Tailoring the size and size distribution of nanoclusters through ion irradiation

Nanoclusters (N) can be generated by ion implantation of impurity atoms into a host matrix and subsequent phase separation of the impurity phase from the matrix during annealing. This is a CMOS technology compatible process, which has great potential for applications. However, a serious problem arises: The NCs have a broad size distribution, which obscures the size dependent characteristics of the NCs.
Here, we show that irradiation of NCs with high-energy ions can be used to overcome this problem. During irradiation, the collisional mixing at the NC-matrix interfaces competes with phase separation. A negative interface tension can be the consequence, which can only be understood in terms of non-equilibrium thermodynamics. The negative interface tension leads to unexpected results: The system will evolve towards a state of maximal surface area!! Thus, a flat interface
becomes instable. Here, we focus on the Gibbs-Thomson relation with a negative interface tension, where we find an increasing solute concentration with increasing NC size. This is inverse to equilibrium behavior. Consequently, we find inverse Ostwald-ripening, e.g. small NCs grow at the expense of large ones. This can be used for the fabrication of monodisperse NCs. These theoretical predictions have been verified by kinetic MC simulations and by ion irradiation of Au NCs in a SiO2 matrix.