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Abstract: The formation of strained layers and a non-monotonic evolution of strain in high energy (100MeV) silver ion (Ag7+) irradiated undoped semi-insulating GaAs are observed and analyzed using Raman scattering and high resolution X-ray diffraction (HRXRD) measurements. At low fluence, compressively strained layers are formed, whereas, with increase in fluence both compressive and tensile strains appear as observed from HRXRD measurements. Further, at low fluence, the change in compressive strain with increase in fluence is found to be sharper than what is observed at higher fluence, thereby suggesting a critical fluence value, beyond which there is a simultaneous generation and annihilation of vacancy type defects. The initial blue shift and subsequent relative red shift beyond above critical fluence in the Raman peak also qualitatively reveal non-monotonic evolution of strain in this case. Finally, we demonstrate the sensitivity of Raman spectroscopy in detecting the decrease in lattice ordering in the crystal in the low fluence regime, below the detection limit of Rutherford back-scattering channeling (c-RBS) measurements. [Copyright &y& Elsevier]