Host-guest Crystal Engineering Tailors the Room Temperature Spin Dynamics in Molecular Quantum Devices

• URL: http://arxiv.org/abs/2607.16466v1
• Date: Fri, 17 Jul 2026 19:26:23 GMT
• Title: Host-guest Crystal Engineering Tailors the Room Temperature Spin Dynamics in Molecular Quantum Devices
• Abstract summary: Molecular materials that enable coherent control over an electron's spin state at room temperature are promising candidates for quantum technologies.<n>Host-guest molecular crystals enable independent control of spin-active guests and their local environments.<n>We demonstrate the ability to tune triplet population, depopulation, and spin-lattice relaxation by modulating host-dependent lattice rigidity and vibrational coupling.
• Score: 0.7066716686670619
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Molecular materials that enable coherent control over an electron's spin state at room temperature are promising candidates for quantum technologies, including quantum sensors and ultra-low noise microwave amplifiers, known as masers. Host-guest molecular crystals enable independent control of spin-active guests and their local environments to enhance molecular spin properties and so improve device performance. Using electron paramagnetic resonance and optically-detected magnetic resonance, we demonstrate the ability to tune triplet population, depopulation, and spin-lattice relaxation by modulating host-dependent lattice rigidity and vibrational coupling to significantly reduce the operating requirements for building useful masers. Importantly, the most rigid host, picene, reveals the ability to slow spin-lattice relaxation without lengthening triplet lifetime, though at the cost of strain-induced line width broadening and reduced triplet spin polarisation. We also find that deuteration reduces the triplet resonance line width and vibrationally-mediated triplet depopulation. Consequently, we find that perdeuterated pentacene in perdeuterated p-terphenyl is the most viable candidate for building a continuous wave maser. This work demonstrates host-guest engineering as an important and practical method for tuning the spin-dependent performance of room-temperature molecular quantum technologies.

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