To start, the ‘pick list item’ sorting you configure in the Form Meta Menu only applies to the order in this dialog (as it does for other subviews in the app) rather than actually changing the sort order you see in the app for the list of items.
The order of pick list items is controlled entirely by the order each item was created in. If you add all the pick list items in alphabetical order, it will respect that when shown on your forms.
If you want to change the order of pick list items, the simplest thing to do is to remove all the items and re-add them in the desired order. If you do, you’ll want to change the ‘Order By’ to ordinal again in the meta menu to avoid confusion.
If you do choose to remove and re-add those items, make sure to keep the value exactly as it was, otherwise it will break the link between the pick list title and value in your database.
If you need all of your pick lists reordered alphabetically, I can do so on the back-end automatically for you since you are hosted on Specify Cloud. Just give me the word and I’ll take care of it!