Spin-orbit coupling induced homogeneous broadening of the acetone ODMR transitions

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Abstract
The zero-field ODMR transitions of the acetone triplet state were observed to be homogeneously broadened. The linewidths (4 and 8 MHz for the Tx1 −Ty1 and Ty1 −Tz1 transitions, respectively) do not change upon deuteration. Thus broadening due to fluctuating (proton or deuteron) hyperfine fields has to be ruled out. Instead the homogeneous broadening is related to the spin-orbit contribution to the zero-field splitting of the acetone 3nπ* state which was evaluated previously. A straightforward calculation based on Zewail’s idea, that the spin-orbit coupling strength correlates with the homogeneous linewidth for 3nπ* states, is in fairly good agreement with the experimental results.