AB,
I'm guessing that what you are seeing is erratic ignition. If you still have it, even with the increased charge, you might try backing the new load down 5% and use a magnum primer and work back up to see if that settles it any. At 4.9 grains you are at less than 25% case fill, so there is a lot of empty space for the primer to pressurize. If not, I would be checking that the gun's chamber diameters are the same (often they are not on a revolver) and you get them reamed to match, which also generally improves accuracy.
I don't know what barrel length you have, but for the 6.1 grain load, for various revolver barrel lengths (revolver barrel lengths don't include the chamber, as pistol barrel lengths do), and assuming a chamber and barrel identical in dimensions to the one Hodgdon has (that caveat is always there), QuickLOAD has:
Velocities for 6.1 grains 231 in .44 Colt seated 0.135" different revolver barrel lengths.
2": 678 fps
3": 753 fps
4": 806 fps
5": 846 fps
6": 878 fps
7": 904 fps
8": 926 fps
You can interpolate those barrel lengths for what you actually have, then, as you work up, if you get a pressure sign, like sticky case extraction, you stop. If you hit 6.1 grains before you hit the velocity listed for your barrel length, then you stop, or if you hit the velocity first, you stop. That's a good first step.
QuickLOAD actually thinks you could get as high as around 7.0 grains and over 1000 fps (8" barrel) loaded to CIP specs, but I'm inclined to stick with Hodgdon's pressures for the time being and if and only if there are still zero pressure signs, think about going up. I am mentioning it here only to give you a sense that there is still some safety margin likely available. But again, only the pressure signs will tell.
Trail Boss should work well. I do not trust QuickLOAD's model of this powder because the maximums come out too much higher than those Hodgdon publishes. But it will fill the case way better and that may eliminate some of your erratic velocity results, so I expect it's worth a try.