Titanium-related color centers in diamond: a density functional theory prediction,Journal of Materials Chemistry C

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Titanium-related color centers in diamond: a density functional theory prediction
Journal of Materials Chemistry C ( IF 5.7 ) Pub Date : 2018-04-19 00:00:00 , DOI: 10.1039/c8tc00097b
Kamil Czelej _{1,

2,

3,

4,

5} , Karol Ćwieka _{1,

2,

3,

4,

5} , Piotr Śpiewak _{1,

2,

3,

4,

5} , Krzysztof Jan Kurzydłowski _{1,

2,

3,

4,

5}

Affiliation

Transition metal-related paramagnetic centers in diamond exhibiting bright photoluminescence are increasingly important defects for realizing high quality solid state single photon sources. Recently, advanced ab initio calculations of single nickel-related NE4 (nickel-vacancy) and NE8 (nickel-vacancy-nitrogen) complexes in nanodiamond provided an insight into the nature of optical transitions and demonstrated their potential for in vivo biomarker applications. For other transition metal-related defects in diamond, however, a comprehensive understanding of photoluminescence is rather scarce. Here we used first principles, hybrid density functional theory analysis to investigate the electronic structure and magneto-optical properties of titanium-related point defects in diamond. Our theoretical results including the paramagnetic S = 1/2 ground state, the calculated zero-phonon lines, quasi-local vibrational modes associated with Ti atoms, and hyperfine coupling parameters provide strong evidence that the neutral Ti–N and TiV–N complexes are indeed the experimentally observed N3 (titanium–nitrogen) and OK1 (titanium-vacancy–nitrogen) color centers. In addition, we predicted another low energy excitation in the spin minority channel of the TiV–N⁰ defect that needs further experimental verification and might be an interesting candidate for a robust solid state single color emitter in the near IR region. In the case of a yet unobserved, neutral TiV (titanium-vacancy) defect we found a high symmetry D_3d configuration in the triplet ³E_u ground state and we calculated the magneto-optical parameters to mediate its future identification. We emphasize the possibility of the dynamic Jahn–Teller effect for some centers and its impact on the experimentally observed hyperfine structure.

中文翻译：

钻石中与钛有关的色心：密度泛函理论的预测

金刚石中表现出明亮的光致发光的与过渡金属有关的顺磁中心，对于实现高质量固态单光子源而言，是越来越重要的缺陷。最近，对纳米金刚石中单个与镍相关的NE4（镍空位）和NE8（镍空位氮）复合物的从头计算得到了深入的了解，并证明了光学跃迁的本质，并证明了它们在体内的潜力。生物标志物的应用。但是，对于钻石中其他与过渡金属有关的缺陷，对光致发光的全面了解还很少。在这里，我们使用第一原理，混合密度泛函理论分析来研究金刚石中钛相关点缺陷的电子结构和磁光特性。我们的理论结果包括顺磁性S = 1/2基态，计算出的零声子线，与Ti原子相关的准局部振动模式以及超精细耦合参数提供了有力的证据，证明中性Ti–N和TiV–N络合物是实际上，实验观察到的N3（钛-氮）和OK1（钛-空位-氮）色心。此外，我们预测了TiV–N自旋少数通道中的另一个低能激发⁰缺陷需要进一步的实验验证，并且可能是近红外区域中鲁棒的固态单色发射器的一个有趣的候选者。在尚未观察到的中性TiV（钛空位）缺陷的情况下，我们在三重态³ E_u基态中发现了高度对称的D _3d构型，并计算了磁光参数以介导其未来的鉴定。我们强调了某些中心动态Jahn-Teller效应的可能性及其对实验观察到的超精细结构的影响。

更新日期：2018-04-19

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