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Physical Review A

Transient nutations decay: The effect of field-modified dipolar interaction

S. Agnello, R. Boscaino, M. Cannas, F. M. Gelardi, R. N. Shakhmuratov

Published May 1, 1999• 23 citations
Publisher

Abstract

The anomalous behavior of transient nutations is experimentally investigated in a set of two-level $(S=\frac{1}{2})$ spin systems differing only in spin concentration. Our results show that the non-Bloch power dependence of the decay rate of transient nutations is a concentration-dependent effect, which is more and more pronounced in more and more concentrated samples. The experimental results are interpreted in the framework of the recent theory by Shakhmuratov et al. [Phys. Rev. Lett. 79, 2963 (1997)] and support the hypothesis that the anomalous decay of transient nutations in solids originates from radiation-induced changes of the dipolar field, rather than from residual fluctuations of the nominally coherent field.

DOI
10.1103/physreva.59.4087

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The anomalous behavior of transient nutations is experimentally investigated in a set of two-level (S=12)(S=\frac{1}{2})(S=21​) spin systems differing only in spin concentration. Our results show that the non-Bloch power dependence of the decay rate of transient nutations is a concentration-dependent effect, which is more and more pronounced in more and more concentrated samples. The experimental results are interpreted in the framework of the recent theory by Shakhmuratov et al. [Phys. Rev. Lett. 79, 2963 (1997)] and support the hypothesis that the anomalous decay of transient nutations in solids originates from radiation-induced changes of the dipolar field, rather than from residual fluctuations of the nominally coherent field.
Here, a theory of the intensity and concentration dependent damping of nutation signals observed by Boscaino et al. (Phys. Rev B 48, 7077 (1993); Phys. Rev. A 59, 4087 (1999)) and by others in various two-level spin systems is proposed. It is shown that in diluted paramagnetic solids contribution of dipole-dipole interaction to the nutation decay is negligibly small. We elaborated a cavity loss (radiation damping) mechanism that explains the intensity- and concentration dependence of the damping. It is shown that instead of ordinary Bloch's transverse T2 and longitudinal T1 damping parameters the decay of transverse and longitudinal spin components in nutation process are described by one and the same intensity-, concentration-, frequency- and time dependent damping parameter.
We study experimentally the dynamical and decay properties of the Stimulated Nutation Echo (SNE) in a two-level spin system. This is the signal which appears in the transient response of the system to the second pulse at time tau_1 elapsed from its beginning and coinciding with the duration of the first pulse. The information about the first pulse duration is imprinted into the population difference of the inhomogeneously broadened ensemble of the two-level absorbers. The decay of the SNE signal has two contributions. One originates from the population decay during the time tau between the pulses. Another is caused by the coherence loss during the excitation by the first pulse and the reading time of the second pulse. Experimental results on the decay properties induced by these mechanisms are presented. The dependence of these decay rates on the pulse intensity is discussed, and its relationship with the anomalous (non-Bloch) decay of other coherent transients in solids is examined.
Free induction decay and transient nutations are investigated in a system of two-level particles with an inhomogeneously broadened spectrum. The influence of the x (real) and y (imaginary) parts of the complex amplitude of the noise, induced by the driving field in the sample, is considered. It is shown that both noises affect T1{T}_{1}T1​ and T2{T}_{2}T2​ relaxation processes. When field-noise contributions to 1/T2{1/T}_{2}1/T2​ and 1/T1{1/T}_{1}1/T1​ relaxation rates are dominant and equal to each other, Bloch's saturation is changed to Redfield's saturation. This effect also accelerates transient nutation decay. Comparison with experimentally observed free induction decay and transient nutation in color centers in quartz is discussed.
We study experimentally the dynamical and decay properties of the stimulated nutation echo (SNE) in a two-level spin system, the signal of which allows the observation timescale of the driven coherence relaxation to be extended. This signal appears in the transient response of the system to the second pulse at time τ 1 from its start and coinciding with the duration of the first pulse. The information about the first pulse duration is imprinted into the population difference of the inhomogeneously broadened ensemble of the two-level absorbers. The decay of the SNE signal has two contributions. One originates from the population decay during the time τ between the two pulses. Another is caused by the coherence loss during the excitation by the first pulse and the reading time of the second pulse. Experimental results on the decay properties induced by these mechanisms are presented for the first time. We investigate the dependence of these decay rates on the pulse intensity and we examine its relationship with the anomalous (non-Bloch) decay of other coherent transients in solids.
Decay of Rabi oscillations of equivalent spins diluted in diamagnetic solid matrix and coupled by magnetic dipole interactions is theoretically studied. It is shown that these interactions result in random shifts of spin transient nutation frequencies and thus lead to the decay of the transient signal. Averaging over random spatial distribution of spins within the solid and over their spectral positions within magnetic resonance line, we obtain analytical expressions for the decay of Rabi oscillations. The rate of the decay in the case when the half-width of magnetic resonance line exceeds Rabi frequency is found to depend on the intensity of resonant microwave field and on the spin concentration. The results are compared with the literature data for E ′ 1 centers in glassy silica and [AlO 4 ] 0 centers in quartz.
A consistent explanation of recent studies by Szabo and Muramoto [Phys. Rev. A 39, 3992 (1989); 38, 5928 (1988)] on the experimental test of modified optical Bloch equations is presented. It is shown that the observed peculiarities of optical transients in solids are connected with the mechanism of relaxation in systems with slow stochastic modulation. A theory of laser-modified relaxation and analysis of free induction decay (FID), hole burning, and rotary echo (RE) in such systems are presented. The universal character of the FID time dependence and field-independent RE decay is predicted.