I would recommend that you set the high idle under no-load (neutral or park). The no-load speed will be around 200-300 rpm higher than the defuel rpm. The reason for this is that the extra rpm is needed to spin the flywheights on the governor fast enough to produce the necessary force to overcome the spring tension. I don't think it makes sense to set the high idle in 2nd gear as the engine will have a load on it and you won't get an accurate reading. 2nd gear can be used to find your defuel point though. The reason for using 2nd gear is that you'll be going at a relatively safe speed while taking readings. If you try it in 3rd, you'll probably be at about 70mph, and in OD around 100mph.
Cheers,
Sean