Crystalline Arrays of Copper Porphyrin Qubits Based on Ion-Paired Frameworks,Journal of the American Chemical Society

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Crystalline Arrays of Copper Porphyrin Qubits Based on Ion-Paired Frameworks
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-08-08 , DOI: 10.1021/jacs.3c04786
Casandra M Moisanu ₁ , Robert M Jacobberger ₁ , Luke P Skala ₁ , Charlotte L Stern ₁ , Michael R Wasielewski ₁ , William R Dichtel ₁

Affiliation

Molecular electronic spin qubits have great potential for use in quantum information science applications because their structure can be rationally tuned using synthetic chemistry. Their integration into a new class of materials, ion-paired frameworks, allows for the formation of ordered arrays of these molecular spin qubits. Three ion-paired frameworks with varying densities of paramagnetic Cu(II) porphyrins were isolated as micron-sized crystals suitable for characterization by single-crystal X-ray diffraction. Pulse-electron paramagnetic resonance (EPR) spectroscopy probed the spin coherence of these materials at temperatures up to 140 K. The crystals with the longest Cu–Cu distances had a spin–spin relaxation time (T_m) of 207 ns and a spin–lattice relaxation time (T₁) of 1.8 ms at 5 K, which decreased at elevated temperature because of spin–phonon coupling. Crystals with shorter Cu–Cu distances also had lower T₁ values because of enhanced cross-relaxation from qubit–qubit dipolar coupling. Frameworks with shorter Cu–Cu distances exhibited lower T_m values because of the increased interactions between qubits within the frameworks. Incorporating molecular electronic spin qubits in ion-paired frameworks enables control of composition, spacing, and interqubit interactions, providing a rational means to extend spin relaxation times.

中文翻译：

基于离子对骨架的铜卟啉量子位晶体阵列

分子电子自旋量子位在量子信息科学应用中具有巨大的潜力，因为它们的结构可以使用合成化学进行合理调整。它们集成到一类新型材料——离子对框架中，可以形成这些分子自旋量子位的有序阵列。三种具有不同密度顺磁性 Cu(II) 卟啉的离子对骨架被分离为微米级晶体，适合通过单晶 X 射线衍射表征。脉冲电子顺磁共振 (EPR) 光谱在高达 140 K 的温度下探测了这些材料的自旋相干性。具有最长 Cu-Cu 距离的晶体具有 207 ns 的自旋-自旋弛豫时间 (T m )和_自旋- 5 K 时晶格弛豫时间 ( T ₁ ) 为 1.8 ms，由于自旋声子耦合，晶格弛豫时间在升高的温度下会降低。由于量子位-量子位偶极耦合的交叉弛豫增强，Cu-Cu 距离较短的晶体也具有较低的T _1值。Cu-Cu 距离较短的框架表现出较低的T _m值，因为框架内量子位之间的相互作用增加。将分子电子自旋量子位纳入离子对框架中，可以控制组成、间距和量子位间相互作用，从而提供延长自旋弛豫时间的合理方法。

更新日期：2023-08-08

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