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 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.

physics.chem-phCross-listedarXiv:2603.29509Apr 1, 20260 citations

Understanding the spin coherence of molecular photoexcited triplet states from first principles

Ecaterina Păunică, Sam L. Bayliss

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, $D$ , can prolong $T_2$ ; 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 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, $D$, can prolong $T_2$; 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.

quant-pharXiv:2609.16851Sep 16, 2026

Enhancing Spin Coherence of Optically-Addressed Molecular Qubit by Nuclear Spin Hyperpolarization

Boning Li, Patrick Hautle, Duhan Zhang +6 more

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 $60\%$ polarization of the proton spin bath. The measured scaling of the spin-echo decay time ( $T_2$ ) 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.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 $60\%$ polarization of the proton spin bath. The measured scaling of the spin-echo decay time ($T_2$) 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.

physics.chem-phCross-listedarXiv:2603.27872Mar 31, 2026

Robust AC vector sensing at zero magnetic field with pentacene

Boning Li, Garrett Heller, Jungbae Yoon +6 more

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 $1~μ\mathrm{T}/\sqrt{\mathrm{Hz}}$ 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.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 $1~μ\mathrm{T}/\sqrt{\mathrm{Hz}}$ 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.

cond-mat.mes-hallCross-listedarXiv:2512.06272Dec 9, 2025

Singlet fission for quantum information and quantum computing: the parallel JDE model

Kori E. Smyser, Joel David Eaves

Singlet fission is a photoconversion process that generates a doubly excited, maximally spin entangled pair state. This state has applications to quantum information and computing that are only beginning to be realized. In this article, we construct and analyze a spin-exciton hamiltonian to describe the dynamics of the two-triplet state. We find the selection rules that connect the doubly excited, spin-singlet state to the manifold of quintet states and comment on the mechanism and conditions for the transition into formally independent triplets. For adjacent dimers that are oriented and immobilized in an inert host, singlet fission can be strongly state-selective. We make predictions for electron paramagnetic resonance experiments and analyze experimental data from recent literature. Our results give conditions for which magnetic resonance pulses can drive transitions between optically polarized magnetic sublevels of the two-exciton states, making it possible to realize quantum gates at room temperature in these systems.Singlet fission is a photoconversion process that generates a doubly excited, maximally spin entangled pair state. This state has applications to quantum information and computing that are only beginning to be realized. In this article, we construct and analyze a spin-exciton hamiltonian to describe the dynamics of the two-triplet state. We find the selection rules that connect the doubly excited, spin-singlet state to the manifold of quintet states and comment on the mechanism and conditions for the transition into formally independent triplets. For adjacent dimers that are oriented and immobilized in an inert host, singlet fission can be strongly state-selective. We make predictions for electron paramagnetic resonance experiments and analyze experimental data from recent literature. Our results give conditions for which magnetic resonance pulses can drive transitions between optically polarized magnetic sublevels of the two-exciton states, making it possible to realize quantum gates at room temperature in these systems.

arXiv:2004.00103Scientific ReportsOct 28, 202095 citations

Hyperpolarized Molecular Nuclear Spins Achieve Magnetic Amplification

Shengbang Zhou, Qing Li, Yi Ren +6 more

The use of nuclear spins as physical sensing systems is disadvantaged by their low signal responsivity, particularly when compared to sensing techniques based on electron spins. This primarily results from the small nuclear gyromagnetic ratio and the difficulties in achieving high spin polarization. Here we develop a new approach to investigating the response of hyperpolarized molecular nuclear spins to magnetic fields and demonstrate orders-of-magnitude enhanced magnetic responsivity over state-of-the-art proton and Overhauser magnetometers. Using hyperpolarized molecules with proton spins, we report the realization of magnetic amplification in linear and nonlinear types. We further extend this amplification to hyperpolarized scalar-coupled multi-spin molecules and observe substantial magnetic amplification exceeding 10%. Moreover, we observe an anomalous amplification with dispersive frequency dependence that originates from magnetic interference effects. Our work highlights the potential of hyperpolarized molecular nuclear spins for use in a new class of quantum sensors, with promising applications in both applied and fundamental physics, including highly accurate absolute magnetometry and the exploration of axion-nucleon exotic interactions.The use of nuclear spins as physical sensing systems is disadvantaged by their low signal responsivity, particularly when compared to sensing techniques based on electron spins. This primarily results from the small nuclear gyromagnetic ratio and the difficulties in achieving high spin polarization. Here we develop a new approach to investigating the response of hyperpolarized molecular nuclear spins to magnetic fields and demonstrate orders-of-magnitude enhanced magnetic responsivity over state-of-the-art proton and Overhauser magnetometers. Using hyperpolarized molecules with proton spins, we report the realization of magnetic amplification in linear and nonlinear types. We further extend this amplification to hyperpolarized scalar-coupled multi-spin molecules and observe substantial magnetic amplification exceeding 10%. Moreover, we observe an anomalous amplification with dispersive frequency dependence that originates from magnetic interference effects. Our work highlights the potential of hyperpolarized molecular nuclear spins for use in a new class of quantum sensors, with promising applications in both applied and fundamental physics, including highly accurate absolute magnetometry and the exploration of axion-nucleon exotic interactions.

quant-pharXiv:2511.11242Nov 17, 2025

D

, can prolong

T_2

; 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.

60\%

polarization of the proton spin bath. The measured scaling of the spin-echo decay time (

T_2

) 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.

1~μ\mathrm{T}/\sqrt{\mathrm{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.