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The Journal of Chemical Physics

A presentation of pulsed nuclear magnetic resonance with full quantization of the radio frequency magnetic field

J. Jeener, Françoise Hénin

Published May 8, 2002• 17 citations
Publisher

Abstract

We show that there is excellent quantitative agreement between the usual semiclassical predictions for nuclear magnetic resonance experiments (quantized spins interacting with a classical radio frequency magnetic field, including radiation damping), and the predictions of a fully quantized description of the same experiment. We also propose a pictorial description of the relevant dynamical quantum states, which helps to lead the intuition towards the same conclusion. Our model ignores spin relaxation, and simulates the equivalent damping resistor of the sample circuit by a very long piece of lossless coaxial cable. The classical rf field (pulses and free induction decay) is described quantum mechanically by means of Glauber’s “coherent” or “quasiclassical” states.

DOI
10.1063/1.1467332

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Dissipação e ruído de dipolos magnéticos coletivamente acoplados a um circuito ressonante

Alencar José de Faria

We study the radiation damping and the spin noise of a magnetic material coupled with a resonant circuit.Radiation damping in magnetic resonance is a dissipation phenomenon, where magnetization prepared after a Rabi pulse decays toward its equilibrium state.The magnetic sample loses its energy by the coupling with resonant circuit, that must be tuned in Larmor frequency of the sample spins.Even though this phenomenon had been studied many years ago, no full quantum description was done.We present a quantum Hamiltonian model, that explains the radiation damping.We use quantum Langevin equation method for this task.Beyond radiation damping, we show the magnetization acquires an unusual intrincate motion, if the circuit initial state is coherent.Using the same Langevin equation, we study the sample inuence on the resonant circuit noise.We calculate the current spectral density in the case of thermal equilibrium of whole system.We can verify the method eectiveness, comparing former papers.Moreover we study modications in the circuit noise, if an external oscillating tension is applied.In this situation, other two peaks emerge in the central peak sidebands of the sample absorption spectrum.It leads to appear three dips in circuit current spectrum.This eect is due to the splitting of the spin energy states.We comment about the analogy between this phenomenon and the resonance uorescence in Quantum Optics.

•Mar 17, 2008•0 citations
We show that there is excellent quantitative agreement between the usual semiclassical predictions for nuclear magnetic resonance experiments (quantized spins interacting with a classical radio frequency magnetic field, including radiation damping), and the predictions of a fully quantized description of the same experiment. We also propose a pictorial description of the relevant dynamical quantum states, which helps to lead the intuition towards the same conclusion. Our model ignores spin relaxation, and simulates the equivalent damping resistor of the sample circuit by a very long piece of lossless coaxial cable. The classical rf field (pulses and free induction decay) is described quantum mechanically by means of Glauber’s “coherent” or “quasiclassical” states.
We apply the methods of cavity quantum electrodynamics (CQED), to obtain a microscopic and fully quantum-mechanical picture of radiation damping in magnetic resonance, and the nascent formation of the free induction signal. Numerical solution of the Tavis-Cummings model - i.e., multiple spins 1∕2 coupled to a lossless single-mode cavity - shows in fine detail the transfer of Zeeman energy, via spin coherence, to excite the cavity - represented here by a quantized LC resonator. The case of a single spin is also solved analytically. Although the motion of the Bloch vector is non-classical, we nonetheless show that the quantum mechanical Rabi nutation frequency (as enhanced by cavity coupling and stimulated emission) gives realistic estimates of macroscopic signal strength and the radiation damping constant in nuclear magnetic resonance. We also show how to introduce dissipation: cavity losses by means of a master equation, and relaxation by the phenomenological method of Bloch. The failure to obtain the full Bloch equations (unless semi-classical conditions are imposed on the cavity) is discussed in light of similar issues arising in CQED (and in earlier work in magnetic resonance as well), as are certain problems relative to quantization of the electromagnetic near-field.
In NMR experiments, interaction of quantized radio-frequency (rf) field leads to entanglement of nuclear spin with the electromagnetic field. In an entangled state, the nuclear spins are depolarized with no net magnetization, which cannot give a detectable signal in inductive detection. We show that when the electromagnetic field is in coherent state, inductive detection is just true. We develop the mathematics to study the evolution of a coherent rf-field with a sample of all polarized spins. We show that evolution can be solved in closed form as a separable state of rf-field and spin ensemble, where spin ensemble evolves according to Bloch equations in an rf field. We extend the analysis and results to a spin ensemble with Boltzmann polarization. The rabi frequency and coupling strength of spins to rf-field depends on number state of the rf-field. We show that in interaction with a coherent rf-field, this variation in coupling strength, introduces negligible error.
In this paper, we study the interaction of quantized radio-frequency (rf)/microwave-field with nuclear spin in Nuclear Magnetic Resonance (NMR) or electron spin in Electron Paramagnetic Resonance (EPR). In magnetic resonance experiments, interaction of quantized rf-field leads to entanglement of spin with the electromagnetic field. In an entangled state, the spins are depolarized with no net transverse magnetization, which cannot give a detectable signal in inductive detection (or Q detection) that detects transverse magnetization. We show that when the electromagnetic field is in coherent state, inductive detection becomes possible. We use the mathematics of quantum optics to study the evolution of a coherent rf-field with a sample of all polarized spins. We show that evolution can be solved in closed form as a separable state of rf-field and spin ensemble, where spin ensemble evolves according to Bloch equations in an rf-field. We extend the analysis and results to a spin ensemble with Boltzmann polarization. The rabi frequency and coupling strength of spins to rf-field depends on number state of the rf-field. We show that in interaction with a coherent rf-field, this variation in coupling strength introduces negligible error.
We numerically solve the Liouville equation for the Tavis Cummings model of multiple spins coupled to a lossless single mode cavity, starting from an initial condition with small numbers of fully polarized spins tipped by a specified angle, and the cavity in its ground Fock state. Time evolution of the magnetizations and cavity states, following small to medium nutation by a classical field, yields a microscopic quantum mechanical picture of radiation damping in magnetic resonance, and the formation of the free induction signal, that is, the transfer of Zeeman energy, via spin coherence, to cavity coherence. Although the motion of the Bloch vector is nonclassical, our quantum description is related to the macroscopic picture of NMR reception, by showing the close relationship between the usual radiation damping constant, and the quantum mechanical Rabi nutation frequency (as enhanced by cavity coupling and stimulated emission.) That is, each is the product, of a nutation rate per oscillator current, and a current. Although the current in the damping constant is explicitly limited by cavity losses, which do not enter the formula for the Rabi frequency, we nonetheless show (in an appendix) how these losses can be introduced into our problem by means of a master equation. Numerical solution of the classical Bloch-Kirchhoff equations reinforces the conclusion that the strength of the free induction
Large-amplitude oscillations are predicted in the free-induction decay (FID) of atomic or spin two-level quantum systems that are coherently prepared by a resonant electromagnetic field in the form of a square amplitude pulse of duration TTT. The effect should be detectable in nuclear magnetic resonance (NMR) or in optical resonance experiments when the transition line shape is inhomogeneously broadened (${T}_{2}^{*}\ensuremath{\ll}{T}_{2}$) and the applied field is intense enough that the pulse area $\ensuremath{\chi}T\ensuremath{\ge}2\ensuremath{\pi}$, where $\ensuremath{\chi}$ is the Rabi frequency. Physically, the effect is due to Rabi oscillations which are generated in the preparative stage and are then reproduced because of atomic memory in the radiative period which follows. The atomic polarization derived from the Bloch equations assumes the form of an integral over the inhomogeneous line shape, and can be evaluated numerically for arbitrary linewidth $\ensuremath{\sigma}$ or analytically when $\ensuremath{\sigma}\ensuremath{\rightarrow}\ensuremath{\infty}$. The characteristics of the oscillation are unusual since the oscillation frequency, which is of order $\ensuremath{\chi}$, increases with time while the oscillation envelope vanishes identically for times $t\ensuremath{\ge}2T$. Coherent emission is therefore confined to one pulse width TTT immediately following the pulse. Previous NMR and infrared FID experiments with small-area pulses ($\ensuremath{\chi}T\ensuremath{\le}4\ensuremath{\pi}$), interpreted erroneously in terms of an edge echo effect, support the oscillatory FID behavior described here. For the case $\ensuremath{\chi}T>4\ensuremath{\pi}$, an experimental test would be even more decisive, as the oscillations are more pronounced.
We study the radiation damping and the spin noise of a magnetic material coupled with a resonant circuit.Radiation damping in magnetic resonance is a dissipation phenomenon, where magnetization prepared after a Rabi pulse decays toward its equilibrium state.The magnetic sample loses its energy by the coupling with resonant circuit, that must be tuned in Larmor frequency of the sample spins.Even though this phenomenon had been studied many years ago, no full quantum description was done.We present a quantum Hamiltonian model, that explains the radiation damping.We use quantum Langevin equation method for this task.Beyond radiation damping, we show the magnetization acquires an unusual intrincate motion, if the circuit initial state is coherent.Using the same Langevin equation, we study the sample inuence on the resonant circuit noise.We calculate the current spectral density in the case of thermal equilibrium of whole system.We can verify the method eectiveness, comparing former papers.Moreover we study modications in the circuit noise, if an external oscillating tension is applied.In this situation, other two peaks emerge in the central peak sidebands of the sample absorption spectrum.It leads to appear three dips in circuit current spectrum.This eect is due to the splitting of the spin energy states.We comment about the analogy between this phenomenon and the resonance uorescence in Quantum Optics.