Physical review. B, Condensed matter

Quantum-beat free-induction decay in Tm2+ :Sr F2 : Fourier-transform ESR spectroscopy by optical means

T. Kohmoto, Yukio Fukuda, M. Tanigawa, Tomobumi Mishina, T. Hashi

Published Sep 1, 1983• 13 citations

Abstract

We demonstrate, for the first time, a nanosecond Fourier-transform ESR experiment in solids achieved by optical means. ESR free-induction-decay signals in 0-100 Oe have been observed in the ground state of ${\mathrm{Tm}}^{2+}$:Sr${\mathrm{F}}_{2}$ as a new type of quantum beat generated by an optical excitation to the absorption band with a circularly polarized light pulse. The Fourier transform of the observed signals gives the ESR spectrum, and the origin of the decay is attributed to the superhyperfine interaction between the ${\mathrm{Tm}}^{2+}$ ion and neighboring fluorine nuclei.

DOI: 10.1103/physrevb.28.2869

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Physical review. B, Condensed matter

Quantum-beat free-induction decay in Tm2+ :Sr F2 : Fourier-transform ESR spectroscopy by optical means

T. Kohmoto, Yukio Fukuda, M. Tanigawa, Tomobumi Mishina, T. Hashi

Published Sep 1, 1983• 13 citations

Publisher

Abstract

{\mathrm{Tm}}^{2+}

:Sr

{\mathrm{F}}_{2}

as a new type of quantum beat generated by an optical excitation to the absorption band with a circularly polarized light pulse. The Fourier transform of the observed signals gives the ESR spectrum, and the origin of the decay is attributed to the superhyperfine interaction between the

{\mathrm{Tm}}^{2+}

ion and neighboring fluorine nuclei.

DOI: 10.1103/physrevb.28.2869

Related papers

Interference pulses in optical free induction decay

K. L. Foster, Stig Stenholm, Richard G. Brewer

A new feature of optical free induction decay (FID) is observed in a coherently prepared sample of $^{13}\mathrm{CH}$ $_{3}\mathrm{F}$ by the method of Stark switching. The preparative phase is due to the resonant steady-state excitation by a cw laser beam, and is followed by FID upon sudden application of a dc Stark field that switches the molecular sample out of resonance. The emission is not observed as a simple decay but instead appears as a train of sharp pulses regularly spaced in time as a result of a repetitive interference. This situation arises because an entire set of infrared transitions within the Stark split manifold are initially prepared, in contrast to our previous study of a nondegenerate transition. The emission, which beats with the laser, produces a heterodyne beat spectrum, consisting of a set of regularly spaced frequencies, that is the Fourier transform of the slowly decaying pulse progression observed. We thus demonstrate what is the optical analog of the well-known NMR method of high-resolution pulse Fourier spectroscopy. The detailed behavior of the pulse train agrees well with an FID theory that assumes the transitions to be uncoupled. The subtle behavior of FID near the time origin is explored also by approximate analytic expressions that reveal either a near zero amplitude or sizable amplitude depending on the degree of saturation in the preparative stage. The experimental technique discussed offers an attractive way for obtaining high-resolution optical spectra without Doppler broadening, and for generating an optical pulse train whose time scale can be compressed by simply increasing the Stark field.A new feature of optical free induction decay (FID) is observed in a coherently prepared sample of $^{13}\mathrm{CH}$$_{3}\mathrm{F}$ by the method of Stark switching. The preparative phase is due to the resonant steady-state excitation by a cw laser beam, and is followed by FID upon sudden application of a dc Stark field that switches the molecular sample out of resonance. The emission is not observed as a simple decay but instead appears as a train of sharp pulses regularly spaced in time as a result of a repetitive interference. This situation arises because an entire set of infrared transitions within the Stark split manifold are initially prepared, in contrast to our previous study of a nondegenerate transition. The emission, which beats with the laser, produces a heterodyne beat spectrum, consisting of a set of regularly spaced frequencies, that is the Fourier transform of the slowly decaying pulse progression observed. We thus demonstrate what is the optical analog of the well-known NMR method of high-resolution pulse Fourier spectroscopy. The detailed behavior of the pulse train agrees well with an FID theory that assumes the transitions to be uncoupled. The subtle behavior of FID near the time origin is explored also by approximate analytic expressions that reveal either a near zero amplitude or sizable amplitude depending on the degree of saturation in the preparative stage. The experimental technique discussed offers an attractive way for obtaining high-resolution optical spectra without Doppler broadening, and for generating an optical pulse train whose time scale can be compressed by simply increasing the Stark field.

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Ryuzi Yano, Naoshi Uesugi

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A. I. Alekseev, O. V. Zhemerdeev

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Journal of the Optical Society of America BJan 1, 19872 citations

{\mathrm{Tm}}^{2+}

:Sr

{\mathrm{F}}_{2}

{\mathrm{Tm}}^{2+}

ion and neighboring fluorine nuclei.

A new feature of optical free induction decay (FID) is observed in a coherently prepared sample of

^{13}\mathrm{CH}

_{3}\mathrm{F}

by the method of Stark switching. The preparative phase is due to the resonant steady-state excitation by a cw laser beam, and is followed by FID upon sudden application of a dc Stark field that switches the molecular sample out of resonance. The emission is not observed as a simple decay but instead appears as a train of sharp pulses regularly spaced in time as a result of a repetitive interference. This situation arises because an entire set of infrared transitions within the Stark split manifold are initially prepared, in contrast to our previous study of a nondegenerate transition. The emission, which beats with the laser, produces a heterodyne beat spectrum, consisting of a set of regularly spaced frequencies, that is the Fourier transform of the slowly decaying pulse progression observed. We thus demonstrate what is the optical analog of the well-known NMR method of high-resolution pulse Fourier spectroscopy. The detailed behavior of the pulse train agrees well with an FID theory that assumes the transitions to be uncoupled. The subtle behavior of FID near the time origin is explored also by approximate analytic expressions that reveal either a near zero amplitude or sizable amplitude depending on the degree of saturation in the preparative stage. The experimental technique discussed offers an attractive way for obtaining high-resolution optical spectra without Doppler broadening, and for generating an optical pulse train whose time scale can be compressed by simply increasing the Stark field.

ESR signals of

{\mathrm{Tm}}^{2+}

{\mathrm{SrF}}_{2}

are observed in the ground

{(}^{2}

{\mathrm{F}}_{7/2}

{E}_{5/2}

) and metastable

{(}^{2}

{\mathrm{F}}_{5/2}

{E}_{5/2}

) states in low magnetic fields (0--300 Oe) at liquid-helium temperatures. We achieved a very high detection sensitivity (\ensuremath{\sim}

{10}^{9}

spins in the ground state) using optical means; the population differences are created by circular dichroism and spin memory, and the change of the Faraday rotation is detected by a polarimeter. Several interesting phenomena were observed. The signals in the ground and metastable states appeared with opposite polarities. The preferential pumping from the metastable state was examined by a double pumping experiment. We also measured the Faraday rotation between 4000 and 7000 A\r{}. The experimental results suggest that the magnetization in the metastable state created by the preferential pumping from the ground state followed by the spin memory is in the opposite direction to that in the ground state. Anomalous behavior of the metastable-state signals was observed both in frequency and time domains. These are explained as an effect of the metastable-state--ground-state cross relaxation enhanced by the ground-state--ground-state cross relaxation.