Ab Initio Study of the Dynamical Si–O Bond Breaking Event in α-Quartz*

The Si–O bond breaking event in the α-quartz at the first triplet (T1) excitation state is studied by using ab initio molecular dynamics (AIMD) and nudged elastic band calculations. A meta-stable non-bridging oxygen hole center and E' center (NBOHC-E') is observed in the AIMD which consists of a broken Si–O bond with a Si–O distance of 2.54 A. By disallowing the re-bonding of the Si and O atoms, another defect configuration (III-Si/V-Si) is obtained and validated to be stable at both ground and excitation states. The NBOHC-E' is found to present on the minimal energy pathway of the initial to III-Si/V-Si transition, showing that the generating of the NBOHC-E' is an important step of the excitation induced structure defect. The energy barriers to produce the NBOHC-E' and III-Si/V-Si defects are calculated to be 1.19 and 1.28 eV, respectively. The electronic structures of the two defects are calculated by the self-consistent GW calculations and the results show a clear electron transition from the bonding orbital to the non-bonding orbital.