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Stimulated Electron Spin Polarization in Strongly Coupled Triplet–Doublet Spin Pairs

机译：强耦合三重态-双重态自旋对中的受激电子自旋极化

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摘要

The possibility of stimulating electron spin polarization in a system consisting of a stable paramagnetic center and a chromophore that can be excited into its triplet state is discussed. In such systems, the doublet state of the paramagnetic center couples to the excited triplet state of the chromophore and if the coupling is larger than the difference in the precession frequencies of the doublet and triplet, the eigenstates of the coupled system are quartet and doublet states. The quartet state is usually the lowest energy excited state. Following light excitation, the initial electronic relaxation to the quartet state generates strong multiplet polarization if it is governed by the spin–orbit coupling that follows the molecular symmetry. It is shown that application of a selective π-pulse to the ±3/2 ↔ ±1/2 transitions of the quartet converts this multiplet polarization into net polarization. The magnitude and orientation dependence of the generated polarization is estimated on the basis of a simple analytical model. The experimental conditions required for this net polarization to be retained in the ground state after decay of the quartet state are discussed. The viability of using this as a method to enhance the signal strength of a spin label or metal center in selective excitation experiments is considered.
机译：讨论了在由稳定的顺磁中心和发色团组成的系统中激发电子自旋极化的可能性，发色团可以被激发成三重态。在这样的系统中，顺磁性中心的二重态与发色团的激发三重态耦合，如果耦合大于二重态和三重态进动频率之差，则耦合系统的本征态为四重态和二重态。 。四重态通常是最低的能量激发态。在光激发之后，如果由遵循分子对称性的自旋-轨道耦合控制，则初始电子弛豫到四重态将产生强多重峰极化。结果表明，在四重奏的±3/2↔±1/2跃迁上施加选择性π脉冲，可将这种多重极化转变为净极化。在简单的分析模型的基础上估算了产生的极化的幅度和方向依赖性。讨论了在四重态衰变后将这种净极化保持在基态所需的实验条件。考虑了在选择性激发实验中将其用作增强自旋标记或金属中心信号强度的方法的可行性。

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