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Hyperpolarised Naphthalene and Levitated Optomechanics for Fundamental Tests of Physics

Marit Ottilie Eva Steiner

Published Jan 1, 2026• 0 citations
Publisher

Abstract

Levitated nanoparticles, free from the clamping losses and decoherence channels imposed by mechanical support, offer a growing versatile platform for precision sensing and tests of fundamental physics at increasingly larger masses. This thesis follows complementary directions based on this platform: the coupling of optically controllable nuclear spin ensembles to the mechanical and rotational degrees of freedom of levitated solids, and the identification of decoherence mechanisms that limit levitated systems in tests of macroscopic quantum superpositions. In the first part, we study levitated solids doped with non-permanent, optically addressable electron spins, with pentacene-doped naphthalene as a prime exam ple, whose nuclear spins can be hyperpolarised using dynamic nuclear polarisation techniques to over 80% at cryogenic temperatures, with lifetimes extending over weeks. Exploiting the homogeneous spin distribution and absence of a preferred nuclear quantisation axis in such materials, we design a multi-spin Stern-Gerlach interferometry protocol that circumvents key limitations of colour centres in nan odiamonds like NV centres, and use it to place improved bounds on objective collapse models. We further show that the unconstrained rotation available to levitated particles enables magic angle spinning at frequencies beyond current NMRstandards, and propose a protocol for reading out spin ensemble polarisation directly from the particle’s mechanical motion. Building on the same hyperpo larisation mechanism, we propose experiments to observe the nuclear Einstein-de Haas effect, using the hyperpolarised bath of nuclei as a reservoir for angular mo mentum. Furthermore, we propose a protocol to investigate the nuclear Barnett effect in the solid state, using the MHz-scale rotation rates accessible to levitated particles. We find that the proposed Stern-Gerlach interferometer could improve upon existing bounds on collapse-model parameters and that the nuclear Einstein de Haas and Barnett effects could be observable using near-term experimental technology, within parameter ranges already accessible to the community. In the second part, we turn to a central obstacle facing proposals for gravitationally induced entanglement (GIE) between levitated masses, namely the conducting and magnetic shields required to suppress direct electromagnetic coupling. We show that residual Casimir and magnetic-dipole interactions between the particles and the shield, averaged over run-to-run positional and orientational fluctuations of the experimental set-up, generate decoherence, and that the shield can itself mediate spurious entanglement between the particles that might mimic a genuine gravitational-entanglement signature. From this, we derive quantitative stability thresholds considerably stricter than previously assumed.

DOI
10.18725/oparu-61419

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Levitated nanoparticles, free from the clamping losses and decoherence channels imposed by mechanical support, offer a growing versatile platform for precision sensing and tests of fundamental physics at increasingly larger masses. This thesis follows complementary directions based on this platform: the coupling of optically controllable nuclear spin ensembles to the mechanical and rotational degrees of freedom of levitated solids, and the identification of decoherence mechanisms that limit levitated systems in tests of macroscopic quantum superpositions. In the first part, we study levitated solids doped with non-permanent, optically addressable electron spins, with pentacene-doped naphthalene as a prime exam ple, whose nuclear spins can be hyperpolarised using dynamic nuclear polarisation techniques to over 80% at cryogenic temperatures, with lifetimes extending over weeks. Exploiting the homogeneous spin distribution and absence of a preferred nuclear quantisation axis in such materials, we design a multi-spin Stern-Gerlach interferometry protocol that circumvents key limitations of colour centres in nan odiamonds like NV centres, and use it to place improved bounds on objective collapse models. We further show that the unconstrained rotation available to levitated particles enables magic angle spinning at frequencies beyond current NMRstandards, and propose a protocol for reading out spin ensemble polarisation directly from the particle’s mechanical motion. Building on the same hyperpo larisation mechanism, we propose experiments to observe the nuclear Einstein-de Haas effect, using the hyperpolarised bath of nuclei as a reservoir for angular mo mentum. Furthermore, we propose a protocol to investigate the nuclear Barnett effect in the solid state, using the MHz-scale rotation rates accessible to levitated particles. We find that the proposed Stern-Gerlach interferometer could improve upon existing bounds on collapse-model parameters and that the nuclear Einstein de Haas and Barnett effects could be observable using near-term experimental technology, within parameter ranges already accessible to the community. In the second part, we turn to a central obstacle facing proposals for gravitationally induced entanglement (GIE) between levitated masses, namely the conducting and magnetic shields required to suppress direct electromagnetic coupling. We show that residual Casimir and magnetic-dipole interactions between the particles and the shield, averaged over run-to-run positional and orientational fluctuations of the experimental set-up, generate decoherence, and that the shield can itself mediate spurious entanglement between the particles that might mimic a genuine gravitational-entanglement signature. From this, we derive quantitative stability thresholds considerably stricter than previously assumed.
We explore the potential of levitating solids embedded with non-permanent, optically controllable electron spins, which can be used to hyperpolarize their nuclear spin environment with exceptionally long lifetimes. For example, pentacene-doped naphthalene, which will also serve as our prime example, can achieve bulk polarization exceeding 80 % at cryogenic temperatures with polarization lifetimes extending over weeks. These materials make a compelling case for applications such as matter-wave interferometry and novel uses of established NMR techniques. In that spirit, we design a multi-spin Stern-Gerlach-type interferometry protocol which, thanks to the homogeneous spin distribution and the absence of a preferential nuclear-spin quantization axis in such materials, avoids many of the limitations associated with solid state crystals hosting electronic spin defects, such as nanodiamonds containing NV centers. We assess the potential of our interferometer to enhance existing bounds on the free parameters of objective collapse models. Beyond matter-wave interferometry, we analyze the prospects for implementing magic angle spinning at frequencies surpassing the current standard in NMR, capitalizing on the exceptional rotational capabilities offered by levitation. Additionally, we outline a novel protocol for measuring spin ensemble polarization via the position of the nanoparticle and conduct an analysis of dominant noise sources, benchmarking the required isolation levels for various applications.
Levitated macroscopic particles exhibiting quantum mechanical effects are garnering increased attention as a means for precision sensing and testing quantum mechanics. Defects in diamond, such as the nitrogen-vacancy (NV) centre possess optically-addressable spins with long coherence times at room temperature and offer an intriguing system to examine quantum spin dynamics coupled to a macroscopic classical particle. In this work, we convert the outcome of a quantum measurement on an ensemble of spins into a macroscopic rotation of the host particle via spin-mechanical coupling. Following a sequence of green laser and microwave control pulses, spin-mechanical coupling between the final qubit spin state and the host particle -- an electrically-levitated diamond -- exerts a torque on the particle that deflects a weak near-infra-red laser beam. We measure spin readout contrast in excess of 70\%, and demonstrate pulsed mechanical detection of coherent Rabi oscillations, spin-echo interferometry and T1T_1T1​-induced relaxation. We directly measure with temporal resolution the particle reorientation from a 60\,attonewton-metre spin torque induced by flipping the spins. Our results open up interesting new opportunities for levitated spin-mechanical systems using pulsed control, from improved sensing to the prospect of realising macroscopic quantum superposition states.
The probing of the quantum nature of a macroscopic object is an open problem. Approaches in preparing quantum superposition towards a larger scale, which has been progressively accessible in a variety of experimental implementations, may detect new physics or extend the boundary of quantum theory. Development on a nano-mechanical system in the framework of quantum optics and information theory has opened new research directions. It paves ways to manipulate the wavefunction of a massive particle over a large spatial range and probe its quantum behavior to an unprecedented precision. In this thesis, quantum superposition on a mechanical system is studied theoretically in the light of possible implementations under current techniques in order to test superposition principle and the quantum nature of gravity in the mesoscopic region. The work includes two lines of study. In the first line, the motion of the center of mass (c.m.) of the mechanical system is coupled to its internal spin system magnetically, and a Ramsey scheme is developed based on coherent spin control. The wavepacket of the test object, under a spin-dependent force, may then be delocalized to a macroscopic scale. A gravity induced dynamical phase (accrued solely on the spin state, and measured through a Ramsey scheme) is used to reveal the above spatially delocalized superposition of the spin-nano-object composite system that arises during the scheme. A remarkable immunity to the motional noise in the c.m. (initially in a thermal state with moderate cooling) and also a dynamical decoupling nature of the scheme itself is revealed. A careful examination of the perturbation effect due to setup imperfection and environment-induced decoherence is performed, which shows that the Ramsey fringes have a high tolerance on those unwanted faults under realistic experimental conditions. The scheme also facilitates a gravimetry protocol that potentially could be developed for a novel on-chip gravimeter with a precision of 10−6g/Hz10^{-6}g/\sqrt{\text{Hz}}10−6g/Hz​. In the second line, an opto-mechanical experiment is proposed to entangle the motion of two mechanical oscillators through their mutual gravitational interaction. The feasibility of such an experiment is critically examined within the framework of cavity optomechanics. It is shown that within the decoherence time of mechanical noise and potentially gravitational induced state collapse, entanglement between mirrors could be obtained when the initial state of the cavity field is prepared in some particular states. Strategies that give enhancement to entanglement generation rate are studied in light of quantum estimation theory. It is shown that for a cavity initially in a coherent state, the resulting entanglement generation rate would be enhanced linearly with the amplitude of the coherent state. Lastly, it shows that in the proposed setup Casimir effect would significantly affect the gravity-induced entanglement. A proper shield can eliminate the detrimental effect of Casimir force, which, however, will constrain the closest distance between the mirrors in its implementation.
Levitated optomechanical systems are approaching the regime where macroscopic quantum superpositions become experimentally accessible. A central question is whether gravity itself, through its unavoidable coupling to material quantum fluctuations, imposes a fundamental decoherence channel on such superpositions. Starting from two independently well-tested physical elements—the quantum vacuum fluctuations of the material energy-momentum tensor, and the weak-field linear response kernel of classical general relativity—we derive a structurally rigid scaling law for the gravitational decoherence rate: \Gamma \propto G M^2 d^2 / (\hbar L^3) \cdot \Phi(l_*/L). The exponents and dependence on mass M, superposition separation d, and object size L are fixed entirely by dimensional analysis and the semiclassical field equations, without tunable parameters. The overall amplitude is set by a single phenomenological input—the ultraviolet cutoff scale l_* of the effective geometric noise. Identifying l_* with the Planck length yields \Phi \sim \mathcal{O}(1) and a decoherence rate of order 1\,\text{Hz} for nanoparticles with M \sim 10^{-14}\,\text{kg}, d \sim 10^{-7}\,\text{m}, and L \sim 10^{-6}\,\text{m}, placing the prediction within the foreseeable sensitivity window of next-generation levitated optomechanical setups. We provide explicit falsification conditions, a three-path staged verification strategy that does not require simultaneous optimisation of all parameters, and operational signatures—including a distinctive pure-dephasing channel without energy relaxation—that distinguish this mechanism from environmental noise, zero-temperature electromagnetic vacuum fluctuations, and the Diósi-Penrose model.
Abstract Tests of quantum mechanics on a macroscopic scale require extreme control over mechanical motion and its decoherence1–3. Quantum control of mechanical motion has been achieved by engineering the radiation–pressure coupling between a micromechanical oscillator and the electromagnetic field in a resonator4–7. Furthermore, measurement-based feedback control relying on cavity-enhanced detection schemes has been used to cool micromechanical oscillators to their quantum ground states8. In contrast to mechanically tethered systems, optically levitated nanoparticles are particularly promising candidates for matter-wave experiments with massive objects9, 10, since their trapping potential is fully controllable. Here we optically levitate a femtogram (10−15 grams) dielectric particle in cryogenic free space, which suppresses thermal effects sufficiently to make the measurement backaction the dominant decoherence mechanism. With an efficient quantum measurement, we exert quantum control over the dynamics of the particle. We cool its centre-of-mass motion by measurement-based feedback to an average occupancy of 0.65 motional quanta, corresponding to a state purity of 0.43. The absence of an optical resonator and its bandwidth limitations holds promise to transfer the full quantum control available for electromagnetic fields to a mechanical system. Together with the fact that the optical trapping potential is highly controllable, our experimental platform offers a route to investigating quantum mechanics at macroscopic scales11.
We propose NACE-LNGS (Naphthalene Aromatic Collapse Experiment), a dedicated experiment designed to test Penrose’s Objective Reduction (OR) mechanism using diamagnetically levitated pentacene-doped naphthalene nanoparticles. Unlike the original LNGS experiment (Grand Sasso), searching for spontaneous radiation from nuclear-scale collapses in high-purity germanium crystal detectors [1,2], our NACE approach probes mesoscopic superpositions in a protected aromatic π-electron environment that directly mimics the “quantum underground” hypothesized in the Orch-OR theory of consciousness [3,4]. By employing multi-spin Stern-Gerlach matter-wave interferometry on hyperpolarized nuclear-spin ensembles (N ≈ 10^7–10^8 spins per nanoparticle), the experiment achieves unprecedented sensitivity to gravitational self-energy-induced decoherence while operating in the ultra-low-background environment similar to one deployed in LNGS experiment. We highlight the material properties, experimental protocol, noise budget, and sensitivity analysis. In the discussion, we reflect on the 2022 LNGS (Grand Sasso) null results that significantly constrained the simplest Diósi–Penrose (DP) model, the current status of Orch-OR, and why NACE protocol offers potentially the first realistic path to confirming OR as a biologically relevant process confined to shielded aromatic pathways - extrapolating also prebiotic quantum substrates on early Earth.