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The Journal of Chemical Physics

The Aharonov–Anandan phase and geometric double-quantum excitation in strongly coupled nuclear spin pairs

Christian Bengs, Mohamed Sabba, Malcolm H. Levitt

Published Mar 6, 2023• 9 citations

Abstract

The Aharonov-Anandan phase is a contribution to the phase acquired by the cyclic evolution of a quantum state, which depends only on the geometric properties of its trajectory. We report the study and the exploitation of the Aharonov-Anandan phase by nuclear magnetic resonance interferometry techniques in homonuclear spin-1/2 pairs in the near-equivalence limit. We introduce a new method for engineering effective zero-quantum Hamiltonians with an arbitrary phase in the transverse plane. We use this method to generate a variety of cyclic zero-quantum paths, enabling direct study of the geometric Aharonov-Anandan phase to probe the rotational characteristics of the zero-quantum subspace. We show that the geometric Aharonov-Anandan phase may be used for efficient double-quantum excitation in strongly coupled spin pairs. We find that geometric double-quantum excitation outperforms the standard method by a factor of 2 in experiments performed on a typical case involving near-equivalent spin pairs.

DOI: 10.1063/5.0138146

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The Aharonov-Anandan phase is a contribution to the phase acquired by the cyclic evolution of a quantum state, which depends only on the geometric properties of its trajectory. We report the study and the exploitation of the Aharonov-Anandan phase by nuclear magnetic resonance interferometry techniques in homonuclear spin-1/2 pairs in the near-equivalence limit. We introduce a new method for engineering effective zero-quantum Hamiltonians with an arbitrary phase in the transverse plane. We use this method to generate a variety of cyclic zero-quantum paths, enabling direct study of the geometric Aharonov-Anandan phase to probe the rotational characteristics of the zero-quantum subspace. We show that the geometric Aharonov-Anandan phase may be used for efficient double-quantum excitation in strongly coupled spin pairs. We find that geometric double-quantum excitation outperforms the standard method by a factor of 2 in experiments performed on a typical case involving near-equivalent spin pairs.

Quantum states which evolve cyclically in their projective Hilbert space give rise to a geometric (or Aharonov-Anandan) phase. An aspect of primary interest is stable cyclic behaviour as realized under a periodic Hamiltonian. The problem has been handled by use of time-dependent transformations treated along the lines of Floquet's theory as well as in terms of exponential operators with a goal to examine the variety of initial states exhibiting cyclic behaviour. A particular case of special cyclic initial states is described which is shown to be important for nuclear magnetic resonance experiments aimed at the study of the effects of the geometric phase. An example of arbitrary spin j in a precessing magnetic field and spin j=1 subject to both axially symmetric quadrupolar interaction and a precessing magnetic field are presented. The invariant (Kobe's) geometric phase is calculated for special cyclic states.

We introduce a benchtop NMR method for interferometric detection of geometric phase (also known as Berry/Aharonov-Anandan phase) via spin coherence holonomy in bulk ensembles using phase-wound echo trains. Consecutive π pulses with cyclic phase incrementation drive closed spinor trajectories on the Bloch sphere, while a parity-based analysis isolates the geometric contribution and cancels dynamical offsets by comparing positive and negative winding experiments with a zero-winding reference. The extracted phase increases linearly with echo number, reverses sign under winding reversal, and is independent of echo time in the adiabatic regime, consistent with spinor holonomy arising from parallel transport. Experiments performed in strongly inhomogeneous, low-field conditions demonstrate robustness to B₀ gradients and diffusion. This approach establishes a practical foundation for probing geometric phase effects in NMR, with extensions to non-adiabatic transport, heterogeneous systems, and quantum sensing applications.

We show that cyclic quantum evolution can be realized and the Aharonov-Anandan (AA) geometric phase can be determined for any spin-j system driven by periodic fields. Two methods are extended for the study of this problem: the generalized spin-coherent-state technique and the Floquet quasienergy approach. Using the former approach, we have developed a generalized Bloch-sphere model and presented a SU(2) Lie-group formulation of the AA geometric phase in the spin-coherent state. We show that the AA phase is equal to j times the solid angle enclosed by the trajectory traced out by the tip of a generalized Bloch vector. General analytic formulas are obtained for the Bloch vector trajectory and the AA geometric phase in terms of external physical parameters. In addition to these findings, we have also approached the same problem from an alternative but complementary point of view without recourse to the concept of coherent-state terminology. Here we first determine the Floquet quasienergy eigenvalues and eigenvectors for the spin-j system driven by periodic fields. This in turn allows the construction of the time-evolution propagator, the total wave function, and the AA geometric phase in a more general fashion.