Well, I completed a batch of chili using smoked chuck instead of browned chuck. TL;DR: The results were excellent! I found that the smoked meat flavor balanced out the spiciness of the peppers even more than the other ingredients (see below), but still allowed the flavor profile of the peppers to come through. There is definitely a place for browned meat in place of smoked in this chili. The result is a bit more delicate flavor, with much more spiciness from the peppers. That said, I really like the smoked option!
The recipe I used is the one I had been using for awhile, and is unlike most of the suggestions I've see in this thread and others on SMF -- which I'm sure are very good as well; no offense intended. I attached a Word document with the recipe to my original post, but I'm not sure how attachments are handled here, so if you want the recipe and can't access it, I'll try to post it another way. The chili I'm describing here is very much like the chile con carne that is often served atop tamales in Mexican restaurants.
Here are two pictures of the key ingredients I used. Not pictured are a large onion and a bottle of beer. The pictures contain 7 types of dried peppers plus a can of chipotles in adobo sauce. I used all but the dried puyas. Dried peppers have to be toasted and soaked in water in order to make the pepper puree. When you're toasting these, you'll note that the aromas contain hints of chocolate and berries among other pleasant things. Blending the different types of peppers creates a very complex flavor profile that I really like. These can be very spicy, but I find that their flavors mellow out during cooking and as ingredients like beer, chocolate, and masa are added during the cook. I remove almost all seeds and ribs before toasting them in order to keep the spiciness manageable.
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My chuck roast was just over 5 pounds before cooking, and cost just over $41. I smoked it in my Smokin-It Model 2 with a box temp of 250 targeting 180 IT. Before smoking, I dry-brined with Kosher salt for about 4 hours. After 15 hours in the box, the IT was 165 and the roast was drying out, so I pulled it. I pulled the roast apart along the connective tissues and tried to remove as much of those tissues at as possible, then cut it into 1 inch cubes. Here is a picture of the cubed chuck. It may not be clear from the picture, but the exterior surfaces accumulated lots of tasty bark. I used a mix of pecan and hickory for the smoke.
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The cooking process consisted of sauteeing onion and garlic in the Dutch oven after frying up some bacon. Then the cubed meat is added along with the dry spices, bacon bits, some water, a cup of coffee, and a bottle of beer. The pepper puree is then added, the chili is brought to a boil, then simmered for 5 hours. Note that I did collect drippings from the smoking process. Those were extremely salty from the dry brine but otherwise very tasty. I couldn't use all of them, but I did use several tablespoons in place of salt in the chili. After 5 hours, masa and chocolate are added and the chili is cooked for another 30 minutes or so and it's "done". Here is a picture of the finished chili:
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Thanks again for the thoughts and ideas. I'm pretty sure there is more experimentation on this topic in the future for me!