Spin-Phonon Relaxation and Decoherence in a Three-Dimensional Paired-Ion Framework Composed of Vanadyl Porphyrin Qubits

IF 4.5 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2026-10-22 DOI:10.1021/acs.jpclett.6c02513

Christian A. Epure,Georgia C. Mantel,Casandra M. Moisanu,Jonathan R. Palmer,Madison I. Bardot,Michael R. Wasielewski,William R. Dichtel

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Abstract

Molecular electron spin qubits are an emerging platform for quantum technologies due to their atomic-scale synthetic tunability. Supramolecular structures can also place these qubits at precise positions within ordered arrays, allowing the scale-up of qubit architectures through a bottom-up approach. Here, we introduce the first three-dimensional paired-ion framework (PIF), VO-3D-PIF-1, which is composed of a concentrated array of S = 1/2 vanadyl porphyrin spin qubits arranged by ionic lattice interactions. The PIF was characterized using electron paramagnetic resonance spectroscopy to demonstrate the impact of framework structure and spin density on spin–lattice relaxation (T1) and spin decoherence (Tm). The high vanadyl porphyrin spin density within the framework (0.125 spins/nm3) promotes dipolar-driven decoherence, with Tm = 200–400 ns over a temperature range of 140–5 K. Spin–lattice relaxation mirrors that of vanadyl porphyrins in dilute solution, suggesting that the weak ionic interactions assembling the porphyrins within the secondary coordination sphere do not adversely affect phonon-induced T1 relaxation.

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由钒基卟啉量子比特组成的三维对离子框架中的自旋声子弛豫和退相干

分子电子自旋量子比特由于其原子尺度的合成可调性而成为量子技术的新兴平台。超分子结构还可以将这些量子位放置在有序阵列中的精确位置，从而通过自下而上的方法扩大量子位结构的规模。本文介绍了第一个三维对离子框架（PIF）， VO-3D-PIF-1，它由离子晶格相互作用排列的S = 1/2钒基卟啉自旋量子比特组成。利用电子顺磁共振谱对PIF进行了表征，以证明框架结构和自旋密度对自旋晶格弛豫（T1）和自旋退相干（Tm）的影响。在140-5 K温度范围内，钒基卟啉的高自旋密度（0.125个自旋/nm3）促进了偶极驱动的退相干，Tm = 200-400 ns。自旋晶格弛豫反映了稀溶液中钒基卟啉的弛豫，表明在二级配位球内组装卟啉的弱离子相互作用不会对声子诱导的T1弛豫产生不利影响。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

9.60

自引率

7.00%

发文量

1519

审稿时长

1.6 months

期刊介绍： The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.