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First, be careful in Salta. 3 years ago my wife had her purse with her documents, cell phone, etc, stolen during breakfast at Continental Hotel near the bus station. Be suspicious of men with a coat in his arm, it is a way to hide stolen goods. I continue going to Argentina and Chile every year driving from Brazil, only I am more careful now.

From Cafayate to Tilcara, and continuing to La Quiaca the roads are paved and safe. I prefer Purmamarca, see also Uquia, Maimara, and if you have time, see Humahuaca (don´t miss), La Quiaca and Yavi.

The roads are very scenic, specially from Cafayate to La Viña and from Yala (near Jujuy) to Purmamarca and La Quiaca. Driving slow and stopping many times for photos it takes more, usual time to travel from Salta to Cafayate about 3 h, 1 1/2 h (usual road) or 2 1/2 h (mountain road) from Salta to Jujuy, and a one hour from Jujuy to Purmamarca, less than 1 h from Purmamarca to Tilcara.

A good place to sleep near Cafayate is in Cololao del Valle, there is a good, inexpensive, friendly hotel owned by the municipality. The tourism office in Cafayate main square has all information about free visits to the vineyards and other interesting places. In Dec you can eat Torrontes grapes, typical from the region, there are not so many grapes delicious to eat and good for wine.

I think a good alternative is one day in Salta and one in Jujuy, smaller and as interesting as Salta. There is a slow, paved, interesting road from Salta to Jujuy thru the green mountains with lovely towns (La Caldera).

From Humahuaca up to La Quiaca the people, clothes, traditions are more similar to Bolivia than to Argentina. It is higher, colder, lots of llamas and other animals, domestic and wild. It doesn´t take long from Tilcara to La Quiaca. Yavi is about 25 km more, scenic good road, very interesting museum and church with translucid stone windows.

The best way to enjoy the region is with a rented car. You will stop many times for photos.

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Jaloisio is a man after my own heart! I would agree with him - hire a car in Salta (ask your hotel / hostel). Worth a visit are the Termas de Reyes near Jujuy: stay a night (not expensive) in the hotel and pamper yourself with hot spas etc. The only word of caution about driving in Salta (probably the same in most Argentine cities bilut on the grid system - becaise of the one way streets, sometimes you have to do a bit of navigating to get to your destination if it is the wrong way round from where your car is geaded! Also, be careful at junctions, where, I think, you have to give way from the right.