LAA is just another 4 gig patch applet, and all it does is alter the header bit in the SH4.exe file that then shows to Windows that the game is able to address memory properly, which is known as making the exe "Large Address Aware". The differences between the various apps just has to do with their respective front-ends, and what they are written with. If you see LAA netFramework, it uses the newer netFramework dll calls, instead of the "traditional" Windows API calls. So no matter the program, they all accomplish the same thing.
Specifically at LAA, the default interface when it first loads is "Basic", which is fine. There is a write-up in the FotRSU Support folder in the "Install Notes For the Various Versions of SH4 in Windows.pdf" file, starting on Page 10, with pictures (I like pictures... ) on Page 11. The 'basic' idea is to click on that ellipse box [...] under "Step 1: Select an executable", and browse to the proper folder to select the proper "SH4.exe" file. That should then fill in the Step 1 box, and activate the "Step 2: Large Adress Aware flag", which if it is empty, click in the little box to put a check-mark in there. If there is already a check-mark in there, leave it. Once that is finished, then "Step 3: Commit Changes" and the "Save" button become active. Hit the "Save" button, then click on the little "X" icon in the upper-right corner to close the dialog, and you should be good to go! Windows does the rest (that's not scary).