All your references live in My Library. You can organize those references into collections and subcollections, represented by a folder icon. When you add a reference to a collection, Zotero does not make an additional copy of the reference. It simply displays that reference in both My Library and the collection you've chosen. You can add a reference to as many collections and subcollections as you wish; the reference is still simply mirroring the My Library reference. In this way, Zotero operates like your music library on your phone, and collections are your playlists.
Create a new collection by tapping the New Collection button on the toolbar at the top of the navigation pane (left pane). This button looks like a folder with a "+" icon.

Name the new collection, and choose My Library. You can reorganize collections and subcollections at any time by dragging and dropping (see below).

By right-clicking a collection, you can rename it, delete it, or add a subcollection. Deleting your collection also deletes any subcollections, but the references themselves will still remain in My Library and in any other collections you placed them in unless you choose Delete Collection and Items.

You can reorganize your hierarchy at any time by dragging and dropping the folders, including making folders subcollections or promoting them to top-level collections. To do the latter, drag the collection into My Library.

To add an item to a collection, drag and drop it there from My Library or from any other collection it currently lives in. To remove an item from a collection, right-click it and select Remove Item from Collection. It is not possible to accidentally remove an item from My Library.
If you are currently in a collection when you use the Zotero Connector, it will automatically import into both My Library and that collection. You can change what's happening in the "Saving to" box in your browser if you're quick enough, or you can go into Zotero and remove it manually.

To see which collections your references are in, select a reference in the center pane. In the details pan, click the Libraries and Collections icon from the menu on the right.

In the details pane, you can also click the "+" icon to add the reference to additional collections.
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To see your references that are only in My Library, tap the Unfiled Items special collection.

Tags are descriptive keywords about references in your library. They appear in the Tag Selector box at the bottom of the navigation pane. Clicking on a tag will show you only references with that tag.
Why use tags?
Automatic tags can help you explore your library using the terminology preferred by databases you use. Manual tags can be especially useful to label references with things like "to read," "project name," "name of colleague who sent me this article/who might enjoy this article," etc. You can also create your own thematic tags.
Automatic Tags
Zotero frequently imports tags automatically, pulling in data like subject headings when you import a reference from a database. You can turn this off in your preferences. You can also hide or delete automatic tags by tapping the filter icon in the bottom right of the Tag Selector.

Manual Tags
To apply an existing tag or add a new tag to a reference, select the reference in the center pane and tap the Tags icon in the details pane.

Manual tags will have a blue icon next to them, as opposed to the grey icon for automatic tags. Tap Add and begin typing. If there's already a tag in your library similar to what you're typing, it will show up as a suggestion. You can select that suggestion or create a new tag. To remove a tag, tap the minus sign next to it.

Manage Tags
Right-clicking a tag in the Tag Selector allows you to delete or rename it. Deleting a tag removes it from any reference it was previously associated with. Renaming a tag to the exact same text as another existing tag will merge the two, applying the revised tag to items that had the old tag.

You can also assign a color to a tag. This shows a colored dot next to the tagged items in the center pane. It also prioritizes the tag, moving it to the top of the Tag Selector.


Searching Tags
You can search your existing tags using the search box at the bottom of the Tag Selector.

Quick Search
The search box at the top right of the center pane allows you to search your library quickly. Quick search works best with a word or short phrase.

The three quick search options are:
Select the appropriate search limit option by clicking the "V" next to the magnifying glass in the search box.
Advanced Search
There is also the option for an advanced search, accessed using the step above.
Here you can use multiple criteria in your search, such as a combination of words from the title of an article, the year of publication, an author, or when you added the reference to Zotero. You can also limit your search to specific collections and subcollections.

You can create a relationship between items in your library using the Related feature. A few examples in which this might be useful would be to connect book chapters to the book in which they were published, conference presentations to articles about the same research study, or references to the article you found them in.
To relate items, select one in the center pane and choose the Related icon in the details pane.

Click the "+" icon to create a relationship. You can browse or search for the reference(s) you want to relate. Highlight the appropriate reference(s) and click "Select."

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