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素晴らしいcalligraphyを素晴らしいものたらしめているのは何かについて学んだ。

I studied what makes great calligraphy to be great.

With regard to たらしめる I don't understand that sentence structure. The presence of means there must be a transitive verb in play (たらしめる?). But, what is もの doing there?

Basically, with regard to sentence structure, what part of speech is "もの"? What does it modify or what is it modified by?

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Did you check a Japanese dictionary for たらしめる? It comes from たり→たら+しめる.

たり is one of the classical copular verbs and is analyzed as a sound change of と+あり; this is the same と you see in things like [呆然]{ぼうぜん}する.

This is then conjugated to its 未然形 (which naturally mimics あり's): たら.

To this a classical helper verb, しむ, that functions as a type of causative like させる (it has other functions too), and survives in set expressions as しめる in the modern language, is added.

=たらしめる≈であらせる・にする・にさせる・にしてあるようにする

〇〇こそ、人を人たらしめるものだ
It is precisely 〇〇 that makes man man.

And もの can be used to give a concrete / obvious feeling to a statement.

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