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I love the models and the fluff, just wondering what their general play style was before I pick some up...

In my experiance, Buff stacking is what they really do good.

They also (generally) don't run many beasts well, they usually have a couple and then mainly infantry. There's a couple of casters than can run more beasts but generally they're an infantry faction, kinda like Khador in Warmachine. But then most of their infantry is on medium bases and tough.

They tend to be more infantry heavy (and reliant) than most other hordes factions, though there are a few decent beast casters. They tend to lean more towards attrition and tough bricks than anything else - they can do faster and tricksy things, but it's not their forte. They tend to be more melee focussed than ranged, (though some recent releases do help with their ranged game). Stacking buffs, and support is very important to them.

I mean there are always exceptions to any of these generalities, but a lot of good builds for Trolls focus on taking a lot of tough, high ARM infantry (often multi-wound), and just wearing the enemy down.

Do you like Tough?

As others have said: the stereotypical Trollblood strengths are attrition-focused, with lots of tough jamming units, and some great beasts.

Newer releases have given them some interesting ranged options, though.

I really like the warcaster models and fluff for Jarl and Gunnbjorn. How do these warcasters typically play? Are they popular warcasters?

I don't know about Jarl, but i think Gunnbjorn isn't meant to be a very good caster.

Jarl Is fairly flexible in his army composition. His main schtick is boosting the mobility of your army while he puts his pistols to good work. As with most troll casters, he can run a couple of beasts, but will mainly want infantry.

Gunnbjorn has a fair bit of support for ranged units/beasts. He can increase the range of your ranged weapons, make his warbeasts more accurate, and create walls to protect your army. -Technically- he can run a decent amount of ranged warbeasts (more than 3), but it's not always advised. I believe he works well with a combined arms approach.

Lots of discussion about Gunny with the new Troll Highwaymen -- right now, it's still mostly theory, though.

Gunnbjorn is believed to have been one of the worst warcasters in the game till Dozer & Smigg came out who's got affinity Gunnbjorn that gives Dozer & Smigg auto boosted blast damage rolls.

Along w/ Gunn's spells that gives boosted attack rolls makes for good synergy with each other.

I've only been playing a short time with trolls always as a in your face smash you into the dirt style but with Gunn Dozer and Smigg and the new highway men coming out I'm tempted to try troll shooty to see how it would work.

Are Jarl or Gunnbjorn particularly compatible with the starter box?

Well, theoretically the two Impalers can benefit greatly from Gunnbjorn's Guided Fire spell that makes all their shooting attack boosted because it is always a good thing to boost a shoot with some nice critical hit damage. On the other hand, the animus of the Impaler is a spell that Gunnbjorn already has, so they do not synergize this way.
Gunnbjorn does not synergize a lot with the axer either, because he is not ranged. All in all, I would say he works okay with them, but nothing spectacular.

Bricky and Tough. Popular lists these days seem try and play like cramming your opponents mouth full of peanut butter and hoping they choke to death, or at least run out of time. Buff stacking is a major a component. They're not slow (getting high speeds on individual models for them is trivial) but lack real mobility for an overall force, especially on a consistent basis.