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Physical Review Letters

Solid-State Nuclear Spin-Flip Maser Pumped by Dynamic Nuclear Polarization

Peter Boesiger, Ernst Brun, D. Meier

Published Mar 14, 1977• 65 citations
Publisher

Abstract

We report the observation of a coherent, maser-type rf radiation of the $^{27}\mathrm{Al}$ nuclear-spin system in ${\mathrm{Al}}_{2}$${\mathrm{O}}_{3}$: ${\mathrm{Cr}}^{3+}$ pumped by dynamic nuclear polarization to negative temperature. A theoretical description is presented for the sharp, superradiant bursts which follow the fast tuning of a resonant $\mathrm{LC}$ circuit to a selected NMR line of $^{27}\mathrm{Al}$. Experimental results are discussed which demonstrate the interplay between dynamic nuclear polarization, relaxation, and the radiation field.

DOI
10.1103/physrevlett.38.602

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We report the observation of a coherent, maser-type rf radiation of the 27Al^{27}\mathrm{Al}27Al nuclear-spin system in {\mathrm{Al}}_{2}$${\mathrm{O}}_{3}: Cr3+{\mathrm{Cr}}^{3+}Cr3+ pumped by dynamic nuclear polarization to negative temperature. A theoretical description is presented for the sharp, superradiant bursts which follow the fast tuning of a resonant LC\mathrm{LC}LC circuit to a selected NMR line of 27Al^{27}\mathrm{Al}27Al. Experimental results are discussed which demonstrate the interplay between dynamic nuclear polarization, relaxation, and the radiation field.
Radio wave amplification by stimulated emission of radiation (NMR laser) was observed in Al2{\mathrm{Al}}_{2}Al2​O3{\mathrm{O}}_{3}O3​: Cr3+{\mathrm{Cr}}^{3+}Cr3+ (ruby) with the 27Al^{27}\mathrm{Al}27Al spin system pumped to an inverted Zeeman state by means of dynamic nuclear polarization (DNP) and with an LC circuit tuned to the NMR transitions. A theory is developed which combines standard Bloch equations with the dynamic equations of a heat-reservoir model for the spin dynamics. Experimental data concerning the relaxation and polarization mechanisms in the nonradiant state are presented, and the parameters of the reservoir model are determined. In accord with these results, dynamic NMR laser equations for different modes of operation (continuous or pulsed) are derived from which the threshold of the NMR laser, its critical behavior near threshold, and its transient response after QQQ-switch tuning can be calculated. The agreement between theory and experiments in the superradiant state reflects unambiguously the interplay between nuclear-spin relaxation, DNP, spin fluctuations, and the self-induced ordering of the 27Al^{27}\mathrm{Al}27Al spins perpendicular to the applied field. In particular, the results highlight the decisive role of the electronic dipole-dipole system in the spin and NMR laser dynamics of ruby. Special emphasis is placed on the close relationship between the NMR laser, as a system far from thermal equilibrium which shows the phenomenon of cooperative self-organization, and a system at thermal equilibrium which undergoes a second-order phase transition. Thus, the rotating nuclear-spin magnetization is treated as an order parameter.
The main part of this review is devoted to the comprehensive description of coherent radiation by nuclear spins. The theory of nuclear spin superradiance is developed and the experimental observations of this phenomenon are considered. The intriguing problem of how coherence develops from initially incoherent quantum fluctuations is analysed. All main types of coherent radiation by nuclear spins are discussed, which are: free nuclear induction, collective induction, maser generation, pure superradiance, triggered superradiance, pulsing superradiance, punctuated superradiance, and induced emission. The influence of electron-nuclear hyperfine interactions and the role of magnetic anisotropy are studied. Conditions for realizing spin superradiance by magnetic molecules are investigated. The possibility of nuclear matter lasing, accompanied by pion or dibaryon radiation, is briefly touched.
We present experimental single and multimode sustained ^{1}H NMR masers in solution on thermally polarized spins at room temperature and 9.4 T achieved through the electronic control of radiation feedback (radiation damping). Our observations illustrate the breakdown of the usual three-dimensional Maxwell-Bloch equations for radiation feedback and a simple toy model of few coupled classical moments is used to interpret these experiments. This Letter represents a significant step to bring the spontaneous radiation damping based NMR masers in various contexts to the next stage of feedback-controlled and reproducible experiments.
A theory is proposed to account for the superradiance emitted by a system of nuclear spins interacting with a resonant circuit. A study is reported of the dependences of the parameters of the superradiance pulses on the main parameters of the medium. A comparison is made of these dependences with the corresponding expressions in the optical superradiance case. The transition from superradiance to maser operation is investigated. It is shown that the calculations are in full agreement with the experimental curves.
Spontaneous generation of the Dicke superradiation (SR) state has been found in the system of inversely polarised proton spins with “frozen” polarisation. SR is observed at the moment when the Larmor frequency crosses the resonance frequency of the passive oscillatory circuit. SR arises from incoherent maser generation of spins. The frequency of a SR generator can be retuned from several hundreds of kilohertz to hundreds of megahertz at very low temperatures. Dependence of incoherent and coherent radiation on the initial polarisation has been investigated. A radio frequency analogue of the optical SR laser is shown to be possible both for weak-amplifying and for strong-amplifying active media, depending on the factor of filling and polarisation of nuclei. SR-reverse of negative polarisation is observed in the latter case.
A study of the physics of a nuclear magnetic resonance gyroscope is described. Experimental results in nuclear polarization and relaxation in 3He are obtained using an optical pumping apparatus and a high resolution rf spectroscopic technique. Polarization in the metastable states of the heavy noble gases (20, 21 Ne, 129, 132 Xe) was observed using a similar optical pumping apparatus. A sensitive detection method based on optical polarization of an excited state transition is developed and compared with the conventional method of monitoring optical transmission through the optical pumping cell. A new concept for the optical pumping of odd-mass-numbered heavy noble was isotopes to provide for ground-state nuclear polarization is discussed. Significant polarization in excited state neon was observed via collisional transfer from optically pumped helium in a cell filled with a mixture of helium and neon isotopes. The measured polarization was essentially independent of the isotopic composition. (Author)