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It's pretty straightforward. That file you uploaded is a zip file. If you "unzip" the file, you can add new files to it. Simple create a text file and rename it to ".itch.toml" and place it in the folder with the other files. Then rezip everything into a new zip file. When you upload the new zip file, users should be able to automatically download your game through itch.

I have created a text file called .itch.toml let me know if it works now.

It doesn't seem to work. Make sure the file is in the root directory of the ZIP file and not within a folder.