Quantum probe hyperpolarisation of molecular nuclear spins

Abstract

The hyperpolarisation of nuclear spins within target molecules is a critical and complex challenge in magnetic resonance imaging (MRI) and nuclear magnetic resonance (NMR) spectroscopy. Hyperpolarisation offers enormous gains in signal and spatial resolution which may ultimately lead to the development of molecular MRI and NMR. At present, techniques used to polarise nuclear spins generally require low temperatures and/or high magnetic fields, radio-frequency control fields, or the introduction of catalysts or free-radical mediators. The emergence of room temperature solid-state spin qubits has opened exciting new pathways to circumvent these requirements to achieve direct nuclear spin hyperpolarisation using quantum control. Employing a novel cross-relaxation induced polarisation (CRIP) protocol using a single nitrogen-vacancy (NV) centre in diamond, we demonstrate the first external nuclear spin hyperpolarisation achieved by a quantum probe, in this case of ${}^1$H molecular spins in poly(methyl methacrylate). In doing so, we show that a single qubit is capable of increasing the thermal polarisation of $\sim 10^6$ nuclear spins by six orders of magnitude, equivalent to an applied magnetic field of $10^5$\,T. The technique can also be tuned to multiple spin species, which we demonstrate using both \C{13} and ${}^1$H nuclear spin ensembles. Our results are analysed and interpreted via a detailed theoretical treatment, which is also used to describe how the system can be scaled up to a universal quantum hyperpolarisation platform for the production of macroscopic quantities of contrast agents at high polarisation levels for clinical applications. These results represent a new paradigm for nuclear spin hyperpolarisation for molecular imaging and spectroscopy, and beyond into areas such as materials science and quantum information processing.

6 pages, 4 figures

References in corpus (5)

• High-sensitivity diamond magnetometer with nanoscale resolution
• Nanoscale NMR Spectroscopy and Imaging of Multiple Nuclear Species
• Optical pumping and vibrational cooling of molecules
• Solution nuclear magnetic resonance spectroscopy on a nanostructured diamond chip
• Spin dynamics of diamond nitrogen-vacancy centres at the ground state level anti-crossing and all-optical low frequency magnetic field sensing

Cited by in corpus (35)

• Pulsed polarisation for robust DNP
• Orientation independent room-temperature optical 13C hyperpolarization in powdered diamond
• Two-dimensional nuclear magnetic resonance spectroscopy with a microfluidic diamond quantum sensor
• Hyperpolarization-enhanced NMR spectroscopy with femtomole sensitivity using quantum defects in diamond
• Hyperpolarized solution-state NMR spectroscopy with optically polarized crystals
• Learning models of quantum systems from experiments
• Microwave-assisted cross-polarization of nuclear spin ensembles from optically-pumped nitrogen-vacancy centers in diamond
• Multi-species optically addressable spin defects in a van der Waals material
• Two-level system hyperpolarization using a quantum Szilard engine
• Prospects for nuclear spin hyperpolarisation of molecular samples using nitrogen-vacancy centres in diamond
• 13C dynamic nuclear polarization in diamond via a microwave-free 'integrated' cross effect
• Photoluminescence at the ground state level anticrossing of the nitrogen-vacancy center in diamond
• Longitudinal spin relaxation model applied to point defect qubit systems
• Three-dimensional nuclear spin positioning using coherent radio-frequency control
• Hyperpolarisation of external nuclear spins using nitrogen-vacancy centre ensembles
• Dynamically Polarizing Spin Register of NV Centers in Diamond using Chopped Laser Pulses
• Large Room Temperature Bulk DNP of ${}^{13}$C via P1 Centers in Diamond
• Parallel detection and spatial mapping of large nuclear spin clusters
• Nano-NMR based flow meter
• The non-vanishing effect of detuning errors in dynamical decoupling based quantum sensing experiments
• Two-electron-spin ratchets as a platform for microwave-free dynamic nuclear polarization of arbitrary material targets
• Confined nano-NMR spectroscopy using NV centers
• Cross-relaxation studies with optically detected magnetic resonances in nitrogen-vacancy centers in diamond in an external magnetic field
• Proposal for the search for new spin interactions at the micrometer scale using diamond quantum sensors
• Quantum control and sensing of nuclear spins by electron spins under power limitations
• Angle Locking of a Levitating Diamond using Spin-Diamagnetism
• Quantum bath control with nuclear spin state selectivity via pulse-adjusted dynamical decoupling
• Nitrogen isotope effects on boron vacancy quantum sensors in hexagonal boron nitride
• Solomon equations for qubit and two-level systems: Insights into non-Poissonian quantum jumps
• High precision single qubit tuning via thermo-magnetic field control
• Enhancing polarization transfer from nitrogen-vacancy centers in diamond to external nuclear spins via dangling bond mediators
• On the creation of near-surface nitrogen-vacancy centre ensembles by implantation of type Ib diamond
• Dynamical nuclear polarization for dissipation-induced entanglement in NV centers
• Room-temperature hybrid 2D-3D quantum spin system for enhanced magnetic sensing and many-body dynamics
• Robust external spin hyperpolarization of quadrupolar nuclei enabled by strain