1964 Valiant wheel allignment

Strange that he requires toe-in in degrees since inches (or mm) is more common. Surely the manual for his alignment machine gives a conversion or might even be in the software. In general, you want as much caster as possible, to allow radial tires. That is the shopping-cart effect. Your car was designed for bias-ply tires which deflect the tire-patch backwards. For radials, you want to move where the projected line thru the ball joints hits the road forward. Push the front bushing pivot of the upper-control arm as far out as possible and pull the aft one inward. That will move the upper ball joint center as far aft as you can. Moog offset bushings make this easier, but ignore their instructions which are to correct bent parts from an accident. That simultaneously affects camber (how tires lean in at top). Aftermarket adjustable tubular upper-control arms make it easiest. You can't adjust where the lower ball joint sits since the strut rod allows no adjustments.

Camber is kind of a personal choice. Some get carried away, with the tops of the tires leaning far inward, for better cornering. Rice-tuners go crazy, even using curved motorcycle-like tires. Your car actually spec'ed the tires leaning slightly outward at top (positive camber). Straight-up isn't bad to improve tread-wear, but most set slight negative camber.

Toe-in is the most critical for handling and tire wear. RWD should set slight toe-in since the wheels rotate outward slightly when driving, depending on how much play in suspension and steering (want them exactly parallel when driving). I set 1/16" toe-in with new tight parts, or 1/8" if slight play. I use a tape measure across front and aft sides of the front wheels, which is easiest if the tread has straight channels. I also hold a straight-edge along a front tire and sight at the rear. Easier for FWD where you set slight toe-out since your sight then should hit slightly inward on the rear tire (1st channel), assuming the track width is the same for fronts and rears. Too much toe-in will quickly wear the inside tread. Even a little toe-out while driving will cause the car to wander.