Abstract

In this work, internal 4T1→6A1 transitions within the half-filled 3d shell of Fe3+ in extremely pure chemical vapor deposition (CVD)-grown ZnO layers were investigated by means of high-resolution, low-temperature continuous wave (cw) photoluminescence (PL), time-resolved PL, photoluminescence excitation (PLE) spectroscopy, Zeeman spectroscopy, and deep level transient spectroscopy (DLTS). For comparison, Zeeman spectroscopy measurements were also performed on commercially available, hydrothermally grown ZnO bulk crystals. Magnetic fields up to 15T were applied parallel and perpendicular to the c-axis of the ZnO crystals in order to investigate the fine structure of included states. The splitting pattern of emission lines related to 4T1→6A1 Fe3+ transitions was theoretically modeled by a Hamiltonian matrix including the crystal field in cubic and trigonal symmetries and spin–orbit interaction for the complete excited 4T1 state. The extremely pure ZnO used in this study, in direct comparison to hydrothermally grown ZnO, allows the identification, investigation, and description of single isolated Fe3+ defects in ZnO for the first time—different from literature reports hitherto, which seemingly were recording data on Fe–Li complexes. The resulting exact energy-level scheme in combination with the experimental data leads to a re-evaluation of 4T1→6A1 Fe3+ transitions in ZnO.

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