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arXiv:2502.14103 · Physical review. D/Physical review. D.

Spin squeezing of macroscopic nuclear spin ensembles

Eric Boyers, Garry Goldstein, Alexander O. Sushkov

Published Mar 14, 2025• 8 citations
arXivHTMLPDF

Abstract

Spin squeezing has been explored in atomic systems as a tool for quantum sensing, improving experimental sensitivity beyond the spin standard quantum limit for certain measurements. To optimize absolute metrological sensitivity, it is beneficial to consider macroscopic spin ensembles, such as nuclear spins in solids and liquids. Coupling a macroscopic spin ensemble to a parametrically-modulated resonant circuit can create collective spin squeezing by generating spin correlations mediated by the circuit. We analyze the squeezing dynamics in the presence of decoherence and finite spin polarization, showing that achieving 7 dB spin squeezing is feasible in several nuclear spin systems. The metrological benefit of squeezing a macroscopic spin ensemble lies in the suppression of technical noise sources in the spin detection system relative to the spin projection noise. This expands the experimental sensitivity bandwidth when searching for signals of unknown frequency and can improve the resonant signal-to-noise ratio. Squeezing macroscopic spin ensembles may prove to be a useful technique for fundamental physics experiments aimed at detecting spin interactions with oscillating background fields, such as ultralight dark matter.

DOI
10.1103/physrevd.111.052004

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Spin squeezing has been explored in atomic systems as a tool for quantum sensing, improving experimental sensitivity beyond the spin standard quantum limit for certain measurements. To optimize absolute metrological sensitivity, it is beneficial to consider macroscopic spin ensembles, such as nuclear spins in solids and liquids. Coupling a macroscopic spin ensemble to a parametrically-modulated resonant circuit can create collective spin squeezing by generating spin correlations mediated by the circuit. We analyze the squeezing dynamics in the presence of decoherence and finite spin polarization, showing that achieving 7 dB spin squeezing is feasible in several nuclear spin systems. The metrological benefit of squeezing a macroscopic spin ensemble lies in the suppression of technical noise sources in the spin detection system relative to the spin projection noise. This expands the experimental sensitivity bandwidth when searching for signals of unknown frequency and can improve the resonant signal-to-noise ratio. Squeezing macroscopic spin ensembles may prove to be a useful technique for fundamental physics experiments aimed at detecting spin interactions with oscillating background fields, such as ultralight dark matter.
Quantum control of many body atomic spins is often pursued in the context of an atom-light quantum interface, where a quantized light field acts as a "quantum bus" that can be used to entangle distant atoms. One key challenge is to improve the coherence of the atom-light interface and the amount of atom-light entanglement it can generate, given the constraints of working with multilevel atoms and optical fields in a 3D geometry. We have explored new ways to achieve this, through rigorous optimization of the spatial geometry, and through control of the internal atomic state. Our basic setup consists of a quantized probe beam passing through an atom cloud held in a dipole trap, first generating spin-probe entanglement through the Faraday interaction, and then using backaction from a measurement of the probe polarization to squeeze the collective atomic spin. The relevant figure of merit is the metrologically useful spin squeezing determined by the enhancement in the resolution of rotations of the collective spin, relative to the commonly used spin coherent state. With an optimized free-space geometry, and by using a 2-color probe scheme to suppress tensor light shifts, we achieve 3(2) dB of metrologically useful spin squeezing. We can further increase atom-light coupling by implementing internal state control to prepare spin states with larger initial projection noise relative to the spin coherent state. Under the right conditions this increase in projection noise can lead to stronger measurement backaction and increased atom-atom entanglement. With further internal state control the increased atom-atom entanglement can then be mapped to a basis where it corresponds to improved squeezing of, e.g., the physical spin-angular momentum or the collective atomic clock pseudospin. In practice, controlling the collective spin of N ~ 10⁶ atoms in this fashion is an extraordinarily difficult challenge because errors in the control of individual atoms tend to be highly correlated. By employing precise internal state control, we have prepared and detected projection noise limited "cat" states (which have initial projection noise that is larger by a factor of 2f = 8 for Cs relative to the spin coherent state) and estimate that we can generate up to 6.0(5) dB of metrologically useful spin squeezing, demonstrating the advantage of using the internal atomic structure as a resource for ensemble control.
We recently showed that macroscopic nuclear spin ensembles prepared in coherent spin states can dramatically enhance the interaction rates of weakly interacting cosmic relics-such as dark matter and the cosmic neutrino background-through collective quantum effects analogous to Dicke superradiance, where the de-excitation and excitation rates scale as the square of the number of spins, N2N^2N2. We thus coined these processes superradiant interactions. In this paper, we propose a protocol to realize this enhancement and boost the discovery potential for such relics. We show how concepts from quantum optics can be adapted to nuclear spins coupled to superconducting circuits, enabling high-sensitivity systems. The spins are first initialized into a coherent spin state via a π/2π/2π/2 Rabi pulse from the ground state. When the circuit is sufficiently detuned from resonance, the spin-circuit interaction implements a squeezing Hamiltonian. Because squeezing must outpace spin relaxation and dephasing, the protocol favors macroscopic ensembles and high-quality superconducting circuits. During this squeezing phase, the standard quantum variance is reduced by up to 4.8 orders of magnitude-equivalent to 48 dB of squeezing-for circuits with quality factors Q∼108Q \sim 10^8Q∼108-10910^9109. The signal imprinted on the spins during the squeezing protocol can be magnified by further utilizing the squeezing interactions, easing the requirement for shot-noise-limited readout. This protocol has the potential to significantly accelerate axion and dark photon dark matter searches and extend the reach of existing axion experiments to probe QCD axion-nuclear spin couplings. More broadly, it paves the way for detecting coherent inelastic interactions from other cosmic relics-most notably the cosmic neutrino background-and establishes nuclear-spin-based systems as a new class of quantum, ultra-low-threshold detectors.
Direct detection of dark matter remains an important outstanding problem since abundant astrophysical evidence points towards its existence, but no experiment has succeeded in detecting it. Axions and axion-like-particles are some of the most compelling candidates for dark matter given their appearance in many theories of physics beyond the Standard Model and their relatively unexplored parameter space compared to other candidates. Recently, the Cosmic Axion Spin Precession Experiment-Electric (CASPEr-e) has used nuclear magnetic resonance (NMR) to search for effective magnetic fields created by axionic dark matter. By decreasing technical noise sources, CASPEr-e is projected to reach the standard quantum limit where spin projection noise is the dominant noise source limiting sensitivity. However, some axion models predict axion couplings to normal matter that would be too small for even a quantum limited CASPEr-e experiment to detect. This creates a need for surpassing the spin projection noise limit in NMR dark matter searches. In this thesis, I explore the prospects for surpassing the quantum limit in NMR by using spin squeezed states, entangled states with variance in one projection reduced below the standard quantum limit. First, I propose an experimental scheme for generating squeezed states by coupling the spins to an off-resonant circuit to create a One-Axis-Twist Hamiltonian. Then, using exact results and numerical simulations, I determine the amount of squeezing that can be achieved given decoherence and noise. Next, I perform modeling to show that squeezing can accelerate dark matter searches despite earlier results that argued squeezing cannot improve experimental sensitivity when subject to decoherence. Finally, I apply these results to the CASPEr-e experiment and show that at axion frequencies near 100MHz, squeezing can speed up the experiment by a factor of up to 30, corresponding to a sensitivity improvement by a factor of over 5.
Squeezing of collective atomic spins has been shown to improve the sensitivity of atomic clocks and magnetometers to levels significantly below the standard quantum limit. In most cases the requisite atom-atom entanglement has been generated by dispersive interaction with a quantized probe field or by state-dependent collisions in a quantum gas. Such experiments typically use complex multilevel atoms like Rb or Cs, with the relevant interactions designed so that atoms behave like pseudospin-12\frac{1}{2}21​ particles. We demonstrate the viability of spin squeezing for collective spins composed of the physical angular momenta of 106{10}^{6}106 Cs atoms, each in an internal spin-4 hyperfine state. A peak metrological squeezing of at least 5dB is generated by quantum backaction from a dispersive quantum nondemolition (QND) measurement, implemented using a two-color optical probe that minimizes tensor light shifts without sacrificing measurement strength. Other significant developments include the successful application of composite pulse techniques for accurate dynamical control of the collective spin, enabled by broadband suppression of background magnetic fields inside a state-of-the-art magnetic shield. The absence of classical noise allows us to compare the observed quantum projection noise and squeezing to a theoretical model that properly accounts for both the relevant atomic physics and the spatial mode of the collective spin, finding good quantitative agreement and thereby validating its use in other contexts. Our work sets the stage for experiments on quantum feedback, deterministic squeezing, and closed-loop magnetometry. The implementation of real-time feedback may also create an opportunity for new types of quantum simulation, wherein the evolution of a quantum system is conditioned on the outcome of a time-continuous QND measurement. Such a scheme has the potential to access new regimes near the quantum-classical boundary, with opportunities to study long-standing issues related to quantum-classical correspondence in chaotic systems.
Spin-squeezed state is a many-body entangled state of great interest for precision measurements. Although the absolute sensitivity at the standard quantum limit is better for a larger atom number, the greater dominance of classical noises over atom projection noise makes it harder to achieve spin squeezing. Here, we show both theoretically and experimentally that adiabatic pulse control of the pump field in state preparation is indispensable to sufficient noise suppression, which is the prerequisite for spin squeezing. This technique is generally applicable to spin-squeezing experiments involving a large ensemble and is thus of significance for quantum metrology applications.
Spin squeezing of 101110^{11}1011 atoms
Atomic ensemble with large number of quantum correlated particles is a desirable resource for precision measurement and quantum simulation. Being a type of quantum correlated state particularly useful for quantum metrology, spin squeezed state (SSS) has been pursued in both cold atom and vapor cell systems, and the largest ensemble so far contains 10810^{8}108 atoms. We report experimental preparation of a SSS in a paraffin-coated macroscopic vapor cell in free space, containing 101110^{11}1011 87Rb^{87}\text{Rb}87Rb atoms, by means of stroboscopic quantum non-demolition measurement. We observed 2.38±0.23 dB2.38\pm0.23~\text{dB}2.38±0.23 dB noise reduction, and 1.31±0.23 dB1.31\pm0.23~\text{dB}1.31±0.23 dB spin squeezing \emph{below coherent spin state} by the Wineland criterion. Our result present the highest angular resolution on the Bloch sphere in all SSS up to date, and will open possibilities to implement quantum control, metrology and quantum simulations using such large entangled atomic ensembles. The universal off-resonance interaction utilized here can also be straightforwardly expanded to other systems, such as trapped ions and mechanical oscillators, in the application of entanglement generation and open-system quantum simulations.