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arXiv:2407.01075

Spin Resonance in Perspective of Floquet Theory and Brillouin-Wigner Perturbation Method

Mingjun Feng, Guobin Liu

Published Jul 1, 2024• 0 citations
arXivHTMLPDF

Abstract

We studied the two-level spin resonance in a new perspective. Using the Floquet theory, the periodic interaction Hamiltonians were transfromed into a time-independent interaction. Using the Brillouin-Wigner perturbation method, a degenerated subspace is constructed, where the effective Hamiltonian is given in a perturbation expansion. In this framework, we found that the upper triangular element $\langle α| H^1 | β\rangle$, determines whether the resonance happens. The generalized Rabi frequency and the Bloch-Siegert shift were solved straightforwardly as the first order and the second order solution, proving the benefit of the developed method.

DOI
10.48550/arxiv.2407.01075

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We studied the two-level spin resonance in a new perspective. Using the Floquet theory, the periodic interaction Hamiltonians were transfromed into a time-independent interaction. Using the Brillouin-Wigner perturbation method, a degenerated subspace is constructed, where the effective Hamiltonian is given in a perturbation expansion. In this framework, we found that the upper triangular element ⟨α∣H1∣β⟩\langle α| H^1 | β\rangle⟨α∣H1∣β⟩, determines whether the resonance happens. The generalized Rabi frequency and the Bloch-Siegert shift were solved straightforwardly as the first order and the second order solution, proving the benefit of the developed method.
An accurate theoretical treatment of periodically driven quantum systems is crucial for various fields in the exact sciences, for instance Nuclear Magnetic Resonance (NMR) spectroscopy. Conventionally, either average Hamiltonian theory or Floquet theory is used to predict or describe experimental outcomes, such as the time evolution or the spectra yielding the information of the sample under study. A detailed analysis of the equivalence of these two approaches with an emphasis on applications in NMR will help to improve the theoretical understanding of NMR experiments. In this work, we identify the Floquet-Magnus expansion as essential to prove the mathematical equivalence of Floquet theory and average Hamiltonian theory. We advocate a calculation scheme which is less prone to algebraic mistakes because explicit integration is avoided. On this basis, we provide the first four orders of both theories. We further examine their applicability to some experiments in NMR. As examples, we investigate the Bloch-Siegert shift and dipolar coupled spin systems under magic-angle spinning. Based on our analysis, we recommend the use of the Floquet-Van Vleck approach including both the effective Hamiltonian and the kick operator. The consistent separation of secular and non-secular contributions appears to be especially advantageous for numerical robustness. Its accuracy is about three times better than the one provided by average Hamiltonian theory despite their formal equivalence. Our findings provide important insights into the theoretical background of Floquet theory and average Hamiltonian theory. This includes the extent of their algebraic and perturbative equivalence, with an emphasis on how these findings are of relevance in the analysis of solid-state NMR experiments.
The Bloch-Siegert-type shifts and multiple-quantum resonance shifts of a spin-one system subjected to an oscillating radio-frequency applied at right angles to a DC field have been calculated to sixth order in V, the amplitude of the oscillating field, for the single-quantum resonance, and to fourth order in V for the higher resonances. The level crossing criterion appropriate to two-level systems cannot be used here, and a resonance condition based on a previously derived analogue of Shirley's equation for spin-one systems is used instead. The calculation uses degenerate continued-fraction perturbation theory. Numerical calculations were performed in order to obtain the shape of the resonances, and partially check the analytic results. The atomic levels were assumed to be completely stable; the corrections due to finite atomic lifetimes are expected to be small.
The Floquet-Magnus expansion is a widely used tool to derive effective descriptions of time-periodic quantum systems by approximating their dynamics with a time-independent Hamiltonian. However, its standard formulation is, strictly speaking, restricted to bounded Hamiltonians. In this work, we extend its definition and analysis to a broad class of time-periodic unbounded Hamiltonians. Our approach is based on an a priori distinct nonperturbative framework for the construction of effective Hamiltonians, which we show to reproduce the Floquet-Magnus expansion. A particular strength of our framework is that it allows us to prove that the resulting effective dynamics approximates the original time evolution propagators to arbitrary order in the high-frequency limit without requiring convergence of the Floquet-Magnus expansion, a condition that is already highly restrictive even in the bounded setting. We illustrate the scope of the method on representative models: the quantum Rabi Hamiltonian in the interaction picture, and the periodically driven quantum harmonic oscillator.
We construct a systematic high-frequency expansion for periodically driven quantum systems based on the Brillouin-Wigner (BW) perturbation theory, which generates an effective Hamiltonian on the projected zero-photon subspace in the Floquet theory, reproducing the quasienergies and eigenstates of the original Floquet Hamiltonian up to desired order in $1/\ensuremath{\omega}$, with $\ensuremath{\omega}$ being the frequency of the drive. The advantage of the BW method is that it is not only efficient in deriving higher-order terms, but even enables us to write down the whole infinite series expansion, as compared to the van Vleck degenerate perturbation theory. The expansion is also free from a spurious dependence on the driving phase, which has been an obstacle in the Floquet-Magnus expansion. We apply the BW expansion to various models of noninteracting electrons driven by circularly polarized light. As the amplitude of the light is increased, the system undergoes a series of Floquet topological-to-topological phase transitions, whose phase boundary in the high-frequency regime is well explained by the BW expansion. As the frequency is lowered, the high-frequency expansion breaks down at some point due to band touching with nonzero-photon sectors, where we find numerically even more intricate and richer Floquet topological phases spring out. We have then analyzed, with the Floquet dynamical mean-field theory, the effects of electron-electron interaction and energy dissipation. We have specifically revealed that phase transitions from Floquet-topological to Mott insulators emerge, where the phase boundaries can again be captured with the high-frequency expansion.
We study a non-Hermitian version of the Rabi model, where a two-level system is periodically driven with an imaginary-valued drive strength, leading to alternating gain and loss. In the Floquet picture, the model exhibits PT\mathcal{PT}PT symmetry, which can be broken when the drive is sufficiently strong. We derive the boundaries of the PT\mathcal{PT}PT phase diagram for the different resonances by doing perturbation theory beyond the rotating-wave approximation. For the main resonance, we show that the non-Hermitian analog of the Bloch-Siegert shift corresponds to maximal PT\mathcal{PT}PT breaking. For the higher-order resonances, we capture the boundaries to lowest order. We also solve the regime of high frequency by mapping to the Wannier-Stark ladder. Our model can be experimentally realized in waveguides with spatially modulated loss or in atoms with time-modulated spontaneous decay.