Abstract Spins are prototypical systems with the potential to probe magnetic fields down to the atomic scale limit. Exploiting their quantum nature through appropriate sensing protocols allows to enlarge their applicability to fields not always accessible by classical sensors. Here we first show that quantum sensing protocols for AC magnetic fields can be implemented with molecular spin ensembles embedded into hybrid quantum circuits. We then show that, using only echo detection at microwave frequency and no optical readout, Dynamical Decoupling protocols synchronized with the AC magnetic fields can enhance sensitivity up to S ≈ 10−10 − 10−9 T Hz−1/2 with a low (4-5) number of applied pulses. These results paves the way for the development of strategies to exploit molecular spins as quantum sensors.
Abstract Spins are prototypical systems with the potential to probe magnetic fields down to the atomic scale limit. Exploiting their quantum nature through appropriate sensing protocols allows to enlarge their applicability to fields not always accessible by classical sensors. Here we first show that quantum sensing protocols for AC magnetic fields can be implemented with molecular spin ensembles embedded into hybrid quantum circuits. We then show that, using only echo detection at microwave frequency and no optical readout, Dynamical Decoupling protocols synchronized with the AC magnetic fields can enhance sensitivity up to S ≈ 10−10 − 10−9 T Hz−1/2 with a low (4-5) number of applied pulses. These results paves the way for the development of strategies to exploit molecular spins as quantum sensors.
Quantum sensors based on individual spins provide unprecedented access to local magnetic fields in condensed matter, chemistry, and biology, with solid-state defect spins emerging as the leading platform. However, their molecular-sensing capabilities are limited by confinement to a host lattice, which prevents placement in close proximity to a target molecule. Molecular spins offer an alternative, enabling chemical tunability and flexible positioning relative to the target system. Here we present a nanoscale sensing platform that combines molecular electron spins, ultrasensitive mechanical readout, and Hamiltonian engineering. Using a modified XYXY dipolar decoupling sequence, we suppress electron-electron dipolar interactions across a broad distribution of control fields, extending coherence times to ∼400μs in an attoliter-scale droplet containing $\sim$100 trityl-OX063 radicals. Leveraging this sequence, we demonstrate frequency-selective detection of nanotesla-scale AC fields and perform sensing and spectroscopy of small, local nuclear-spin ensembles. Collectively, these results establish SQUINT (Spin-based QUantum Integrated Nanomechanical Transduction) as a framework for quantum sensing that affords molecular-level control over sensor properties and enables direct integration into complex molecular targets.
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.
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.
We demonstrate quantum logic enhanced sensitivity for a macroscopic ensemble of solid-state, hybrid two-qubit sensors. We achieve over a factor of 30 improvement in the single-shot signal-to-noise ratio, translating to an ac magnetic field sensitivity enhancement exceeding an order of magnitude for time-averaged measurements. Using the electronic spins of nitrogen vacancy (NV) centers in diamond as sensors, we leverage the on-site nitrogen nuclear spins of the NV centers as memory qubits, in combination with homogeneous and stable bias and control fields, ensuring that all of the ∼10^{9} two-qubit sensors are sufficiently identical to permit global control of the NV ensemble spin states. We find quantum logic sensitivity enhancement for multiple measurement protocols with varying optimal sensing intervals, including XY8 and DROID-60 dynamical decoupling, as well as correlation spectroscopy, using an applied ac magnetic field signal. The results are independent of the nature of the target signal and broadly applicable to measurements using NV centers and other solid-state spin ensembles. This work provides a benchmark for macroscopic ensembles of quantum sensors that employ quantum logic or quantum error correction algorithms for enhanced sensitivity.
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 1μT/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.
Magnetic sensors are typically much more sensitive to oscillating (AC) magnetic fields than static (DC) fields, due to the presence of more noise at lower frequency, typically scaling with a 1/f dependence. For quantum magnetometers, this characteristic noise is reflected in the ensemble dephasing time T2∗, the relevant sensing time for a DC field, being much lower than the spin coherence time T2, which determines the sensitivity to AC fields. Here, we demonstrate measurement of DC magnetic fields using a physically rotating ensemble of nitrogen-vacancy centres at a precision limited by the electron spin coherence time, T2. We rotate the host diamond with a period comparable to T2, such that the angle between the NV axis and the magnetic field to be detected changes as a function of time, upconverting the static magnetic field to an oscillating field in the physically rotating frame. Using spin-echo interferometry, we observe an order of magnitude improvement in DC magnetometer response compared to a conventional Ramsey experiments. Enhancements to our scheme could realise DC sensitivities equivalent to demonstrated AC magnetic field sensitivities with NV centres.