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Optics Express

  • Editor: Michael Duncan
  • Vol. 14, Iss. 24 — Nov. 27, 2006
  • pp: 11715–11720
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Cubic parametric frequency generation in rutile single crystal

Fabien Gravier and Benoît Boulanger  »View Author Affiliations


Optics Express, Vol. 14, Issue 24, pp. 11715-11720 (2006)
http://dx.doi.org/10.1364/OE.14.011715


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Abstract

We experimentally investigated third harmonic generation in TiO2 rutile single crystal, including phase-matching and cubic nonlinearity. We refined the dispersion equations of rutile and we demonstrated that this crystal allows angular non critical phase-matching at useful wavelengths, with a figure of merit 7.5 times that of KTiOPO4. The measured cubic non linear coefficient and the corresponding Miller coefficients are : χ16=5.0×10-21 m2/V2 at 613.2 nm and Δ16=3.5×10-24 m2/V2. These results are used to predict the phase-matching conditions and the efficiency of triple photon generation in rutile.

© 2006 Optical Society of America

The measurement of three-photon quantum correlation requires one to perform efficient thirdorder nonlinear interactions, like third harmonic generation (THG) or triple photon generation (TPG). Both of these interactions were recently performed with success by using phasematching in KTiOPO4 (KTP): a THG conversion efficiency of 2.5% was obtained [1

1. J. P. Fève, B. Boulanger, and Y. Guillien, “Efficient energy conversion for cubic third-harmonic generation that is phase-matched in KTiOPO4,” Opt. Lett. 25, 1373–1375 (2000). [CrossRef]

], and the first experiment of TPG, stimulated by two photons, was demonstrated, leading to 3.34×1013 triple photons/pulse [2

2. J. Douady and B. Boulanger, “Experimental demonstration of a pure third-order optical parametric downconversion process,” Opt. Lett. 29, 2794–2796 (2004). [CrossRef] [PubMed]

]. Despite these good results, KTP is probably not the best material for the purpose: owing to the absence of inversion center, the cubic interactions can be polluted by quadratic cascading processes, with contributions of about 10% for the THG and 0.5 % for the TPG mentioned above [1

1. J. P. Fève, B. Boulanger, and Y. Guillien, “Efficient energy conversion for cubic third-harmonic generation that is phase-matched in KTiOPO4,” Opt. Lett. 25, 1373–1375 (2000). [CrossRef]

, 3

3. J. Douady and B. Boulanger, “Calculation of quadratic cascading contributions associated with a phasematched cubic frequency difference generation in a KTiOPO4,” J. Opt. A: Pure and Applied Optics 7, 467–471 (2005). [CrossRef]

], and the magnitude of the third-order electric susceptibility χ(3) is not so high : χ11=2.32×10-21 m2/V2 and χ22=1.96×10-21 m2/V2 at 1064 nm measured by z-scan experiments [4

4. R. DeSalvo, M. Sheik-Bahae, A. A. Said, D. J. Hagan, and E. W. Van Stryland, “Z-scan measurements of the anisotropy of nonlinear refraction and absorption in crystals,” Opt. Lett. 18, 194–196 (1993). [CrossRef] [PubMed]

]; χ24=1.46×10-21 m2/V2 at 539 nm and χ16=0.80×10-21 m2/V2 at 491 nm determined by THG [5

5. B. Boulanger, J. P. Fève, P. Delarue, I. Rousseau, and G. Marnier, “Cubic optical nonlinearities of KTiOPO4,” J. Phys. B :At. Mol. Opt. Phys. 32, 475–488 (1999). [CrossRef]

]. The identification of a better phase-matched crystal with a higher cubic nonlinearity is then an open issue for the achievement of quantum experiments.

A good candidate seems to be TiO2 rutile. It belongs to the centrosymmetric tetragonal crystal class 4/mmm and to the positive uniaxial optical class, i.e. ne>no where no and ne denote the principal ordinary and extraordinary refractive indices. The χ(3) third order electric susceptibility tensor of rutile has the four following independent elements under Kleinman symmetry [6

6. B. Boulanger, B., and J. Zyss, in International Tables for Crystallography, Vol. D : Physical Properties of Crystals, A. Authier ed., (International Union of Crystallography, Kluwer Academic Publisher, Dordrecht, Netherlands, 2003), Chap. 1.8, pp. 178–219.

]:

χxxxx=χyyyy(χ11)
χxxzz=χxzxz=χxzzx=χyyzz=χyzyz=χyzzy=χzyyz=χzyzy=χzzyy=χzxxz=χzxzx=χzzxx(χ16)
χxxyy=χxyxy=χxyyx=χyxxy=χyxyx=χyyxx(χ18)
χzzzz(χ33)
(1)

The indices x, y and z refer to the dielectric frame where the z-axis is oriented along the quaternary axis. The χij correspond to the contracted notation according to the standard convention. The third order effective coefficient magnitude ranges between 13.0×10-21m2/V2 and 16.0×10-21m2/V2 according to nonlinear index measurements performed by degenerate four-wave mixing (DFWM) or by nearly degenerate three-wave mixing (TWM) methods respectively [7

7. V. Vogel, M. J. Weber, and D. M. Krol, “Nonlinear optical phenomena in glass,” Phys. Chem. Glasses 32, 231 (1991).

, 8

8. R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refractive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989). [CrossRef]

], and according to non phase-matched THG [9

9. T. Hashimoto, T. Yoko, and S. Sakka, “Sol-Gel preparation and third-order nonlinear optical properties of TiO2 thin films,” Bull. Chem. Soc. Jpn 67, 653–660 (1994). [CrossRef]

]. Furthermore rutile exhibits phase-matching: the THG ω(e)+ω(e)+ω(e)→3ω(o), where ω(o) and ω(e) denote the circular frequencies of the ordinary and extraordinary waves respectively, was investigated in a (110) oriented plate, which lead to the determination of the phase-matching angle corresponding to a fundamental wavelength of λω=1900 nm [10

10. T. Hashimoto and T. Yoko, “Phase matching of rutile single crystal,” Appl. Phys. Lett. 68, 2478–2479 (1996). [CrossRef]

].

The present work deals with a quantitative investigation of collinear phase-matched third order parametric interactions in a TiO2 rutile single crystal involving two ordinary waves (o) and two extraordinary waves (e) : the THG [ω(e)+ω(e)+ω(o)→3ω(o)] and the TPG [ω4(o)→ω1(e)+ω2(e)+ω3(o)]. Collinear phase-matching corresponds to Δk=0 where the mismatch parameter Δk, is defined as:

Δk=ko(ωa)ke(ωb)ke(ωc)ko(ωc)
(2)

with (ωa, ωb, ωc, ωd)=(3ω, ω, ω, ω) for THG and (ωa, ωb, ωc, ωd)=(ω4, ω1, ω2, ω3) for TPG; ko,ei)=[ωi/c] no,ei) are the wave vectors where no,e correspond to the ordinary and extraordinary refractive indices in the considered direction of propagation. The associated effective coefficient is given by [6

6. B. Boulanger, B., and J. Zyss, in International Tables for Crystallography, Vol. D : Physical Properties of Crystals, A. Authier ed., (International Union of Crystallography, Kluwer Academic Publisher, Dordrecht, Netherlands, 2003), Chap. 1.8, pp. 178–219.

]:

χeff=i,j,k,l[eio(ωa).eje(ωb).eke(ωc).elo(ωd)]χijkl(ωa)
(3)

The indices i, j, k and l refer to the dielectric frame (x, y, z). eαβ , with α=(i, j, k, l) and β=(o,e), is the α Cartesian coordinate of the unit vector of the ordinary (o) or extraordinary (e) electric field. χ ijkl refers to the third order nonlinear coefficients given by (1).

We performed THG measurements on a 1mm-thick (100) rutile crystal provided by MTI Corporation. A Continuum Panther OPO pumped by a tripled Nd:YAG laser (10-Hz repetition-rate, 5-ns half-width at 1/e2) and tuneable from 400 nm to 2400 nm, is used as the fundamental beam for the THG experiments. The beam is focused with a 10-mm-focal length in the rutile plate. The optimization of the THG conversion efficiency is made by adjusting the polarization of the fundamental wave with an achromatic half wave plate, and by translating the crystal with respect to the fundamental beam waist. A collecting lens that is placed behind the crystal allows the emergent beams to be focused on a prism. The third harmonic (TH) beam is separated from the non converted fundamental by the prism and a long-wavelength rejection filter. The TH power is measured with a silicon detector and the corresponding wavelength is determined by using a Chromex 250SM monochromator. The THG fundamental wavelength, corresponding to the maximum of the THG conversion efficiency, is measured at λωPM=1839.6 nm. Calculations made from available dispersion equations of rutile lead to smaller values of λωPM, which ranges between 1752 nm and 1794 nm [11–13

11. J. R. DeVore, “Refractive indexes of rutile and spharelite,” J. Opt. Soc. Am. 41, 416 (1951). [CrossRef]

]. We refined the dispersion equations of the ordinary and extraordinary principal refractive indices of rutile by taking into account our phase-matching measurement. We found the following equations:

no2(λ)=6.0125+0.20136λ20.101460.05072λ2
ne2(λ)=7.07355+0.29834λ20.07957
(4)

The measured spectral acceptance (full width of the tuning curve at 0.405 of the maximum) is L.Δλω=0.47nm.cm, as shown in Fig. 1 where the normalized TH intensity I(ξ)/I(ξPM) is plotted as a function of the fundamental wavelength ξ=λω from either side of the phasematching fundamental wavelength ξPM=λωPM=1839.6 nm.

Fig. 1. Normalized generated third harmonic intensity as a function of the fundamental wavelength around phase-matching. The squares are the experimental data and the line is the calculation from the refined dispersion equations of the principal refractive indices.

As shown in Fig. 1, there is a good agreement between the measurement and the calculation from the dispersion Eq. (4) and the following general expression :

I3ω(ξ)I3ω(ξPM)=sinc2(Δk(ξ)L2)
(5)

where L is the crystal length, ξ is the dispersive parameter, and Δk is the mismatch parameter given by Eq. (2).

The fundamental wavelength being kept maintained at the phase-matching value λωPM, the rutile plate is then rotated on it-self around the y-axis of the dielectric frame (x, y, z) in order to determine the θ angular acceptance associated with the phase-matching direction [100], i.e. the x-axis with the spherical coordinates θ=90° and ϕ=0°: the measured angular acceptance is equal to L.Δθ=0.42°.cm as shown in Fig. 2; it is close to the theoretical value calculated with relation (5), where ξ=θ and ξPM=90°, and with the dispersion Eq. (4). Note that L.Δϕ is infinite because rutile is an uniaxial crystal.

Fig. 2. Normalized generated third harmonic intensity as a function of the direction of propagation : θ is the angle between the z-axis and the x-axis of the dielectric frame (x,y,z). The squares are the experimental data and the line is the calculation from the refined dispersion equations of the principal refractive indices.

The very good agreement between the measured and calculated angular and spectral acceptances indicates that the refined dispersion equations are valid over the concerned wavelength range on one hand, and that the whole crystal length L corresponds to the effective interaction length on the other hand. This last point is of prime importance for the determination of the effective coefficient from frequency conversion measurements.

The THG [ω(e)+ω(e)+ω(o)→3ω(o)] in rutile was compared with a THG of same type in a 1 mm-thick (100) KTP crystal phase-matched at λω=1618 nm. In the two cases, there is not spatial walk-off because the waves propagate along a principal axis of the dielectric frame. The THG energy conversion efficiencies, ηTHG=u/uω, of KTP and TiO2 are measured by using the same experimental setup; they are given in Fig. 3 as a function of the incident fundamental intensity, Iω. The measured efficiencies are weak because the considered fundamental intensities are very low, below 50 MW/cm2. For both crystals, ηTHG versus Iω exhibit a quadratic behavior as expected by the theory.

Fig. 3. Third harmonic energy conversion efficiency as a function of the fundamental intensity in a 1-mm-long TiO2 crystal and a 1-mm-long KTP crystal phase-matched along the x-axis. The squares are the experimental data and the lines correspond to the calculation.

The exact calculation of ηTHG under the plane-wave limit and the undepleted pump approximation, in the case of temporally and spatially Gaussian beams that are phase-matched in a direction without spatial and temporal walk-off gives:

ηTHG=4π293T1(ω)T2(ω)T3(ω)T4(3ω)λω2FOMIω2L2
(5)

The different Ta coefficients correspond to the Fresnel transmissions of the interacting waves, L is the crystal length, and FOM is the figure of merit expressed as:

FOM=χeff2n1(ω)n2(ω)n3(ω)n4(3ω)
(6)

χeff is the THG effective coefficient that reduces to χ16 (3ω) for TiO2 and χ24 (3ω) for KTP according to (1) and (3) for the considered phase-matching type and direction of propagation. The corresponding refractive indices are (n1, n2, n3, n4)≡(ne, ne, no, no) for TiO2 and (n1, n2, n3, n4)≡(nz, nz, ny, ny) for KTP.

Equation (5) can be applied to our experimental conditions since the Rayleigh length of the focused beam is larger than the crystal length, the walk-off angle is nil, and the group velocity dispersion is negligible in nanosecond regime. FOM of TiO2 is found to be 7.5 larger than that of KTP according to Fig. 3 and Eq. (5). Then from Eq. (6) and the magnitude of χ24 of KTP [5

5. B. Boulanger, J. P. Fève, P. Delarue, I. Rousseau, and G. Marnier, “Cubic optical nonlinearities of KTiOPO4,” J. Phys. B :At. Mol. Opt. Phys. 32, 475–488 (1999). [CrossRef]

], we find that χ16=5.0×10-21 m2/V2 for TiO2 at λ=613.2 nm. This value is smaller than those previously determined by nonlinear index measurements [7–9

7. V. Vogel, M. J. Weber, and D. M. Krol, “Nonlinear optical phenomena in glass,” Phys. Chem. Glasses 32, 231 (1991).

], which can be explained in part by the fact that the involved coefficients of the χ(3) tensor are different. The calculation of χ16 at any wavelength can be done by considering the cubic Miller coefficient Δ16, which is a non dispersive parameter given by [14

14. R. C. Miller, “Optical second harmonic generation in piezoelectric crystals,” App. Phys. Lett.5, 17–19 (1964). [CrossRef]

]:

Δ16=χ16(3ω)(ne2(ω)1)(ne2(ω)1)(no2(ω)1)(no2(3ω)1)
(7)

We find Δ16=3.5×10-24 m2/V2 from Eq. (7) and the magnitude of χ16 measured at λ=613.2nm.

Fig. 4. Calculated phase-matching curves of TPG [λ4oλ1e+λ2e+λ3o] in TiO2 rutile. The indices o and e refer to the ordinary and extraordinary polarizations respectively. The three dotted lines correspond to the situations where two wavelengths are equal. Point D corresponds to the degeneracy in wavelength, i.e. λ1e=λ2e=λ3o. Each continuous line refers to phasematching directions of equal θ angles. The points A and B are defined by the intersections between the phase-matching curves at θ=90° and the locations where λ1e=λ3o and λ2e=λ3o.

The two phase-matching areas are symmetrical according to the diagonal, where λ1e=λ2e, since these two wavelengths can be permuted due to the identity of their polarization states. Note that the value of λ3o corresponding to a given set (λ1e, λ2e) is easily obtained by using photon-energy conservation, i.e. (λ3o)-1=(λ4o)-1-(λ1e)-1-(λ2e)-1. The two phase-matching areas are formed by a framework of curves, each of them corresponding to a given phasematching angle. The locations where λ3o=λ1e and λ3o=λ2e given in Fig. 4 allow us to identify two interesting situations that are marked out by the two symmetrical points A and B: they correspond to the equivalent triple states [λ1e=2940 nm, λ2e=830 nm, λ3o=2940 nm], and [λ1e=830 nm, λ2e=2940 nm, λ3o=2940 nm], respectively. These schemes are relevant from the experimental point of view because the spatial walk-off is nil and they facilitate the necessary stimulation of the TPG, by two photons, as previously demonstrated in the case of KTP [2

2. J. Douady and B. Boulanger, “Experimental demonstration of a pure third-order optical parametric downconversion process,” Opt. Lett. 29, 2794–2796 (2004). [CrossRef] [PubMed]

]: the double injection in TiO2 can be done at a single wavelength, i.e. at 2940 nm, in the ordinary and extraordinary polarizations states. In this situation and according to the magnitude of FOM of TiO2 compared with that of KTP, it is possible to expect more than 1014 triple photons per pulse for few tenths of GW/cm2 and a crystal length of 10 mm, which is suited to correlation measurements [15

15. I. Abram, R. K. Raj, J. L. Oudar, and G. Dolique, “Direct observation of the second-order coherence of parametrically generated light,” Phys. Rev. Lett. 57 (20), 2516–2519 (1986). [CrossRef] [PubMed]

].

Acknowledgments

The authors whish to thank Martin M. Fejer from Stanford University for stimulating discussions.

References and links

1.

J. P. Fève, B. Boulanger, and Y. Guillien, “Efficient energy conversion for cubic third-harmonic generation that is phase-matched in KTiOPO4,” Opt. Lett. 25, 1373–1375 (2000). [CrossRef]

2.

J. Douady and B. Boulanger, “Experimental demonstration of a pure third-order optical parametric downconversion process,” Opt. Lett. 29, 2794–2796 (2004). [CrossRef] [PubMed]

3.

J. Douady and B. Boulanger, “Calculation of quadratic cascading contributions associated with a phasematched cubic frequency difference generation in a KTiOPO4,” J. Opt. A: Pure and Applied Optics 7, 467–471 (2005). [CrossRef]

4.

R. DeSalvo, M. Sheik-Bahae, A. A. Said, D. J. Hagan, and E. W. Van Stryland, “Z-scan measurements of the anisotropy of nonlinear refraction and absorption in crystals,” Opt. Lett. 18, 194–196 (1993). [CrossRef] [PubMed]

5.

B. Boulanger, J. P. Fève, P. Delarue, I. Rousseau, and G. Marnier, “Cubic optical nonlinearities of KTiOPO4,” J. Phys. B :At. Mol. Opt. Phys. 32, 475–488 (1999). [CrossRef]

6.

B. Boulanger, B., and J. Zyss, in International Tables for Crystallography, Vol. D : Physical Properties of Crystals, A. Authier ed., (International Union of Crystallography, Kluwer Academic Publisher, Dordrecht, Netherlands, 2003), Chap. 1.8, pp. 178–219.

7.

V. Vogel, M. J. Weber, and D. M. Krol, “Nonlinear optical phenomena in glass,” Phys. Chem. Glasses 32, 231 (1991).

8.

R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refractive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989). [CrossRef]

9.

T. Hashimoto, T. Yoko, and S. Sakka, “Sol-Gel preparation and third-order nonlinear optical properties of TiO2 thin films,” Bull. Chem. Soc. Jpn 67, 653–660 (1994). [CrossRef]

10.

T. Hashimoto and T. Yoko, “Phase matching of rutile single crystal,” Appl. Phys. Lett. 68, 2478–2479 (1996). [CrossRef]

11.

J. R. DeVore, “Refractive indexes of rutile and spharelite,” J. Opt. Soc. Am. 41, 416 (1951). [CrossRef]

12.

J. Rams, A. Tejeda, and J. M. Cabrera, “Refractive indices of rutile as a function of temperature and wavelength,” J. Appl. Phys. 82, 994 (1997). [CrossRef]

13.

Data from Almaz Optics, Inc., http://www.almazoptics.com/TiO2.htm.

14.

R. C. Miller, “Optical second harmonic generation in piezoelectric crystals,” App. Phys. Lett.5, 17–19 (1964). [CrossRef]

15.

I. Abram, R. K. Raj, J. L. Oudar, and G. Dolique, “Direct observation of the second-order coherence of parametrically generated light,” Phys. Rev. Lett. 57 (20), 2516–2519 (1986). [CrossRef] [PubMed]

OCIS Codes
(190.2620) Nonlinear optics : Harmonic generation and mixing
(190.4400) Nonlinear optics : Nonlinear optics, materials

ToC Category:
Nonlinear Optics

History
Original Manuscript: July 21, 2006
Revised Manuscript: September 15, 2006
Manuscript Accepted: September 20, 2006
Published: November 27, 2006

Citation
Fabien Gravier and Benoît Boulanger, "Cubic parametric frequency generation in rutile single crystal," Opt. Express 14, 11715-11720 (2006)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-14-24-11715


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References

  1. J. P. Fève, B. Boulanger, and Y. Guillien, "Efficient energy conversion for cubic third-harmonic generation that is phase-matched in KTiOPO4," Opt. Lett. 25, 1373-1375 (2000). [CrossRef]
  2. J. Douady and B. Boulanger, "Experimental demonstration of a pure third-order optical parametric downconversion process," Opt. Lett. 29, 2794-2796 (2004). [CrossRef] [PubMed]
  3. J. Douady and B. Boulanger, "Calculation of quadratic cascading contributions associated with a phase-matched cubic frequency difference generation in a KTiOPO4," J. Opt. A: Pure and Applied Optics 7, 467-471 (2005). [CrossRef]
  4. R. DeSalvo, M. Sheik-Bahae, A. A. Said, D. J. Hagan and E. W. Van Stryland, "Z-scan measurements of the anisotropy of nonlinear refraction and absorption in crystals," Opt. Lett. 18, 194-196 (1993). [CrossRef] [PubMed]
  5. B. Boulanger, J. P. Fève, P. Delarue, I. Rousseau, and G. Marnier, "Cubic optical nonlinearities of KTiOPO4," J. Phys. B : At. Mol. Opt. Phys. 32, 475-488 (1999). [CrossRef]
  6. B. Boulanger, B. and J. Zyss, in International Tables for Crystallography, Vol. D : Physical Properties of Crystals, A. Authier, ed., (International Union of Crystallography, Kluwer Academic Publisher, Dordrecht, Netherlands, 2003), Chap. 1.8, pp. 178-219.
  7. V. Vogel, M. J. Weber, and D. M. Krol, "Nonlinear optical phenomena in glass," Phys. Chem. Glasses 32, 231 (1991).
  8. R. Adair, L. L. Chase, and S. A. Payne, "Nonlinear refractive index of optical crystals," Phys. Rev. B 39, 3337-3350 (1989). [CrossRef]
  9. T. Hashimoto, T. Yoko and S. Sakka, "Sol-Gel preparation and third-order nonlinear optical properties of TiO2 thin films," Bull. Chem. Soc. Jpn 67, 653-660 (1994). [CrossRef]
  10. T. Hashimoto and T. Yoko, "Phase matching of rutile single crystal," Appl. Phys. Lett. 68, 2478-2479 (1996). [CrossRef]
  11. J. R. DeVore, "Refractive indexes of rutile and spharelite," J. Opt. Soc. Am. 41, 416 (1951). [CrossRef]
  12. J. Rams, A. Tejeda, and J. M. Cabrera, "Refractive indices of rutile as a function of temperature and wavelength," J. Appl. Phys. 82, 994 (1997). [CrossRef]
  13. Data from Almaz Optics, Inc., http://www.almazoptics.com/TiO2.htm.
  14. R. C. Miller, "Optical second harmonic generation in piezoelectric crystals," Appl. Phys. Lett. 5, 17-19 (1964). [CrossRef]
  15. I. Abram, R. K. Raj, J. L. Oudar, and G. Dolique, "Direct observation of the second-order coherence of parametrically generated light," Phys. Rev. Lett. 57, 2516-2519 (1986). [CrossRef] [PubMed]

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