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Physical Review Letters

Coherent Optical Control of Mössbauer Spectra

Olga A. Kocharovskaya, Roman L. Kolesov, Yuri V. Rostovtsev

Published May 3, 1999• 83 citations
Publisher

Abstract

A compound nuclear-electron system driven by a coherent optical field and probed at the gamma-ray M\"ossbauer transition is analyzed for the first time. The possibility of optical control of the M\"ossbauer spectra is predicted. This study provides the basis for a new branch of spectroscopy, laser-M\"ossbauer spectroscopy, and opens prospects for the realization of a gamma-ray laser.

DOI
10.1103/physrevlett.82.3593

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Summary form only given. Recently, it was predicted that laser radiation can be used to manipulate very efficiently nuclear transitions at gamma-ray energies in solids. It results in both drastic qualitative and strong qualitative modifications of the Mossbauer spectra under the action of coherent optical radiation. The solid sample represents a host matrix where high densities of the ions are embedded by doping. The ions should possess both Mossbauer gamma-ray and optical electronic transitions favorable for the desired effects to be observed. Basically one needs Mossbauer-active ions with strong and sharp optical lines. The latter condition is typically satisfied for rare-earth and transition-metal ions in crystalline hosts and, remarkably, the majority of them are also Mossbauer-active.

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Modification of nuclear resonant absorption by means of laser radiation is analyzed both theoretically and experimentally. Theoretical analysis is done on the basis of four-level model of atom. This model includes both electronic and nuclear excitations. It is predicted that under coherent laser driving nuclear resonant Mossbauer absorption can be significantly modified, e.g. new Mossbauer resonances can appear, some of the existing resonances can vanish, both can be Rabi-split, broadened by laser action. In addition, it is predicted that Mossbauer absorption can be completely suppressed due to coherent population trapping. Experimental observation of laser-induced transformations of Mossbauer spectra of 57Fe2+ : MgO is accomplished. New Mossbauer lines appear with laser driving while the existing are broadened. Possible explanations of the observed changes in 57Fe2+ : MgO Mossbauer spectra are population of higher-lying electronic states of iron ion and significant modification of electronic relaxation processes due to modified Jahn-Teller interaction.

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Time-dependent perturbation of Mössbauer spectra

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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 $^{57}\mathrm{Fe}$. 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.

Physical Review A•Apr 1, 1990•23 citations
A compound nuclear-electron system driven by a coherent optical field and probed at the gamma-ray M"ossbauer transition is analyzed for the first time. The possibility of optical control of the M"ossbauer spectra is predicted. This study provides the basis for a new branch of spectroscopy, laser-M"ossbauer spectroscopy, and opens prospects for the realization of a gamma-ray laser.
Summary form only given. Recently, it was predicted that laser radiation can be used to manipulate very efficiently nuclear transitions at gamma-ray energies in solids. It results in both drastic qualitative and strong qualitative modifications of the Mossbauer spectra under the action of coherent optical radiation. The solid sample represents a host matrix where high densities of the ions are embedded by doping. The ions should possess both Mossbauer gamma-ray and optical electronic transitions favorable for the desired effects to be observed. Basically one needs Mossbauer-active ions with strong and sharp optical lines. The latter condition is typically satisfied for rare-earth and transition-metal ions in crystalline hosts and, remarkably, the majority of them are also Mossbauer-active.
Summary form only given. Recently, it was predicted that laser radiation can be used to manipulate very efficiently nuclear transitions at gamma-ray energies in solids. It results in both drastic qualitative and strong qualitative modifications of the Mossbauer spectra under the action of coherent optical radiation. The solid sample represents a host matrix where high densities of the ions are embedded by doping. The ions should possess both Mossbauer gamma-ray and optical electronic transitions favorable for the desired effects to be observed. Basically one needs Mossbauer-active ions with strong and sharp optical lines. The latter condition is typically satisfied for rare-earth and transition-metal ions in crystalline hosts and, remarkably, the majority of them are also Mossbauer-active.
The project is focused on theoretical and experimental studies of the quantum coherence effects at the atomic and nuclear transitions in solids. The main results are the following. 1. Electromagnetically Induced Transparency (EIT) and all-optical writing and probing of quantum coherence in room temperature solids are demonstrated experimentally in the first time. 2. The method for coherent suppression of excited state absorption in laser crystals is suggested. It opens the prospects for realization of the variety tunable solid state lasers including UV and VUV ranges. 3. High-efficient THz generation by means of resonant three-level mixing based on EIT in solids is predicted. 4. EIT in gamma-ray range of frequencies at the nuclear transitions via the nuclear level crossing is demonstrated experimentally in the first time. 5. Slowing of the gamma-ray photons due to the absorption line doublet is demonstrated in the first time. 6. Modifications of the Mossbauer absorption spectra under the action of laser radiation demonstrated experimentally in the first time. 7. The method for suppression of the inhomogeneous line broadening of the Mossbauer spectra is suggested.
Modification of nuclear resonant absorption by means of laser radiation is analyzed both theoretically and experimentally. Theoretical analysis is done on the basis of four-level model of atom. This model includes both electronic and nuclear excitations. It is predicted that under coherent laser driving nuclear resonant Mossbauer absorption can be significantly modified, e.g. new Mossbauer resonances can appear, some of the existing resonances can vanish, both can be Rabi-split, broadened by laser action. In addition, it is predicted that Mossbauer absorption can be completely suppressed due to coherent population trapping. Experimental observation of laser-induced transformations of Mossbauer spectra of 57Fe2+ : MgO is accomplished. New Mossbauer lines appear with laser driving while the existing are broadened. Possible explanations of the observed changes in 57Fe2+ : MgO Mossbauer spectra are population of higher-lying electronic states of iron ion and significant modification of electronic relaxation processes due to modified Jahn-Teller interaction.
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.