The best indicator of spontaneity in a reaction is the change in Entropy (S or DS). The Second Law of Thermodynamics states that for a reaction to be spontaneous there must be an increase in entropy. For a process to be spontaneous the free energy must be -ve Reason: The change in free energy is related to the change in enthalpy and change in entropy. The change in entropy for a process must always be positive if it is spontaneous.