Hyperspy is surely nicely suited to do these fits, in particular if you want to build your own fitting equations and estimators or want to play with different fit-algorithms.
Unfortunately, I myself am not (yet) experienced enough in it to point you in any direction. (Others hopefully will.)
There is some documentation on curve fitting in the documentation at http://hyperspy.org/hyperspy-doc/current/user_guide/model.html
However, I'm replying to this email because I know that custom plasmon fitting was done with DigitalMicrograph-scripting in at least one publication:
Nanoscale temperature mapping in operating microelectronic devices
M.Mecklenburg et al
Science 06 Feb 2015, Vol. 347, Issue 6222, pp. 629-632
As far as I know, this wasn't done using the NLLS fitting from the menu (which only does Gaussians), but with the general Fitting tool which is available from the "Data Fit" technique in the "Data Analysis" group of GMS 3. This tool can also be accessed by the scripting language. If you contact the first author (Matthew Mecklenburg) he can possibly share the details.
Also: Should you happen to be around at M&M Baltimore this week, make sure to visit the Gatan booth (and ask for Paul Thomas). He possibly has some interesting news regarding fitting and data analysis in the upcoming GMS version.
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