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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Editor: Henry van Driel
  • Vol. 29, Iss. 5 — May. 1, 2012
  • pp: 1055–1064

Optically pump-induced athermal and nonresonant refractive index changes in the reference Cr-doped laser materials: Cr:GSGG and ruby

Thomas Godin, Richard Moncorgé, Jean-Louis Doualan, Mickael Fromager, Kamel Ait-Ameur, Renato Antonio Cruz, and Tomaz Catunda  »View Author Affiliations

JOSA B, Vol. 29, Issue 5, pp. 1055-1064 (2012)

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The refractive index of most ion-doped materials increases with the excited state population. This effect was studied in many laser materials, particularly those doped with Cr3+ and rare earth ions, using several techniques, such as interferometry, wave mixing, and Z-scans. This refractive index variation is athermal (has an electronic origin) and is associated with the difference in the polarizabilites of the Cr3+ ion in its excited and ground states, Δαp. The Cr3+ optical transitions in the visible domain are electric-dipole forbidden, and they have low oscillator strengths. Therefore, the major contribution to Δαp has been assigned to allowed transitions to charge transfer bands (CTBs) in the UV with strengths 3 orders of magnitude higher. Although this CTB model qualitatively explains the main observations, it was never quantitatively tested. In order to further investigate the physical origin of Δαp in Cr3+-doped crystals, excited state absorption (ESA) and Z-scan measurements were thus performed in Cr:Al2O3 (ruby) and Cr:GSGG. Cr:GSGG was selected because of the proximity of its E2 and T24 emitting levels, and thus the possibility to explore the role of the spin selection rule in the ESA spectra and the resulting variations in polarizability by comparing low and room temperature data, which were never reported before. On the other hand, Cr:Al2O3 (ruby) was selected because it is the only crystal for which it is possible to obtain CTB absorption data from both ground and excited states, and thus for which it is possible to check the CTB model more accurately. Thanks to these more accurate and more complete data, we came to the first conclusion that the spin selection rule does not play any significant role in the variation of the polarizability with the E2T24 energy mismatch. We also discovered that using the CTB model in the case of ruby would lead to a negative Δαp value, which is contrary to all refractive index variation (including Z-scan) measurements.

© 2012 Optical Society of America

OCIS Codes
(160.3380) Materials : Laser materials
(160.4760) Materials : Optical properties
(190.4720) Nonlinear optics : Optical nonlinearities of condensed matter
(190.2055) Nonlinear optics : Dynamic gratings
(190.4223) Nonlinear optics : Nonlinear wave mixing

ToC Category:

Original Manuscript: October 6, 2011
Revised Manuscript: December 20, 2011
Manuscript Accepted: December 28, 2011
Published: April 23, 2012

Thomas Godin, Richard Moncorgé, Jean-Louis Doualan, Mickael Fromager, Kamel Ait-Ameur, Renato Antonio Cruz, and Tomaz Catunda, "Optically pump-induced athermal and nonresonant refractive index changes in the reference Cr-doped laser materials: Cr:GSGG and ruby," J. Opt. Soc. Am. B 29, 1055-1064 (2012)

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  1. W. Koechner, Solid-State Laser Engineering, 5th ed. (Springer-Verlag, 1999).
  2. H. J. Eichler, P. Gunter, and D. W. Pohl, Laser-Induced Dynamic Gratings (Springer-Verlag, 1986).
  3. R. C. Powell and S. A. Payne, “Dispersion effects in 4-wave-mixing measurements of ions in solids,” Opt. Lett. 15, 1233–1235 (1990). [CrossRef]
  4. H. K. Lee and S. S. Lee, “Measurements of the anisotropic nonlinear refractive-index coefficients of ruby,” Opt. Lett. 15, 54–56 (1990). [CrossRef]
  5. D. J. Bradley, G. Magyar, and M. C. Richardson, “Intensity dependent frequency shift in ruby laser giant pulses,” Nature 212, 63–64 (1966). [CrossRef]
  6. D. Pohl, “Inversion dependent frequency drifts in giant pulse ruby lasers,” Phys. Lett. A 26, 357–358 (1968). [CrossRef]
  7. S. M. Lima and T. Catunda, “Discrimination of resonant and nonresonant contributions to the nonlinear refraction spectroscopy of ion-doped solids,” Phys. Rev. Lett. 99, 243902 (2007). [CrossRef]
  8. T. N. C. Venkatesan and S. L. Mccall, “Optical bistability and differential gain between 85 and 296K in a Fabry-Perot containing ruby,” Appl. Phys. Lett. 30, 282–284 (1977). [CrossRef]
  9. P. F. Liao and D. M. Bloom, “Continuous-wave backward-wave generation by degenerate 4-wave mixing in ruby,” Opt. Lett. 3, 4–6 (1978). [CrossRef]
  10. T. Catunda, J. P. Andreeta, and J. C. Castro, “Differential interferometric-technique for the measurement of the nonlinear index of refraction of ruby and GdAlO3:Cr3+,” Appl. Opt. 25, 2391–2395 (1986). [CrossRef]
  11. I. McMichael, P. Yeh, and P. Beckwith, “Nondegenerate 2-wave mixing in ruby,” Opt. Lett. 13, 500–502 (1988). [CrossRef]
  12. C. L. Adler and N. M. Lawandy, “Temperature and spectral dependence of the nonlinear index of ruby via nondegenerate 2-wave mixing,” Opt. Commun. 81, 33–37 (1991). [CrossRef]
  13. L. C. Oliveira, T. Catunda, and S. C. Zilio, “Saturation effects in Z-scan measurements,”Jpn. J. Appl. Phys. 35, 2649–2652 (1996). [CrossRef]
  14. S. M. Lima, H. Jiao, L. A. O. Nunes, and T. Catunda, “Nonlinear refraction spectroscopy in resonance with laser lines in solids,” Opt. Lett. 27, 845–847 (2002). [CrossRef]
  15. V. Pilla, P. R. Impinnisi, and T. Catunda, “Measurement of saturation intensities in ion doped solids by transient nonlinear refraction,” Appl. Phys. Lett. 70, 817–819 (1997). [CrossRef]
  16. M. Traiche, T. Godin, M. Fromager, R. Moncorge, T. Catunda, E. Cagniot, and K. Ait-Ameur, “Pseudo-nonlinear and athermal lensing effects on transverse properties of Cr3+ based solid-state lasers,” Opt. Commun. 284, 1975–1981 (2011). [CrossRef]
  17. S. C. Weaver and S. A. Payne, “Determination of excited-state polarizabilities of Cr3+ doped materials by degenerate 4-wave mixing,” Phys. Rev. B 40, 10727–10740 (1989). [CrossRef]
  18. R. C. Powell and S. A. Payne, “Dispersion effects in 4-wave-mixing measurements of ions in solids,” Opt. Lett. 15, 1233–1235 (1990). [CrossRef]
  19. L. J. Andrews, S. M. Hitelman, M. Kokta, and D. Gabbe, “Excited-state absorption of Cr3+ in K2NaScF6 and Gd3Ga2Ga3O12, Gd3Ga2Al3O12,” J. Chem. Phys. 84, 5229–5238 (1986). [CrossRef]
  20. P. Le Boulanger, J. L. Doualan, S. Girard, J. Margerie, and R. Moncorge, “Excited-state absorption spectroscopy of Er3+-doped Y3Al5O12, YVO4, and phosphate glass,” Phys. Rev. B 60, 11380–11390 (1999). [CrossRef]
  21. R. Moncorge, O. N. Eremeykin, J. L. Doualan, and O. L. Antipov, “Origin of athermal refractive index changes observed in Yb3+ doped YAG and KGW,” Opt. Commun. 281, 2526–2530 (2008). [CrossRef]
  22. J. Margerie, R. Moncorge, and P. Nagtegaele, “Spectroscopic investigation of variations in the refractive index of a Nd : YAG laser crystal: experiments and crystal-field calculations,” Phys. Rev. B 74, 235108 (2006). [CrossRef]
  23. Cronemeyer Dc, “Optical absorption characteristics of pink ruby,” J. Opt. Soc. Am. 56, 1703–1705 (1966). [CrossRef]
  24. D. M. Dodd, D. L. Wood, and R. L. Barns, “Spectrophotometric determination of chromium concentration in ruby,” J. Appl. Phys. 35, 1183–1186 (1964). [CrossRef]
  25. T. H. Maiman, R. H. Hoskins, I. J. Dhaenens, C. K. Asawa, and V. Evtuhov, “Stimulated optical emission in fluorescent solids. 2. spectroscopy and stimulated emission in ruby,” Phys. Rev. 123, 1151–1157 (1961). [CrossRef]
  26. S. Sugano, Y. Tanabe, and H. Kamimura, Multiplets of Transition-Metal Ions in Crystals (Academic, 1970).
  27. W. M. Fairbank, G. K. Klauminzer, and A. L. Schawlow, “Excited-state absorption in ruby, emerald, and Mgo double-bond Cr3+,” Phys. Rev. B 11, 60–76 (1975). [CrossRef]
  28. T. Kushida, “Absorption and emission properties of optically pumped ruby,” IEEE J. Quantum Electron. 2, 524–531 (1966). [CrossRef]
  29. J. W. Huang and H. W. Moos, “Absorption spectrum of optically pumped Al2O3:Cr3+,” Phys. Rev. 173, 440–444(1968). [CrossRef]
  30. E. Loh, “Ultraviolet absorption and excitation spectrum of ruby and sapphire,” J. Chem. Phys. 44, 1940–1945 (1966). [CrossRef]
  31. H. H. Tippins, “Charge-transfer spectra of transition-metal ions in corundum,” Phys. Rev. B 1, 126–135 (1970). [CrossRef]
  32. B. Di-Bartolo, Optical Interactions in Solids (Wiley, 1968).
  33. B. Struve, G. Huber, V. V. Laptev, I. A. Shcherbakov, and E. V. Zharikov, “Tunable room-temperature cw laser action in Cr3+:GdScGa-Garnet,” Appl. Phys. B 30, 117–120 (1983). [CrossRef]
  34. W. F. Krupke, M. D. Shinn, J. E. Marion, J. A. Caird, and S. E. Stokowski, “Spectroscopic, optical, and thermomechanical properties of neodymium-doped and chromium-doped gadolinium scandium gallium garnet,” J. Opt. Soc. Am. B 3, 102–114(1986). [CrossRef]
  35. M. Sheikbahae, A. A. Said, and E. W. Van Stryland, “High-sensitivity, single-beam n2 measurements,” Opt. Lett. 14, 955–957 (1989). [CrossRef]
  36. C. Jacinto, D. N. Messias, A. A. Andrade, S. M. Lima, M. L. Baesso, and T. Catunda, “Thermal lens and Z-scan measurements: thermal and optical properties of laser glasses—a review,” J. Non-Cryst. Solids 352, 3582–3597 (2006). [CrossRef]
  37. D. N. Messias, T. Catunda, J. D. Myers, and M. J. Myers, “Nonlinear electronic line shape determination in Yb3+ doped phosphate glass,” Opt. Lett. 32, 665–667 (2007). [CrossRef]
  38. L. C. Oliveira and S. C. Zilio, “Single-beam time-resolved Z-Scan measurements of slow absorbers,” Appl. Phys. Lett. 65, 2121–2123 (1994). [CrossRef]
  39. E. Strauss, “Bulk and local elastic relaxation around optically-excited centers,” Phys. Rev. B 42, 1917–1921 (1990). [CrossRef]
  40. H. Eilers, E. Strauss, and W. M. Yen, “Photoelastic effect in Ti3+doped sapphire,” Phys. Rev. B 45, 9604–9610 (1992). [CrossRef]
  41. R. Soulard, R. Moncorge, A. Zinoviev, K. Petermann, O. Antipov, and A. Brignon, “Nonlinear spectroscopic properties of Yb3+ doped sesquioxides Lu2O3 and Sc2O3,” Opt. Express 18, 11173–11180 (2010). [CrossRef]

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