We provide a perspective on how single-molecule magnets can offer a platform to combine quantum transport and paramagnetic spectroscopy, so as to deliver time-resolved electron paramagnetic resonance at the single-molecule level. To this aim, we first review the main principles and recent developments of molecular spintronics, together with the possibilities and limitations offered by current approaches, where interactions between leads and single-molecule magnets are important. We then review progress on the electron quantum coherence on devices based on molecular magnets, and the pulse sequences and techniques necessary for their characterization, which might find implementation at the single-molecule level. Finally, we highlight how some of the concepts can also be implemented by including all elements into a single molecule and we propose an analogy between donor–acceptor triads, where a spin center is sandwiched between a donor and an acceptor, and quantum transport systems. We eventually discuss the possibility of probing spin coherence during or immediately after the passage of an electron transfer, based on examples of transient electron paramagnetic resonance spectroscopy on molecular materials.

中文翻译：

---

将分子自旋电子学与电子顺磁共振相结合：通往单分子脉冲自旋光谱的途径

我们提供了关于单分子磁体如何提供一个结合量子传输和顺磁光谱的平台的观点，以便在单分子水平上提供时间分辨电子顺磁共振。为此，我们首先回顾了分子自旋电子学的主要原理和最新发展，以及当前方法提供的可能性和局限性，其中引线和单分子磁体之间的相互作用很重要。然后，我们回顾了基于分子磁体的设备上电子量子相干性的进展，以及其表征所需的脉冲序列和技术，这些可能会在单分子水平上实现。最后，我们强调了如何通过将所有元素包含到单个分子中来实现某些概念，并且我们提出了供体-受体三元组（自旋中心夹在供体和受体之间）与量子传输系统之间的类比。我们最终基于分子材料上的瞬态电子顺磁共振光谱的例子，讨论了在电子转移过程中或之后立即探测自旋相干性的可能性。