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Quantum Electronics and Laser Science Conference

High-resolution optical hole burning and double resonance of holmium centers in CaF 2

Z. Hasan, Michael G. Solonenko, Giti A. Khodaparast

Published May 22, 1995• 0 citations
OpenAlex

Abstract

Optical-hole burning and associated double-resonance techniques give unsurpassed resolution to the frequency-domain spectroscopy of solids. The present work not only is a demonstration of the strength of the technique in simplifying a complicated spectrum, Ho3+ in CaF2, but it also gives fundamental information about this system in great detail.

Related papers

Optical hole burning by superhyperfine interactions in CaF_2:Pr^3+

R. M. Macfarlane, Robert M. Shelby, Douglas P. Burum

Optical hole burning has been observed in the 5941-A transition of Pr(3+) in a charge-compensated tetragonal site of CaF(2) . The Pr(3+) ground state is doubly degenerate and shows a large first-order hyperfine splitting, which is clearly resolved because of the very narrow inhomogeneous linewidth of 650 MHz. The hole burning involves a new mechanism, in which optically induced spin flips of neighboring nuclei (here (19)F) shift the optical transition frequency outside its homogeneous linewidth. This mechanism was confirmed by optical rf double resonance.

Optics Letters•Dec 1, 1981•38 citations

Laser Hole Burning Spectroscopy: A High Resolution Probe of Molecular Environments.

R. M. Macfarlane, Robert M. Shelby

Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.

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Frequency and time domain techniques of homogeneous laser spectroscopy of ions in solids are reviewed. Applications in three areas of current interest in our lab are described. These are: resonant energy transfer in ruby, strain characterization of crystals and the possible application of optical hole burning of inhomogeneously broadened lines in solids to a high capacity optical memory.

lase•Jan 1, 1981•0 citations

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Materials for spectral hole-burning storage

W. E. Moerner

One very exciting application of laser spectroscopy would be to use the high-resolution capabilities of today’s lasers and the phenomenon of persistent spectral hole-burning to form a frequency domain optical storage system.1 In such a system, bits of information would be stored by locally modifying (in the frequency domain) the shape of an inhomogeneously broadened absorption line of an absorber in a solid at low temperatures. Because typical homogeneous widths are 1000X (or more) narrower than typical inhomogeneous widths, as many as 1000 bits could be written in one diffraction-limited 1-μm spot In a sample, yielding the impressive storage density of 1011 bits/cm2.

Conference on Lasers and Electro-Optics•Jan 1, 1983•1 citation

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:

Annual Review of Physical Chemistry•Jan 1, 1989•230 citations
Optical-hole burning and associated double-resonance techniques give unsurpassed resolution to the frequency-domain spectroscopy of solids. The present work not only is a demonstration of the strength of the technique in simplifying a complicated spectrum, Ho3+ in CaF2, but it also gives fundamental information about this system in great detail.
Optical hole burning has been observed in the 5941-A transition of Pr(3+) in a charge-compensated tetragonal site of CaF(2) . The Pr(3+) ground state is doubly degenerate and shows a large first-order hyperfine splitting, which is clearly resolved because of the very narrow inhomogeneous linewidth of 650 MHz. The hole burning involves a new mechanism, in which optically induced spin flips of neighboring nuclei (here (19)F) shift the optical transition frequency outside its homogeneous linewidth. This mechanism was confirmed by optical rf double resonance.
Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.
One very exciting application of laser spectroscopy would be to use the high-resolution capabilities of today’s lasers and the phenomenon of persistent spectral hole-burning to form a frequency domain optical storage system.1 In such a system, bits of information would be stored by locally modifying (in the frequency domain) the shape of an inhomogeneously broadened absorption line of an absorber in a solid at low temperatures. Because typical homogeneous widths are 1000X (or more) narrower than typical inhomogeneous widths, as many as 1000 bits could be written in one diffraction-limited 1-μm spot In a sample, yielding the impressive storage density of 1011 bits/cm2.
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: