The problem with the code is, when I try to generate a number, if the spin is equal 1 it generates values inside range (1,2,3) if if try to use the loop to sum random values
The problem is that you are creating random generators too close in time. The random generator constructor uses the current time to seed the generator, and when you create them too close in time they will all be seeded using the same time.
Create one random generator and use in the loop:
Random rnd = new Random();
for (int i = 1; i <= spind3.Value; i++) {
diceCalc[1] += rnd.Next(1, 4);
}