Correlation between photorefractive index changes and optical
Transcription
Correlation between photorefractive index changes and optical
Correlation between photorefractive index changes and optical damage thresholds in z-cut proton-exchanged-LiNbO3 waveguides F. Luedtke1,*, J. Villarroel2, A. García-Cabañes2, K. Buse1, and M. Carrascosa2 2 1 Physikalisches Institut, Universitaet Bonn, 53115 Bonn, Germany Departamento de Física de Materiales C-IV, Universidad Autónoma de Madrid, Campus Cantoblanco, E-28049 Madrid, España * Corresponding author: [email protected] Abstract: An interferometric Mach-Zehnder technique very recently developed has been applied to measure photorefractive index changes in different types of z-cut proton-exchanged planar waveguides in LiNbO3. These measurements are complemented by determining the intensitythreshold for the onset of optical damage with a standard single-beam setup. In the intensity region just below the threshold-intensity obtained in the single-beam experiment the refractive index change is found to saturate at values around 1× 10−4 . Furthermore, we measure the dark conductivities of proton-exchanged waveguides by monitoring the decay of the light-induced index changes. Via the time constant of the decay we obtain dark conductivities of the order of about 5 × 10−16 Ω −1 cm −1 , that are negligible compared with the photoconductivity within the light intensity range used. The results of the measurements compare well with the predictions of a recent work, that uses a two-center model to explain the optical damage. ©2009 Optical Society of America OCIS codes: (160.5320) Photorefractive materials; (160.3730) Lithium niobate; (230.7370) Waveguides References and links 1. E. Glavas, J. M. Cabrera, and P. D. Townsend, "A comparison of optical damage in different types of LiNbO3 waveguides," J. Phys. D: Appl. Phys. 22, 611–616 (1988). 2. T. Fujiwara, X. Cao, R. Srivastava, and R.V. Ramaswamy, "Photorefractive effect in annealed protonexchanged LiNbO3 waveguides," Appl. Phys. Lett. 61, 743-745 (1992). 3. A. Alcázar-de-Velasco, J. Rams, J. M. Cabrera and F. Agulló-López, "Light-induced damage mechanisms in α-phase proton-exchanged LiNbO3 waveguides," Appl. Phys. B 68, 989–993 (1999). 4. O. Caballero-Calero, A. García-Cabañes, J. M. Cabrera, M. Carrascosa, and A. Alcázar, "Optical damage in x-cut proton exchanged LiNbO3 planar waveguides," J. Appl. Phys. 100, 093103 (2006). 5. T. Fujiwara, R. Srivastava, X. Cao, and R. V. Ramaswamy, "Comparison of photorefractive index change in proton-exchanged and Ti-diffused LiNbO3 waveguides," Opt. Lett. 18, 346–348 (1993). 6. M. Carrascosa, J. Villarroel, J. Carnicero, A. García-Cabañes, and J. M. Cabrera, "Understanding light intensity thresholds for catastrophic optical damage in LiNbO3," Opt. Express 16, 115 (2008). 7. J. Rams, A. Alcázar-de-Velasco, M. Carrascosa, J. M. Cabrera, and F. Agulló-López, "Optical damage inhibition and thresholding effects in lithium niobate above room temperature," Opt. Commun. 178, 211216 (2000) 8. I. Breunig, M. Falk, B. Knabe, R. Sowade, K. Buse, P. Rabiei, and D. H. Jundt, "Second harmonic generation of 2.6 W green light with thermoelectrically oxidized undoped congruent lithium niobate crystals below 100 °C," Appl. Phys. Lett. 91, 221110 (2007) 9. F. Luedtke, J. Villaroel, A. García-Cabañes, M. Carrascosa, H. Steigerwald, and K. Buse "Mach-Zehnder technique for investigation of optical damage in planar LiNbO3 waveguides," Ferroelectrics, in press 10. A. Méndez, A. García-Cabañes, M. Carrascosa, and J. M. Cabrera, "Photorefractive charge compensation in α-phase proton-exchanged LiNbO3 waveguides," J. Opt. Soc. Am. B 17, 1412-1419 (2000). 11. M. Falk and K. Buse, "Thermo-electric method for nearly complete oxidization of highly iron-doped lithium niobate crystals," Appl. Phys. B 81, 853–855 (2005). #104101 - $15.00 USD (C) 2009 OSA Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 658 12. J. M. Cabrera, J. Olivares, M. Carrascosa, J. Rams, R. Müller, and E. Diéguez, "Hydrogen in lithium niobate," Adv. Phys. 45, 349-392 (1996) 13. O. Caballero-Calero, A. García-Cabañes, J. M. Cabrera, M. Carrascosa, and A. Alcázar, "Light intensity measurements in optical wavegudies using prism couplers," J. Appl. Phys. 102, 074509 (2007). 14. F. Agulló-López, G.F. Calvo, and M. Carrascosa, Photorefractive Materials and their Applications 1 – Basic Effects, P. Günter and J.-P. Huignard, ed. (Springer, 2005), Chap. 3. 15. J. Villarroel, M. Carrascosa, A. García-Cabañes, and J. M. Cabrera, "Light intensity dependence of holographic response and dark decays in α-phase PE:LiNbO3 waveguides," J. Opt. A: Pure Appl. Opt. 10, 104008 (2008). 16. A. Mansingh and A. Dhar, "The AC conductivity and dielectric constant of lithium niobate single crystals," J. Phys. D: Appl. Phys. 18, 2059-2071 (1985). 17. O. Althoff and E. Krätzig, ''Strong light-induced refractive index changes in LiNbO3,'' Nonlinear Optical Materials III, SPIE 1273, 12-19 (1990). 18. F. Jermann and J. Otten, ''Light-induced charge transport in LiNbO3:Fe at high light intensities,'' J. Opt. Soc. Am. B 10, 2085-2092 (1993). 19. M. Falk, Th. Woike, and K. Buse, "Reduction of optical damage in lithium niobate crystals by thermoelectric oxidization," Appl. Phys. Lett. 90, 251912 (2007). 20. J. Carnicero, M. Carrascosa, A. Mendez, A. García-Cabañes, and J. M. Cabrera, "Optical damage control via the Fe2+/Fe3+-ratio in proton-exchanged LiNbO3 waveguides," Opt. Lett. 32, 2294-2296 (2007). 1. Introduction Photorefractive optical damage in lithium niobate (LiNbO3) waveguides continues to be a crucial problem for applications at light powers above 10 mW. Although great effort has been devoted to characterize [1, 2, 3, 4], understand [5, 6] and reduce [7, 8] optical damage, many experimental and theoretical aspects remain open, and the definite method for optical damage inhibition is still lacking. For the development of even more efficient methods of optical damage reduction a reliable and well-understood model of the effect is desired. So far it is unclear which index changes Δn are acceptable, i.e. do not cause critical beam distortions, and which values are unacceptable. Also more information is needed about the origin of the Δn , in particular the role of secondary centers and of the dark conductivity deserve special attention. To work on these tasks we take advantage of an interferometric technique we developed for the measurement of the refractive index change in planar waveguides. The method is described in detail in [9]. The main advantage of this technique is that, compared to holographic approaches [10], it measures the change of the effective mode index Δneff for single-beam propagation, the case more appropriate to investigate optical damage. Moreover, it is applicable to z-cut guides for which very scarce measurements of Δneff have been reported because, the z-axis being normal to the guide plane, the typical holographic method fails. In this work we study planar proton-exchanged (PE) waveguides. The obtained data for Δneff will be related to complementary measurements of the intensity threshold for the onset of beam distortion, thus getting more complete information about optical damage. Furthermore, we study the dark conductivity in these waveguides. 2. Experimental Methods 2.1 Sample preparation Three different z-cut LiNbO3 substrates have been used: congruently melting undoped, congruently melting thermo-electrically oxidized [11], and 5.0 % mol Mg-doped material. Every sample undergoes the same treatment of immersion for 24 h at 300 °C in benzoic acid buffered with 3 wt. % lithium benzoate in a sealed glass ampoule [10]. This procedure results in formation of α-phase proton-exchanged LiNbO3 (PE:LiNbO3) waveguides with extraordinary index jumps at the surface of Δne ≈ 0.01 and smooth Fermi-like index-profiles with effective depths in the 1-2 µm range [10]. These guides support one or two modes at the #104101 - $15.00 USD (C) 2009 OSA Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 659 wavelengths 532 and 633 nm. One of the edges of each sample is polished to optical grade in order to enable decoupling of light via the waveguide edge in the interferometer setup described below. Slight differences with respect to the waveguide fabrication are noticed between the different substrates. Both, the waveguides in the thermo-electrically oxidized substrate and in the magnesium-doped substrate tend to guide rather one than two modes at the two wavelengths mentioned above. For magnesium-doped LiNbO3 it is known that the protonexchange process is slower than in undoped material [12]. 2.2 Determination of the threshold intensity for beam degradation In order to measure the threshold intensity for the onset of appreciable distortion of the outcoupled light we use a simple setup schematically shown in Fig. 1 and described in [3]. While continuously illuminating the waveguide with light at λ = 532 nm, the output power passing through a diaphragm placed 30 cm behind the waveguide is monitored. The size of the diaphragm is chosen such, that at low intensities (no light-induced scattering) about 70% of the total out-coupled power is transmitted. The light intensity inside the waveguide has been estimated (to a ±15% accuracy) by following the procedure described in [13]. Nd:YAG laser 532 nm Powermeter 2 Powermeter 1 Polarizer Photodetector 1 (total power) Photodetector 2 and diaphragm Prisms Lens f = 300 mm 10 mm Beam splitter Waveguide sample Fig. 1. Schematic sketch of the single-beam setup that is used for the determination of optical damage thresholds via the detection of significant beam distortion. 2.3 Measuring optical damage with the interferometric method The interferometric technique for characterizing the optical damage in waveguides is based on the measurement of relative phase changes between two weak He-Ne laser beams that propagate along the two arms of a Mach-Zehnder interferometer (Fig. 2). The key feature of the setup is the fact that both interferometer beams (represented in Fig. 2 by a dotted and a dashed line, respectively) propagate separately, but next to each other in the same planar waveguide. Thus, the setup is insensitive to changes of the external parameters, such as the ambient temperature, since both interferometer arms are equally influenced. Optical damage is induced in one of the arms by intense collinear illumination with visible light (532 nm in our case). The probe beam and the pump beam interact over the whole propagation length from the incoupling prism to the end face of the waveguide. The measured quantity is the modulation of the red light-intensity pattern at the output of the interferometer. The use of chopped probe light and a lock-in amplifier enable us to detect changes in the interference pattern with a high signal-to-noise ratio. Our realization of the Mach-Zehnder interferometer #104101 - $15.00 USD (C) 2009 OSA Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 660 in planar waveguides together with its features and limitations have been previously described in [9]. HeNe laser, 633 nm Nd:YAG laser, 532 nm Lock-in amplifier and recorder Collimation optics Crossed polarizers Reference frequency Diaphragm Chopper Microscope objective Mirror Mirror Beam splitter and mirror Mirror Beam splitter Prisms } Lens f = 400 mm Waveguide sample on thermally stabilized mount Microscope objective Mirror Diaphragm, bandpass filter (633 nm) and photodetector Fig. 2. Experimental setup for the interferometric measurement of photorefractive index changes in planar waveguides. The dashed and the dotted lines on the lower left-hand side represent the two arms of the interferometer. These two lines are separated in the direction perpendicular to the plane of the paper. The experimental procedure is as follows: With the green beam blocked, the coupling angles for the weak red beams are adjusted to the best interference signal. Afterwards, the coupling angle for the green beam is adjusted at very low in-coupled power to avoid optical damage before the actual measurement starts. Then, with the red beam going through and a green blocking-filter placed in front of the detector, the green intensity is increased up to the value the measurement is supposed to be conducted with. The measuring time starts when the shutter for the green light is opened. Depending on the in-coupled intensity, and therefore on the expected rise time of the photorefractive effect, the modulated intensity is recorded for a few minutes up to one hour. In order to compare the relative importance of dark and photoconductivity, we have also studied dark decays of previously recorded effective index changes ( ≈ 10−4 ). In this case, the measuring time starts when the green shutter is closed. In order to determine the dark conductivity σd from these decay measurements, it is necessary to decrease the intensity of the red probe light to be sure that the induced optical erasure is negligible compared with σ d ( I red ≈ 0.05 Wcm −2 inside the waveguide). Doubling of the probe intensity does not accelerate the decay, ensuring that the 0.05 Wcm −2 are small enough to monitor purely the dark relaxation. Since these dark decays are much slower than the production of optical damage upon illumination, the typical measurement times here are several hours. All measurements described in this section are performed with the temperature of the sample holder being stabilized to ( 25.0 ± 0.1 ) °C. #104101 - $15.00 USD (C) 2009 OSA Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 661 3. Experimental results 3.1 Single-beam setup The results of the measurements of the threshold intensity are summarized in Fig. 3. As long as the in-coupled beam does not cause appreciable optical damage in the guiding layer, the out-coupled beam maintains its shape and the power detected behind the diaphragm is proportional to the in-coupled power. The loss of this proportionality marks the threshold intensity for the onset of optical damage. It can be seen in Fig. 3 that the waveguides on the congruent substrate, either untreated or thermoelectrically oxidized, exhibit very similar thresholds around 270 Wcm −2 . This value is a little higher than the threshold intensity I thr measured for the same type of waveguide (i.e. produced by the same fabrication procedure) and with the same experimental method, but fabricated in x-cut congruent substrates ( I thr ≈ 100 Wcm −2 ) [4]. In the Mg-doped sample no significant degradation of the out-coupled beam could be measured up to the highest intensity available, 105 Wcm −2 . The threshold intensities I thr for all the samples used can be found in Table 1. The criterion that we apply to determine I thr is as follows: I thr is the intensity where for the first time the derivative dI out / dI in is smaller than 0.15. This value is arbitrarily chosen, but the result is in good accordance with the intuitive impression given by Fig. 3, thus it provides a reasonable criterion for quantitative comparison of different waveguides. 105 Iout / Wcm-2 104 103 102 101 100 100 101 102 103 -2 Iin / Wcm 104 105 Fig. 3. Results of the measurements with the single-beam setup: outcoupled intensity Iout versus incoupled intensity Iin Table 1. Intensity thresholds for the different types of waveguides I thr [Wcm −2 ] Sample undoped, untreated, z-cut 260 undoped, oxidized, z-cut 280 MgO-doped, z-cut #104101 - $15.00 USD (C) 2009 OSA > 10 5 Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 662 3.2 Mach-Zehnder interferometer In the standard photorefractive model [14], the time dependence of Δneff (t ) involves a saturating exponential function as follows: Δneff (t ) = Δneff , sat (1 − e−t / τ ) , (1) where Δneff , sat is the effective index change at saturation and τ is the rise time. This dependence is valid for our data (see the fit in Fig. 4(a)). Beyond the threshold intensity for significant beam distortion, the interferometric method becomes problematic. This is because, due to increasing beam divergence, the intensity inside the waveguide is no longer well defined. We measure the development of the change of the effective mode index with time, Δneff (t ) , for all types of waveguides guides (see Section 2) for an intensity range of 10 – 2000 Wcm −2 . From the interferometer signals we extract the time evolution of the refractive index changes as described in [9]. Thus we obtain values for the saturation index change Δneff , sat and the rise constant τ−1 as functions of the intensity inside the waveguide. With regard to τ−1 , it turns out to be of the same order of magnitude as those values obtained by the holographic method for congruent samples [15]. Fig. 4. Typical measurement results obtained with the Mach-Zehnder interferometer for the build-up (a) and dark-decay (b) of optical damage. The solid lines correspond to exponential fits of Eq. (1) and Eq. (2), respectively. The dependence of Δneff , sat on the intensity has been plotted in Fig. 5 for all the guides. All curves show an increase of Δneff , sat with the light intensity I inside the waveguide that seems to saturate for higher intensities. In the low-intensity-region (< 60 Wcm −2 ) the curves appear to have also a lower sensitivity to the variation of light intensity. In accordance with the behavior present in Fig. 3, the thermo-electrically oxidized and the congruent guides exhibit very similar Δneff , sat ( I ) . It is worthwhile noticing that the intensity thresholds from Fig. 3 roughly coincide with the region in which Δneff , sat seems to saturate with I. Finally, for the MgO-doped samples, the measured index changes are too small to detect a reliable Δneff , sat increase within the intensity range used, in agreement with the much higher intensity threshold seen in Fig. 3. Since the competition of dark conductivity σd and photoconductivity σ ph in photorefractive charge transport was often used in early papers [5] to explain dependences similar to that of Fig. 5, we have also measured the dark decay time of Δneff in order to determine σ d . In analogy to Eq. (1), we expect the decay of the index change to behave like Δneff (t ) = Δneff (t = 0)e −t / τd , #104101 - $15.00 USD (C) 2009 OSA (2) Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 663 where τd is the time constant of the dark decay. It is connected to the dark conductivity via τd = εε0 . σd (3) In Eq. (3), ε0 and ε are the vacuum permittivity and the relative permittivity, respectively. We take ε ≈ 27 [16] to calculate σd from the measured decay times. These are Δneff, sat / 10-4 typically in the range of a few 1000 s (corresponding to σd of a few 10−16 Ω −1 cm −1 ). Comparing this to the optical damage rise-time of a few seconds, it becomes unambiguously clear that the dark conductivity plays no role for the suppression of optical damage for our experimental conditions. An example of the measured time evolution of the index change during a dark decay is displayed in Fig. 4(b). 1.0 0.1 1 10 100 Iin / Wcm-2 1000 Fig. 5. Saturation values of the refractive index changes Δneff ,sat for all three types of waveguides versus incident light intensity Iin. Solid and dashed lines are just guides to the eye, in analogy to presentations in [6, 17, 18]. 5. Discussion The Mach-Zehnder interferometric technique applied to measure photorefractive index changes in planar waveguides has proved to be a complementary useful tool for characterizing the optical damage. First, it has confirmed previous experimental data on a strong increase of the induced saturation index change Δneff , sat at high intensities obtained by the holographic method in x-cut planar guides [15] or the Mach-Zehnder method in channel guides [5]. Also measurements of the photorefractively induced birefringence in x-cut bulk crystals with a Senarmont compensator setup showed an enhancement of Δn with I up to values of about 10−4 [19]. Moreover, comparing the results with those from the single-beam technique, it is observed that the optical damage threshold occurs when the Δneff , sat ( I ) starts to saturate. We interpret this result as follows: For low enough intensities the photorefractive index changes, independently of their possible increase with I, are too small to appreciably affect the light propagation inside the guide. For increasing intensity, Δneff , sat becomes sufficient for modifying the beam profile and generating noticeable self-defocusing along the propagation direction causing the sublinear dependence seen in Fig. 3. This should occur #104101 - $15.00 USD (C) 2009 OSA Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 664 for Δneff , sat ≈ 10−4 as shown in Fig. 5. For higher in-coupled intensities the actual intensity inside the guide can hardly increase due to the self defocusing. Hence, in our case the onset of serious beam distortion is at Δneff , sat of about 1× 10−4 . This threshold, however, may depend on several parameters like the interaction length and the beam diameter. Finally it is worth to mention that waveguides fabricated in Mg-doped substrates exhibit Δneff , sat well below 1× 10−4 even for the highest intensities used. This result is in good accordance with the absence of measurable optical damage thresholds in the intensity region checked. The dark conductivity measurements achieved with the Mach-Zehnder technique clearly indicate that its contribution to charge transport is negligible when compared with the photoconductivity. Consequently, models based the on the role of dark conductivity to explain the increase of Δneff , sat with I are not applicable, and different approaches should be invoked. Conversely, our results are in good semi-quantitative accordance with the intensity dependence for the Δneff , sat predicted based on a two-center model for undoped LiNbO3 applied to α-phase waveguides [6]. In particular, Δneff starts to grow sharply at similar light intensities. In this model the intensity dependence of Δneff , sat is attributed to the increasing importance of the highly bulk photovoltaic defect of niobium on lithium lattice sites (NbLi) in the charge transport. Regarding the different crystals used we have fabricated α-phase PE waveguides on thermoelectrically oxidized LiNbO3 substrates. Unfortunately, the PE treatment seems to alter the oxidation state of the waveguide layer so that the obtained waveguide has an optical damage resistance similar to that of standard α-phase guides. This result is indirectly a further confirmation of the conclusions of a recent work that reports a significant reduction of the samples during the PE treatment [20]. This effect should cancel the previous strong oxidation obtained by the thermoelectric technique. 6. Summary In summary, we applied the recently developed interferometric Mach-Zehnder technique for characterizing photorefractive optical damage in planar waveguides. The study of α-phase PE:LiNbO3 guides, fabricated in different z-cut substrates, has shown that the steadystate index change monotonously increases with the light intensity up to a saturating value. This last value coincides with serious beam divergence, i.e. the threshold for the onset of optical damage. Dark conductivity appears negligible compared with photoconductivity within the light intensity range used. Up to saturation, measured values compare well with results of simulations performed within the two-center model which considers the anti-site or NbLi-site defect as a secondary photorefractive center. Acknowledgments This work was supported by the Ministerio de Educación y Ciencia (MEC) under grant MEC/MAT2005-06359-C03-01. F. Luedtke acknowledges gratefully financial funding by the Deutscher Akademischer Austauschdienst (DAAD) and the Deutsche Telekom AG. and J. Villarroel acknowledges his FPI fellowship from the Spanish MEC. The authors also thank Prof. J.M. Cabrera for very useful discussions and comments. #104101 - $15.00 USD (C) 2009 OSA Received 14 Nov 2008; revised 23 Dec 2008; accepted 5 Jan 2009; published 7 Jan 2009 19 January 2009 / Vol. 17, No. 2 / OPTICS EXPRESS 665