Physical Review A

Laser-Induced Fluorescence-Line-Narrowing Spectroscopy of Glass: Nd

L. A. Riseberg

Published Feb 1, 1973• 80 citations

Abstract

Laser-induced fluorescence line narrowing has been studied in a series of samples of glass: Nd. The features of the nonresonant-excitation technique are described, and the results are discussed in terms of the known spectroscopic properties of the glass: Nd system. The concentration and temperature dependence of the line narrowing have been studied, and the spectral diffusion that is observed is analyzed in terms of resonant ion-ion energy transfer.

DOI: 10.1103/physreva.7.671

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Physical Review A

Laser-Induced Fluorescence-Line-Narrowing Spectroscopy of Glass: Nd

L. A. Riseberg

Published Feb 1, 1973• 80 citations

Publisher

Abstract

DOI: 10.1103/physreva.7.671

Related papers

Observation of Laser-Induced Fluorescence Line Narrowing in Glass: Nd

L. A. Riseberg

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Using resonance ruby-laser excitation, narrowing of the ruby ${R}_{1}$ fluorescence line to width 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ at 4.2\ifmmode^\circ\else\textdegree\fi{}K is observed. Absence of spectral diffusion indicates that a short-range interaction rather than earlier postulated multipolar interactions is responsible for energy transfer in concentrated ruby.Using resonance ruby-laser excitation, narrowing of the ruby ${R}_{1}$ fluorescence line to width 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ at 4.2\ifmmode^\circ\else\textdegree\fi{}K is observed. Absence of spectral diffusion indicates that a short-range interaction rather than earlier postulated multipolar interactions is responsible for energy transfer in concentrated ruby.

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Peter M. Selzer, David L. Huber, B. B. Barnett +1 more

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We report the direct observation of energy migration and spectral diffusion in the $^{3}P_{0}$ state of La ${\mathrm{F}}_{3}$ : ${\mathrm{Pr}}^{3+}$ using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.We report the direct observation of energy migration and spectral diffusion in the $^{3}P_{0}$ state of La${\mathrm{F}}_{3}$: ${\mathrm{Pr}}^{3+}$ using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.

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Hole-Burning Spectroscopy

Silvia Volker

The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:

Annual Review of Physical ChemistryJan 1, 1989230 citations

Laser-induced fluorescence line narrowing has been observed for the first time in a nonresonantly excited rare-earth system. Excitation with the 4727-\AA{}

{A}^{+}

line into the

^{4}G_{\frac{11}{2}}

level of

{\mathrm{Nd}}^{3+}

in glass results in narrowing of transitions from the

^{4}F_{\frac{3}{2}}

to both the

^{4}I_{\frac{9}{2}}

ground manifold and the

^{4}I_{\frac{11}{2}}

excited manifold. The concentration dependence of the line narrowing provides information regarding resonant ion-ion energy transfer within the inhomogeneously broadened system.

Using resonance ruby-laser excitation, narrowing of the ruby

{R}_{1}

fluorescence line to width 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ at 4.2\ifmmode^\circ\else\textdegree\fi{}K is observed. Absence of spectral diffusion indicates that a short-range interaction rather than earlier postulated multipolar interactions is responsible for energy transfer in concentrated ruby.

Fluorescence-line-narrowing and time-resolved studies have been conducted in ruby crystals and powders, in concentrations varying from 0.025 to 0.9 at.%. The resonance fluorescence component of the

{R}_{1}

line at low temperatures is observed to increase dramatically as the laser is tuned from line center toward the low-energy wing of the inhomogeneously broadened absorption. This is presumed to indicate the presence of weakly coupled pairs in the wings of the line. Intraline and interline (${R}_{1}\ensuremath{\rightarrow}{N}_{1,2}$) energy transfer have also been studied, and an elaboration of earlier work is given. Time-resolved selective-excitation scans have revealed numerous channels in the vicinity of the

R

lines by which the different pairs can be directly excited. These are assumed to be Cr ions near enough to a pair to be in a highly perturbed environment. Various experimental results are shown to be consistent with a model of rapid transfer between resonant Cr ions which feeds the pairs via a weak, nonresonant coupling to these perturbed ions. Macroscopic strain broadening is also shown to be favored over microscopic broadening, and the implications for Anderson localization in ruby are discussed.

We report the direct observation of energy migration and spectral diffusion in the

^{3}P_{0}

state of La

{\mathrm{F}}_{3}

{\mathrm{Pr}}^{3+}

using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.