Frequently I get the same question. Why Assyrians are close to Armenians in various charts. The answer to this question is both simple and complicated.
Simple because Assyrians do have extra non Levantine ancestry which pulls them away from other Levantine people. And make close to Armenians. Which btw is also visible in Y dna structure of Assyrians.
But it's also complicated because one should understand that history of an ethnic group do not stop in Iron Age. So one must learn the whole history how Arameans initially living Syria became modern Assyrians. Morever an ethnic group over time can transform into ethno-religious group which can affect seriously the genetic structure of that population. This part is beyond the scope of this thread. So my point will be genetic.
The first PCA shows the relative position of Assyrians marked as Arameans. Notice if they had simply Armenian admixture they would be between Levant and Armenia. But they have also a shift toward Iranian pops. Which means that they have extra Iranian ancestry or something related to them. In the second PCA it's visible that Georgian Jews also plot in the same place as Assyrians.
This fits well with the geographic position of Assyrians (NW Iran, North Iraq, East Turkey etc) It must be noted that North Iraq probably had witnessed number of migrations from Iran (Gutians, Carduchoi , Turukeans etc ) So that region almost certainly had an extra Iranian shift before the arrival of real Iranians in Iron Age. As for Jews there are historic records mentioning Adiabene people and even some Iranian nobility converting to Judaism ( like Amatuni ) Good knowledge of history is needed for better understanding this genetic results.