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It depends on the complexity of the calculation, what it is operating over (how many cells/rows/columns), are you using a Tableau data extract or a live connection to the Excel file, etc.
With my volumes of data (10M records or less, often a lot less, almost always using Tableau data extracts) I try to do most of my calcs in Tableau. However there are some "data prep" things that are effectively slowly changing dimensions like whether a patient has a history of chronic obstructive pulmonary disease that I pre-compute outside of Tableau. There's also a limitation of joining tables where we we can't create a calculated field in Tableau and then join on those results (though we can often do that with a Tableau data blend).
Given Excel's volume limitations that shouldn't be an issue, however depending on how complex your calcs are that may affect performance enough to need to do them in Excel. There are also calculations that can be performed in Excel (in particular highly iterative calcs) that are either not possible or not very feasible in Tableau unless you are using the R integration.
Thank you, Jonathan. It sounds like the best way to determine this is by trying both.