I've done a quick test and this seems to work (WinXPsp2):

Control Panel > Java icon (opens Java Control Panel) 
> "Java" tab > "Applet run-time configuration" > "Show" button 
> on row "JRE" (latest version if there are several), click on the textbox 
> under "Parameters" and type:

-Xmx###m

where ### is the amount of memory in MB (hence the "m" after it)

I can only enter values up to -Xmx256m; higher gives an error. But I 
have 512 MB RAM, maybe with more memory you can go higher.

The expanded memory is working, as my empty Jmol applet says by 
default (pop-up menu, About)
        13 MB used
        6 MB free
        95 MB max
and, after the trick, it says
        13 MB used
        6 MB free
        254 MB max

I will try to remember to add all this to the Wiki at
http://wiki.jmol.org:81/index.php/Jmol_Applet





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