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Optics Letters

Kilohertz-resolution pump–probe spectroscopy in Pr^3+:YAlO_3

Masaharu Mitsunaga, Kazuhiko Sugiyama, Naoshi Uesugi

Published Aug 1, 1993• 20 citations
Publisher

Abstract

We observed saturated absorption spectra of hole widths as narrow as 10.5 kHz with an excellent signal-to-noise ratio in a cryogenic Pr(3+):YA1O(3) sample, using a frequency-stabilized dye laser in a noncollinear frequency-domain pump-probe measurement. More-detailed theoretical and experimental analyses revealed the existence of an ultranarrow peak of width 10 Hz at the center of the line shape that could be attributed to grating diffraction of the pump beam.

DOI
10.1364/ol.18.001256

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A novel phase-modulation technique which permits subkilohertz-laser stability and new levels of precision in laser spectroscopy was reported recently. For spectroscopy, the basic arrangement consists of a combination of an optical pump and a probe field which is phase modulated. The pump prepares the atomic sample by burning a narrow hole within the atom's inhomogeneous line shape, and the probe beam samples the prepared hole when its modulation sidebands are swept into resonance. Off resonance, the probe is balanced as pairs of sidebands produce heterodyne beat signals of opposite phase which just cancel. On resonance, the balance is upset and yields a nonvanishing beat signal with a Lorentzian absorption or dispersion line shape and with residual noise approaching the shot noise limit. Here we investigate the theory of phase-modulation spectroscopy. We treat the nonlinear response of an atomic two-level quantum system subject to an intense pump and a weak copropagating or counterpropagating phase-modulated probe beam. The density-matrix equations of motion are solved by a Laplace-transform method and by the novel use of a translation operator which allows the infinite hierarchy of coupled equations to close. A solution equivalent to the rate-equation result is developed and coherence corrections are found which predict new resonances that have just been detected in this laboratory. The delayed pump-probe technique encountered in solid-state laser spectroscopy is analyzed in this context for two- and three-level quantum systems. The response of a Fabry-Perot cavity to a phase-modulated light wave is examined also and reveals an unexpected absorption feature.

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Materials for spectral hole-burning storage

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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

Compact laser frequency stabilization at 1.5 μm using spectral hole burning

Thomas Böttger, Geoff J. Pryde, Nick Strickland +1 more

Summary form only given. Laser frequency stabilization to 200 Hz on a 5 ms time scale and to 1 kHz over 30 minutes has been demonstrated using persistent and transient spectral holes in inhomogeneously broadened resonances of Er/sup 3+/,D/sup -/:CaF/sub 2/, Er/sup 3+/:Y/sub 2/SiO/sub 5/, and Er/sup 3+/:KTiOPO/sub 4/ at cryogenic temperatures. Persistent spectral holes with lifetimes of weeks or longer provide a programmable and transportable secondary frequency reference, and kilohertz wide transient spectral holes provide excellent references at millisecond time scales appropriate for spectroscopy and coherent transient signal processing devices. This locking technique has significant applications to devices beyond the field of spectral hole burning.

Quantum Electronics and Laser Science Conference•Nov 13, 2002•0 citations

Pump-probe spectroscopy of cold rubidium atoms in an integrating sphere

Wenli Wang, Richang Dong, Jianliao Deng +1 more

Absorption spectra of cold rubidium atoms in an integrating sphere under the influence of a diffuse laser field have been systematically investigated. A pronounced dispersionlike structure centered at the light-shifted pump frequency is observed with a subnatural linewidth. In particular, two clearly resolved absorption resonances on the $5{S}_{1/2}(F=2)\ensuremath{\rightarrow}5{P}_{3/2}({F}^{\ensuremath{'}}=3)$ transitions occur with variable probe beam intensity, which is consistent with our proposed theoretical model. Based on the two absorption resonances,we measure the dependence of light shifts, from which we can directly extract the effective Rabi frequency in a diffuse laser field, on the probe laser intensity, pump laser intensity, and pump laser detuning. Our work helps to identify the physical mechanisms behind these spectral features and is beneficial for studying the corresponding effect in a cold sample.

Physical Review A•May 5, 2016•0 citations

LASER FREQUENCY STABILIZATION TO SPECTRAL HOLE BURNING FREQUENCY REFERENCES IN ERBIUM-DOPED CRYSTALS: MATERIAL AND DEVICE OPTIMIZATION

Thomas Böttger

Narrow spectral holes in the absorption lines of Er doped crystals have been explored as references for frequency stabilizing external cavity diode lasers at the important 1.5 μm optical communication wavelength. Allan deviations of the beat signal between two independent stabilized lasers as low as 200 Hz over 10 ms integration time have been achieved using regenerative spectral holes in Er:Y2SiO5 and Er:KTP, while drift was reduced to ~ 7 kHz/min by incorporating the inhomogeneous absorption line as a fixed reference. During active stabilization, the transient spectral hole was continuously regenerated as hole burning balanced relaxation. In contrast, persistent spectral holes in Er:D:CaF2, with lifetimes of several weeks, provided programmable and transportable secondary frequency references that maintained sub-kilohertz stability over several seconds and enabled 6 kHz stability over 3 1.6 10 s × . The error signal was derived from the spectral hole transmission using frequency modulation spectroscopy. A servo amplifier applied fast frequency corrections to the injection current of the laser diode and slower adjustments to the piezo-driven feedback prism plate. These stabilized lasers provide ideal sources for spectral hole burning applications based on optical coherent transients, where laser stability is required over the storage time of the material. Since the lifetime of the frequency reference is exactly the material storage time, this requirement is automatically met by using our technique. This was demonstrated in Er:Y2SiO5 and successfully transferred to high-bandwidth signal processing applications. The material Er:Y2SiO5 was optimized for these applications. The I15/2 and I13/2 crystal field levels were site-selectively determined by absorption and fluorescence spectroscopy. The excited state lifetime was measured to be 11.4 ms for site 1 and 9.2 ms for site 2. Zeeman experiments and two-pulse photon echo spectroscopy as a function of magnetic field orientation were used to determine the anisotropic electronic g-values for both Er sites and established a preferred magnetic field orientation for minimizing homogeneous line broadening by spectral diffusion. The spectral diffusion was characterized by stimulated photon echo spectroscopy and successfully described with established theories. In a 0.02 atomic percent Er:Y2SiO5 crystal at B = 0.8 T and T = 1.6 K, line broadening became significant after 10 μs, increasing the homogeneous linewidth from 7.5 kHz to 75 kHz after 120 μs. Spectral diffusion, primarily caused by direct phonon driven Er spin-flips in the ground state, can be controlled to negligible levels with proper magnetic field strength and orientation, temperature, and erbium concentration. In optimizing Er:Y2SiO5, the narrowest optical resonance in any solid-state material of 73 Hz was measured.

•Jan 1, 2002•15 citations
We observed saturated absorption spectra of hole widths as narrow as 10.5 kHz with an excellent signal-to-noise ratio in a cryogenic Pr(3+):YA1O(3) sample, using a frequency-stabilized dye laser in a noncollinear frequency-domain pump-probe measurement. More-detailed theoretical and experimental analyses revealed the existence of an ultranarrow peak of width 10 Hz at the center of the line shape that could be attributed to grating diffraction of the pump beam.
A novel phase-modulation technique which permits subkilohertz-laser stability and new levels of precision in laser spectroscopy was reported recently. For spectroscopy, the basic arrangement consists of a combination of an optical pump and a probe field which is phase modulated. The pump prepares the atomic sample by burning a narrow hole within the atom's inhomogeneous line shape, and the probe beam samples the prepared hole when its modulation sidebands are swept into resonance. Off resonance, the probe is balanced as pairs of sidebands produce heterodyne beat signals of opposite phase which just cancel. On resonance, the balance is upset and yields a nonvanishing beat signal with a Lorentzian absorption or dispersion line shape and with residual noise approaching the shot noise limit. Here we investigate the theory of phase-modulation spectroscopy. We treat the nonlinear response of an atomic two-level quantum system subject to an intense pump and a weak copropagating or counterpropagating phase-modulated probe beam. The density-matrix equations of motion are solved by a Laplace-transform method and by the novel use of a translation operator which allows the infinite hierarchy of coupled equations to close. A solution equivalent to the rate-equation result is developed and coherence corrections are found which predict new resonances that have just been detected in this laboratory. The delayed pump-probe technique encountered in solid-state laser spectroscopy is analyzed in this context for two- and three-level quantum systems. The response of a Fabry-Perot cavity to a phase-modulated light wave is examined also and reveals an unexpected absorption feature.
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.
Summary form only given. Laser frequency stabilization to 200 Hz on a 5 ms time scale and to 1 kHz over 30 minutes has been demonstrated using persistent and transient spectral holes in inhomogeneously broadened resonances of Er/sup 3+/,D/sup -/:CaF/sub 2/, Er/sup 3+/:Y/sub 2/SiO/sub 5/, and Er/sup 3+/:KTiOPO/sub 4/ at cryogenic temperatures. Persistent spectral holes with lifetimes of weeks or longer provide a programmable and transportable secondary frequency reference, and kilohertz wide transient spectral holes provide excellent references at millisecond time scales appropriate for spectroscopy and coherent transient signal processing devices. This locking technique has significant applications to devices beyond the field of spectral hole burning.
Absorption spectra of cold rubidium atoms in an integrating sphere under the influence of a diffuse laser field have been systematically investigated. A pronounced dispersionlike structure centered at the light-shifted pump frequency is observed with a subnatural linewidth. In particular, two clearly resolved absorption resonances on the $5{S}_{1/2}(F=2)\ensuremath{\rightarrow}5{P}_{3/2}({F}^{\ensuremath{'}}=3)$ transitions occur with variable probe beam intensity, which is consistent with our proposed theoretical model. Based on the two absorption resonances,we measure the dependence of light shifts, from which we can directly extract the effective Rabi frequency in a diffuse laser field, on the probe laser intensity, pump laser intensity, and pump laser detuning. Our work helps to identify the physical mechanisms behind these spectral features and is beneficial for studying the corresponding effect in a cold sample.
Narrow spectral holes in the absorption lines of Er doped crystals have been explored as references for frequency stabilizing external cavity diode lasers at the important 1.5 μm optical communication wavelength. Allan deviations of the beat signal between two independent stabilized lasers as low as 200 Hz over 10 ms integration time have been achieved using regenerative spectral holes in Er:Y2SiO5 and Er:KTP, while drift was reduced to ~ 7 kHz/min by incorporating the inhomogeneous absorption line as a fixed reference. During active stabilization, the transient spectral hole was continuously regenerated as hole burning balanced relaxation. In contrast, persistent spectral holes in Er:D:CaF2, with lifetimes of several weeks, provided programmable and transportable secondary frequency references that maintained sub-kilohertz stability over several seconds and enabled 6 kHz stability over 3 1.6 10 s × . The error signal was derived from the spectral hole transmission using frequency modulation spectroscopy. A servo amplifier applied fast frequency corrections to the injection current of the laser diode and slower adjustments to the piezo-driven feedback prism plate. These stabilized lasers provide ideal sources for spectral hole burning applications based on optical coherent transients, where laser stability is required over the storage time of the material. Since the lifetime of the frequency reference is exactly the material storage time, this requirement is automatically met by using our technique. This was demonstrated in Er:Y2SiO5 and successfully transferred to high-bandwidth signal processing applications. The material Er:Y2SiO5 was optimized for these applications. The I15/2 and I13/2 crystal field levels were site-selectively determined by absorption and fluorescence spectroscopy. The excited state lifetime was measured to be 11.4 ms for site 1 and 9.2 ms for site 2. Zeeman experiments and two-pulse photon echo spectroscopy as a function of magnetic field orientation were used to determine the anisotropic electronic g-values for both Er sites and established a preferred magnetic field orientation for minimizing homogeneous line broadening by spectral diffusion. The spectral diffusion was characterized by stimulated photon echo spectroscopy and successfully described with established theories. In a 0.02 atomic percent Er:Y2SiO5 crystal at B = 0.8 T and T = 1.6 K, line broadening became significant after 10 μs, increasing the homogeneous linewidth from 7.5 kHz to 75 kHz after 120 μs. Spectral diffusion, primarily caused by direct phonon driven Er spin-flips in the ground state, can be controlled to negligible levels with proper magnetic field strength and orientation, temperature, and erbium concentration. In optimizing Er:Y2SiO5, the narrowest optical resonance in any solid-state material of 73 Hz was measured.