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arXiv:2603.29509

Quantum Sensing with Triplet Pair States: A Theoretical Study

Maria Grazia Concilio, Yiwen Wang, Siyuan Wang, Xueqian Kong

physics.chem-phquant-phSubmitted Mar 31, 2026• Announced Apr 1, 2026• 0 citations
v1 · Mar 31, 2026v2 · Apr 1, 2026v3 · May 15, 2026
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Abstract

Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet states of molecular pentacene provide a viable sensing architecture, the triplet pair states produced by singlet fission of pentacene dimers could enable more flexible quantum manipulations through entanglement. In this work, we model the quantum sensing efficacy of a spin-polarized quintet manifold in a photoexcited pentacene dimer generated via intramolecular singlet fission. Using a Lindblad master equation approach, we simulate the evolution of the triplet pair state under standard dynamical decoupling sequences, including spin echo, XY4, and XY8 and provide a direct performance comparison to the traditional pentacene monomer benchmark. While both architectures exhibit comparable sensitivity for isolated single-spin detection, our findings indicate that the dimer architecture provides a superior interaction cross-section for detecting small ensembles of nuclear spins. Analytical expressions derived for fluorescence modulation demonstrate that sensitivity is optimized in the low-magnetic field regime and scales with the number of pulses in the sensing protocol. This study establishes a theoretical baseline for utilizing high-spin multi-excitonic states as chemically tunable, high-sensitivity quantum probes.

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Quantum sensing with triplet pair states: A theoretical study

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Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet states T̂ of molecular pentacene provide a viable sensing architecture, the triplet pair states T̂T̂ produced by singlet fission of pentacene dimers could enable more flexible quantum manipulations through entanglement. In this work, we model the quantum sensing efficacy of a spin-polarized quintet manifold 5T̂T̂0,±1 in a photoexcited pentacene dimer generated via intramolecular singlet fission. Using a Lindblad master equation approach, we simulate the evolution of the triplet-pair state under standard dynamical decoupling sequences-including spin echo, XY4, and XY8-and provide a direct performance comparison to the traditional pentacene monomer benchmark. While both architectures exhibit comparable sensitivity for isolated single-spin detection, our findings indicate that the dimer architecture provides a superior interaction cross section for detecting small ensembles of nuclear spins. Analytical expressions derived for fluorescence modulation demonstrate that sensitivity is optimized in the low-magnetic field regime (≤0.01 T) and scales with the number of pulses in the sensing protocol. This study establishes a theoretical baseline for utilizing high-spin multi-excitonic states as chemically tunable, high-sensitivity quantum probes.

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Quantum sensing based on strongly interacting nuclear spin systems

Qing Li, Yunlan Ji, Ran LIU +3 more

Quantum sensing utilizes the quantum resources of well-controlled quantum systems to measure small signals with high sensitivity, and has great potential in both fundamental science and concrete applications. Interacting quantum systems have attracted increasing interest in the field of precise measurements, owing to their potential to generate quantum-correlated states and exhibit rich many-body dynamics. These features provide a novel avenue for exploiting quantum resources in sensing applications. Although previous studies have shown that using such systems can improve sensitivity, they mainly focused on measuring individual physical quantities. In experiment, the challenge of using interacting quantum systems to achieve high-precision measurements of multiple physical parameters simultaneously has not been explored to a large extent. In this study, we demonstrate a first realisation of interaction-based multiparameter sensing by using strongly interacting nuclear spins under ultra-low magnetic field conditions. We find that, as the interaction strength among nuclear spins becomes significantly larger than their Larmor frequencies, a different regime emerges where the strongly interacting spins can be simultaneously sensitive to all components of a multidimensional field, such as a three-dimensional magnetic field. Moreover, we observe that the strong interactions between nuclear spins can increase their quantum coherence times to as long as several seconds, thereby improving measurement precision. Our sensor successfully achieves precision measurement of three-dimensional vector magnetic fields with a field sensitivity reaching the order of 10–11 T and an angular resolution as high as 0.2 rad. Importantly, this approach eliminates the need for external reference fields, thereby avoiding calibration errors and technical noise commonly encountered in traditional magnetometry. Experimentally optimized protocol further enhances the sensitivity of the interacting spin-based sensor by up to five orders of magnitude compared with non-interacting or classical schemes. These results demonstrate the enormous potential of interacting spin systems as a powerful platform for high-precision multi-parameter quantum sensing. The techniques developed here pave the way for a new generation of quantum sensors that use intrinsic spin interactions to exceed the traditional sensitivity limits, presenting a promising route toward ultra-sensitive, calibration-free magnetometry in complex environments.

Acta Physica Sinica•Jan 1, 2025•1 citation
Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet states of molecular pentacene provide a viable sensing architecture, the triplet pair states produced by singlet fission of pentacene dimers could enable more flexible quantum manipulations through entanglement. In this work, we model the quantum sensing efficacy of a spin-polarized quintet manifold in a photoexcited pentacene dimer generated via intramolecular singlet fission. Using a Lindblad master equation approach, we simulate the evolution of the triplet pair state under standard dynamical decoupling sequences, including spin echo, XY4, and XY8 and provide a direct performance comparison to the traditional pentacene monomer benchmark. While both architectures exhibit comparable sensitivity for isolated single-spin detection, our findings indicate that the dimer architecture provides a superior interaction cross-section for detecting small ensembles of nuclear spins. Analytical expressions derived for fluorescence modulation demonstrate that sensitivity is optimized in the low-magnetic field regime and scales with the number of pulses in the sensing protocol. This study establishes a theoretical baseline for utilizing high-spin multi-excitonic states as chemically tunable, high-sensitivity quantum probes.
Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet states T̂ of molecular pentacene provide a viable sensing architecture, the triplet pair states T̂T̂ produced by singlet fission of pentacene dimers could enable more flexible quantum manipulations through entanglement. In this work, we model the quantum sensing efficacy of a spin-polarized quintet manifold 5T̂T̂0,±1 in a photoexcited pentacene dimer generated via intramolecular singlet fission. Using a Lindblad master equation approach, we simulate the evolution of the triplet-pair state under standard dynamical decoupling sequences-including spin echo, XY4, and XY8-and provide a direct performance comparison to the traditional pentacene monomer benchmark. While both architectures exhibit comparable sensitivity for isolated single-spin detection, our findings indicate that the dimer architecture provides a superior interaction cross section for detecting small ensembles of nuclear spins. Analytical expressions derived for fluorescence modulation demonstrate that sensitivity is optimized in the low-magnetic field regime (≤0.01 T) and scales with the number of pulses in the sensing protocol. This study establishes a theoretical baseline for utilizing high-spin multi-excitonic states as chemically tunable, high-sensitivity quantum probes.
Optically readable molecular spins are attractive as quantum sensors due to their nanoscale modularity, synthetic tunability, and scope for sensitive readout. In particular, photoexcited spin-triplet states in organic molecules are appealing in supporting high optical-spin contrast at room temperature. Their utility is underpinned by their coherence, which warrants a detailed understanding of it. Here, from first principles, we systematically explore the Hahn-echo decoherence of the benchmark molecular system for room-temperature optically detected spin coherence---pentacene guest molecules coupled to a para-terphenyl host. Using generalized cluster-correlation expansion methods, we investigate the mechanisms of nuclear-spin-induced decoherence from zero to high magnetic field, exploring the role of guest vs host molecules, specific nuclei, zero-field splitting interactions, and hyperfine parameters. We describe how zero-field decoherence is driven by ~6 nuclei on the guest, while high-field decoherence is driven by ~600 nuclei in the host; how the longitudinal zero-field splitting parameter, DDD, can prolong T2T_2T2​; and the magnetic-field-dependent processes which drive decoherence. These results advance our understanding of decoherence in optically readable molecular spins, providing insight for their synthetic enhancement and deployment as quantum probes.
Optically addressable molecular triplet spins provide a chemically tunable platform for quantum application, but their coherence is often limited by interactions with surrounding spin baths. Here we demonstrate controlled suppression of nuclear-bath-induced decoherence in photoexcited triplet spins of pentacene co-crystallized in high-purity naphthalene single crystals. By hyperpolarizing the proton spin bath through triplet dynamic nuclear polarization (triplet-DNP), magnetic noise generated by the nuclear spins is suppressed, leading to an extension of the electron spin transverse coherence time. Experimentally, we observe a 25\% enhancement of the spin-echo decay time with 60%60\%60% polarization of the proton spin bath. The measured scaling of the spin-echo decay time (T2T_2T2​) with nuclear polarization quantitatively follows the predicted dependence derived from the polarization-controlled nuclear second moment. Both the enhancement and the absolute value of the coherence time are quantitatively reproduced by cluster correlation expansion (CCE) simulations. These results establish nuclear spin hyperpolarization as a general and actively tunable approach to engineering coherence in molecular qubits. This work provides a broadly applicable design framework for high-coherence molecular and solid-state spin systems.
Quantum sensors based on electronic spins have emerged as powerful probes of microwave-frequency fields. Among other solid-state platforms, spins in molecular crystals offer a range of advantages, from high spin density to functionalization via chemical tunability. Here, we demonstrate microwave vector magnetometry using the photoexcited spin triplet of deuterated pentacene molecules, operating at zero external magnetic field and room temperature. We achieve full three-dimensional microwave field reconstruction by detecting the Rabi frequencies of anisotropic spin-triplet transitions associated with two crystallographic orientations of pentacene in naphthalene crystals. We further introduce a phase alternated protocol that extends the rotating-frame coherence time by an order of magnitude and enables sensitivities of 1 μT/Hz1~μ\mathrm{T}/\sqrt{\mathrm{Hz}}1 μT/Hz​ with sub-micrometer spatial resolution. These results establish pentacene-based molecular spins as a practical and high-performance platform for microwave quantum sensing, and the control techniques are broadly applicable to other molecular and solid-state spin systems.
Fluorescent spin qubits are central building blocks of quantum technologies. Placing these qubits at surfaces maximizes coupling to nearby spins and fields, enabling nanoscale sensing and facilitating integration with photonic and superconducting devices. However, reducing the dimensions or size of established qubit systems without sacrificing the qubit performance or degrading the coherence lifetime remains challenging. Here, we introduce a surface molecular qubit formed by pentacene molecules scaffolded on a two-dimensional (2D) material, hexagonal boron nitride (hBN). The qubit exhibits stable fluorescence and optically detected magnetic resonance (ODMR) from cryogenic to ambient conditions. With fully deuterated pentacene, the Hahn-echo coherence reaches 22 μμμs and further extends to 214 μμμs under dynamical decoupling, outperforming state-of-the-art shallow NV centers in diamond, despite being positioned directly on the surface. We map the local spin environment, resolving couplings to nearby nuclear and electron spins that can serve as auxiliary quantum resources. This platform combines true surface integration, long qubit coherence, and scalable fabrication, opening routes to quantum sensing, quantum simulation, and hybrid quantum devices. It also paves the way for a broader family of 2D material-supported molecular qubits.
Quantum sensing utilizes the quantum resources of well-controlled quantum systems to measure small signals with high sensitivity, and has great potential in both fundamental science and concrete applications. Interacting quantum systems have attracted increasing interest in the field of precise measurements, owing to their potential to generate quantum-correlated states and exhibit rich many-body dynamics. These features provide a novel avenue for exploiting quantum resources in sensing applications. Although previous studies have shown that using such systems can improve sensitivity, they mainly focused on measuring individual physical quantities. In experiment, the challenge of using interacting quantum systems to achieve high-precision measurements of multiple physical parameters simultaneously has not been explored to a large extent. In this study, we demonstrate a first realisation of interaction-based multiparameter sensing by using strongly interacting nuclear spins under ultra-low magnetic field conditions. We find that, as the interaction strength among nuclear spins becomes significantly larger than their Larmor frequencies, a different regime emerges where the strongly interacting spins can be simultaneously sensitive to all components of a multidimensional field, such as a three-dimensional magnetic field. Moreover, we observe that the strong interactions between nuclear spins can increase their quantum coherence times to as long as several seconds, thereby improving measurement precision. Our sensor successfully achieves precision measurement of three-dimensional vector magnetic fields with a field sensitivity reaching the order of 10–11 T and an angular resolution as high as 0.2 rad. Importantly, this approach eliminates the need for external reference fields, thereby avoiding calibration errors and technical noise commonly encountered in traditional magnetometry. Experimentally optimized protocol further enhances the sensitivity of the interacting spin-based sensor by up to five orders of magnitude compared with non-interacting or classical schemes. These results demonstrate the enormous potential of interacting spin systems as a powerful platform for high-precision multi-parameter quantum sensing. The techniques developed here pave the way for a new generation of quantum sensors that use intrinsic spin interactions to exceed the traditional sensitivity limits, presenting a promising route toward ultra-sensitive, calibration-free magnetometry in complex environments.