I looked into that file, and have 2 points:
All Harkonnen are misantrops (hate everyone), i'd make their base attitude -1 and beast rabban -2
I interpret this base attitude as "how willing are people to deal with you".
First, I want to try to move *away* from the just "Harkonnen = bigbadbruteforce".
Vladimir in particular isn't like that; he is cunning and devious, he'll use violence or brutality for a purpose, but he is also very good politically. Vladimir is a *smart* villain; Rabban is a brute force one. And Feyd is young and charismatic; people like him. Hence the positive value.
Second, none of the civs in vanilla have a -2 value there. They are all either -1, 0, 1 or 2.
So Rabban got the lowest, Vladimir the second lowest (no-one really trusts him), and Feyd +1.
Harkonnen are all power hungry, but that doesn't mean that they can't be good manipulators, or can't use diplomacy. Vladimir could well have ended up making Feyd emperor, if Paul had died in the desert.
Leto and Paul should probably be 2 though.
The both shoud be warmongers. Roma is to peacefull in your set, but as i see her in videos she is very evil , swift and agressive. IMO She should be much like Cathy in vanilla personality wise. Fast REX and xpansion, backstab. Executrics should be less REXer, more military and warmonger type, but they both should have hight WArProb, and should be easy to bribe (espessialy Roma) . They love to trade techs, and more they will love to DoW just because some tasty tech.
All Ordos should have Spy on 150 - its just race , BTl should be 150 on espionage too.
I disagree that the Ordos should just be brute-force warmongers. I have made the Executrix more militaristic, but Roma more diplomatic. They are both very very mercenary; its easy to bribe them to go to war. This is already there; look at the DeclareWarRefuseAttitudeThreshold values and the DeclareWarThemRefuseAttitudeThreshold values.
They can be bribed to go to war by anyone, and they can only *not* be bribed to start a war with people they are Friendly with; the highest category.
The key thing about Ordos is that they are mercenaries and infiltrators. Why start a war unless you're getting paid to do so, given that you can wreak havoc with your enemies with espionage without *needing* to declare war.
I gave Roma the highest espionage value in the game, and the Executrix a slightly lower one but still quite high (being more militaristic).
For both of them, war of assassins is their preferred civic (big espionage bonuses).
There is no tech gain from conquest, so going to war for tech doesnt' really make sense here, unless you can wring it out of a peace deal, but you're only going to do that if you're stronger.