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Physical Review A

Floquet-state perturbation theory for the radio-frequency modulation of the Mössbauer resonance

Ilkka Juhani Tittonen, Mikk Lippmaa, Juha Javanainen

Published Feb 1, 1996• 8 citations
Publisher

Abstract

We study theoretically resonance absorption of \ensuremath{\gamma} rays by nuclei exposed to an external radio-frequency (rf) magnetic field. The external field is taken to couple directly to the nuclear magnetic moments. Perturbation theory is developed for M\"ossbauer spectroscopy in terms of Floquet eigenstates that incorporate the rf field exactly. The present treatment allows for calculation of the conventional time-averaged absorption spectrum, as well as analysis of the time dependence of absorption, resolved on the scale of a period of the rf field. An efficient numerical implementation of the theory is described and comparisons with the equally general approach of Salkola and Stenholm [M. Salkola and S. Stenholm, Phys. Rev. A 41, 3838 (1990)] are made. We demonstrate that even at off-resonance frequencies a strong modulation leads to shifts of the original static hyperfine lines. Examples of line splittings of NMR's associated with Rabi flopping are also shown. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.1112

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quant-pharXiv:2609.17121•Sep 16, 2026•0 citations
We study theoretically resonance absorption of \ensuremath{\gamma} rays by nuclei exposed to an external radio-frequency (rf) magnetic field. The external field is taken to couple directly to the nuclear magnetic moments. Perturbation theory is developed for M"ossbauer spectroscopy in terms of Floquet eigenstates that incorporate the rf field exactly. The present treatment allows for calculation of the conventional time-averaged absorption spectrum, as well as analysis of the time dependence of absorption, resolved on the scale of a period of the rf field. An efficient numerical implementation of the theory is described and comparisons with the equally general approach of Salkola and Stenholm [M. Salkola and S. Stenholm, Phys. Rev. A 41, 3838 (1990)] are made. We demonstrate that even at off-resonance frequencies a strong modulation leads to shifts of the original static hyperfine lines. Examples of line splittings of NMR's associated with Rabi flopping are also shown. \textcopyright{} 1996 The American Physical Society.
In this paper we derive a complete semiclassical description of M\"ossbauer spectroscopy with arbitrary external or internal perturbations of the active levels. The \ensuremath{\gamma} rays are taken to be weak enough to allow us to evaluate the linear M\"ossbauer response to lowest order in the intensity, in which case the \ensuremath{\gamma}-ray field can be treated classically. It induces transitions between level manifolds that can have arbitrary interactions inside themselves. The nuclear system is described by a density matrix. In principle, time-dependent perturbations can be handled by the formalism, but the equations are easier to solve for systems that display steady-state behavior. We consider, in particular, the case of magnetic radio-frequency modulation of the M\"ossbauer levels. Utilizing a matrix-continued-fraction technique, we solve for the absorption spectrum, and we choose numerical illustrations with parameters such that they describe the nucleus 57Fe^{57}\mathrm{Fe}57Fe. In this paper we treat mainly the case of magnetic modulation, but other experimental arrangements are discussed too. The calculations are able to treat both saturation and interference effects, which become important when the radio-frequency modulation is very strong. The new feature that emerges is the occurrence of resonances arising from the interference of different physical processes. The calculational method and its results are discussed and compared with other works.
As part of our general programme to develop the field of quantum nucleonics, we have studied Mössbauer spectroscopy when there is Zeeman splitting of the nuclear levels and a further interaction due to an applied rf-radiation field. We have applied the `dressed' state concept, developed in quantum electronics, to this situation. In particular, we have studied the case when the rf frequency is in the neighbourhood of the ground state (spin =1/2) splitting. The dressed-state approach in this case treats the coupling of nuclear Zeeman levels, due to an rf field, by considering the total system made up of nucleus, static magnetic field and rf field as one global quantum system. This allows the time evolution of the system to be handled straightforwardly. The energy levels and corresponding eigenstates of the system are calculated as a function of the rf frequency and the magnitude of the rf magnetic flux density. Mössbauer spectra are calculated for the case in which the source is subjected to both the static and radiation fields while the absorber nuclear levels are unsplit. Spectra are given as a function of the rf frequency, the magnitude of rf-field magnetic flux density, as well as the photon direction.
We present the first experimental observation of the Rabi splitting of M\"ossbauer resonance lines. A radio-frequency magnetic field is tuned to induce transitions between hyperfine sublevels of the Zeeman-split excited or ground state of 57Fe^{57}\mathrm{Fe}57Fe nuclei. The line splitting corresponding to the Rabi flopping frequency is observed using a magnetically soft 57FeNi^{57}\mathrm{FeNi}57FeNi absorber foil of composition with almost zero magnetostriction.
The effect of an ac modulation on a 2-level or 3-level system is studied theoretically. The absorption spectrum is calculated by solving the optical Bloch equations and is interpreted by reference to the Floquet quasienergy spectrum. The dependence of the absorption sidebands on the intensity of the coupling laser field in Rydberg systems submitted to a radio-frequency (rf) field is analysed in detail. It is shown that for sufficiently strong coupling fields additional sidebands appear in the probe absorption spectrum in ladder 3-level systems. These additional sidebands are induced by the coupling of the intermediate state to the Floquet manifold spawned by the upper state under rf modulation.
We conduct a numerical study of the possibility of using the `magic-angle' technique to suppress inhomogeneous broadening of Mössbauer spectra. We use the Floquet-state perturbation theory for the rf modulation of the Mössbauer resonance, which was adjusted to suit our purpose. A system of two nuclei of 57Fe coupled by the dipole–dipole interaction is considered. The analysis here completes studies started in 2004, by including the dipole–dipole interaction between one nucleus in the ground state and the other in the excited state. We show that partial suppression of inhomogeneous broadening remains possible.
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.