I center rectangular stock in the 4-jaw similar to the way shown in the video. However, I mount the DTI on the cross slide, come at the stock horizontally, and use the DTI only as a null device. I use the digital readout (DRO - I could use the screw dials if I didn't have a DRO) as a measuring tool to find out how far off center are the opposite sides of the stock, cranking in the cross-slide and rocking the chuck until the DTI reads 0.000 at the low spot. I back out the cross-slide, turn the chuck 180 degrees, and wind the cross-slide back in until, while rocking the chuck, the DTI reads 0.000 again. The difference between the two DRO readings (or screw collar readings) is the eccentricity. I then know I need to park the cross-slide at the average of the two readings and then drive the stock laterally with the chuck jaws until the DTI again reads 0.000. That usually gets me darn close. Then I switch to the other pair of sides and bring those into truth. I then go back and check the pair of sides i did first to make sure it's position didn't change. It usually does a little.
I also use this technique to produce known amounts of eccentricity, as for a steam engine eccentric. However, once eccentricity becomes too large, the chuck jaws don't grip the part correctly, and I have to switch to alternate ways of holding the part.