A Single-Molecule Spin-Photon Interface

• URL: http://arxiv.org/abs/2605.10077v1
• Date: Mon, 11 May 2026 06:59:26 GMT
• Title: A Single-Molecule Spin-Photon Interface
• Abstract summary: Optical interfaces that connect long-lived spin qubits to photons are a central requirement for quantum networking and distributed quantum information processing.<n>Here we show that a triplet ground state carbene molecule, embedded within a structurally matched host crystal, functions as a robust spin-photon interface with single-molecule addressability.<n>Results establish molecular qubits as a viable platform for single-emitter quantum optics while preserving the advantages of bottom-up chemical design and processable materials.
• Score: 0.2319165683825004
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Optical interfaces that connect long-lived spin qubits to photons are a central requirement for quantum networking and distributed quantum information processing. Currently, solid-state atomic defects are leading candidates due to their inherent spin and optical coherence. Building on these advancements, synthetically tailored molecular systems represent a fundamental change in the field, utilizing precise atomic control and consistent bottom-up assembly. However, the lack of a robust spin-photon interface combining bright fluorescence, high spectral stability, and the persistent spin lifetimes inherent to ground-state systems has prohibited the detection of individual molecular qubits. Here we show that a triplet ground state carbene molecule, embedded within a structurally matched host crystal, functions as a robust spin-photon interface with single-molecule addressability. The system exhibits narrow zero-phonon lines, spectral stability over more than an hour, spin-selective optical transitions and single-molecule optically detected magnetic resonance. Coherent control yields millisecond-scale dynamical-decoupling coherence and tens-of-milliseconds spin relaxation at a temperature of 4.5 K. These results establish molecular qubits as a viable platform for single-emitter quantum optics while preserving the advantages of bottom-up chemical design and processable materials.

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