Transient nucleation effects in glass formation

We extend to the non-isothermal case a numerical technique that was developed to treat transient homogeneous nucleation in a one-component system by modeling directly the reaction by which clusters are produced. Calculations are presented for the nucleation frequency during the quench and for the number of nuclei produced and the volume fraction transformed at the end of quench for different rates of cooling from the melt. Three model systems are considered: an alkali silicate which is a relatively good glass former, and two metallic glasses. These show a wide range of critical cooling rates for glass formation. In some systems transient effects are predicted to be critical for glass formation. A simple technique is presented for determining when transient effects are important based on a calculation using steady state nucleation frequencies and macroscopic growth velocities.