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Chemical nature of point defects, their segregation, cluster or complexformation in ZnO is an important area of investigation. In this report, 1.2 MeVAr ion beam is used to incorporate defects in granular ZnO. Evolution ofdefective state with irradiation fluence 1 x 10^14 and 1 x 10^16 ions/cm2 hasbeen monitored using XPS, PL and Raman spectroscopic study. XPS study showspresence of oxygen vacancies (VO) in the Ar ion irradiated ZnO. Zn(LMM) Augerspectra clearly identifies transition involving metallic zinc in the irradiatedsamples. Intense PL emission from IZn related shallow donor bound excitons(DBX) is visible in the 10 K spectra for all samples. Although overall PL islargely reduced with irradiation disorder, DBX intensity is increased for thehighest fluence irradiated sample. Raman study indicates damage in both zincand oxygen sub-lattice by energetic ion beam. Representative Raman modes fromdefect complexes involving VO, IZn and IO are visible after irradiation withintermediate fluence. Further increase of fluence shows, to some extent, ahomogenization of disorder. Huge reduction of resistance is also noted for thissample. Certainly, high irradiation fluence induces a qualitative modificationof the conventional (and highly resistive) grain boundary (GB) structure ofgranular ZnO. Low resistive path, involving IZn related shallow donors, acrossthe GB can be presumed to explain resistance reduction. Open volumes (VZn andVO) agglomerate more and more with increasing irradiation fluence and finallyget transformed to voids. Results as a whole have been elucidated with a modelwhich emphasizes possible evolution of new defect microstructure that isdistinctively different from the GB related disorder. Based on the model,qualitative explanations of commonly observed radiation hardness, colourationand ferromagnetism in disordered ZnO have been put forward.

Clustered vacancies in ZnO: Chemical aspects and consequences on physical properties