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In the sentence

'The' is one of the most frequently used words in the English language.',

if I deleted the word 'frequently' wouldn't the meaning of the sentence be unchanged? If this is the case, is the expression 'most frequently' right? Wouldn't the word 'frequently' be redundant? I argued with someone that the expression 'most frequently used' is incorrect (or atleast unnecessary).

But Ngrams tells me a very different story. Google search results are certainly higher for 'most used' than 'most frequently used'. But the numbers for the latter are very high as you can see.

I want to know if there is a difference between the two, and if not, which one is a better choice. Thanks in advance.

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In general, the answer depends on the nature of the usage. In your example you're correct. Consider two kinds of usage:

With words, all there is is frequency; if you use a word, that's a use.

On the other hand say you own two cars. You use one frequently for short trips, the other infrequently for extremely long trips. Your most frequently used car and your most used car are likely to be different vehicles.

Ngrams of "most used" and "most frequently used" aren't relevant for this question because the popularity of those phrases has nothing to do with which is applicable. As DRF notes, the Ngrams might not even be capturing what you think you're requesting even if the phrases were relevant.

The phrases do have different meanings, but word use and word frequency happen to be the same numbers.

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It's worth being wary of both google searches and google n-grams for linguistic research. Even n-grams can easily lead you astray. "Most used" might not be a synonym for "most frequently used" such as in "Most used cars sell for less then one third of their original price." And n-grams have no way to pick up on that.

Google search is much much worse though. There is a nice article someplace on language log http://languagelog.ldc.upenn.edu/nll/ , that I can't find at this moment, which explains that as much as linguists would love to use google for analysis it is no longer possible since google search has for some time now been searching for what it thinks you are looking for as opposed to what you tell it to look for.

Having said that "most frequently used" sounds perfectly idiomatic to me and I would certainly use it instead of "most used" which sounds stilted.

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