the contents of the files directly. Rather it creates/reads/writes/deletes/etc. blocks of the files in response to access protocol requests - SCSI via FC/iSCSI, CIFS, NFS, etc. Other operations such as SnapMirror/FlexClone etc. work on either an entire volume or an entire file at a time (leaving out cDot subfile cloning for the moment).
So the idea that the controller can take a series of files and write them into a logical disk format with an OS specific file-system (like NTFS) that an external server can then treat as a disk image just doesn't exist. You'll have to do this the brute force way.