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Optics Express

Optics Express

  • Editor: C. Martijn de Sterke
  • Vol. 18, Iss. 15 — Jul. 19, 2010
  • pp: 15597–15602
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Domain wall characterization in ferroelectrics by using localized nonlinearities

Xuewei Deng and Xianfeng Chen  »View Author Affiliations


Optics Express, Vol. 18, Issue 15, pp. 15597-15602 (2010)
http://dx.doi.org/10.1364/OE.18.015597


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Abstract

In this paper, a method of domain wall characterization in ferroelectrics through Cherenkov second harmonic generation by localized nonlinearities is proposed. By this method, domain wall width is estimated to be less than 10nm. High spatial angular resolution of about 10mrad in the experiment reveals the fine structures of the domain walls. Combined with scanning techniques, this method can reconstruct domain wall patterns with high resolution. This method has advantages of being nondestructive, noncontact, in situ as well as of high resolution.

© 2010 OSA

1. Introduction

Ferroelectric is one kind of the most important materials in nonlinear optics. In the past decade, domain engineering, which is mainly based on ferroelectrics, has attracted great attention and been widely studied, such as the fabrication and application of periodically inverted domain structures [1

1. M. M. Fejer, G. A. Magel, D. H. Jundt, and R. L. Byer, “Quasi-phase-matched second harmonic generation: tuning and tolerances,” IEEE J. Quantum Electron. 28(11), 2631–2654 (1992). [CrossRef]

]. Meanwhile, a number of detection and visualization methods have been developed to observe the domain structures, like chemical etching method [2

2. K. Nassau, H. J. Levinstein, and G. M. Loiacono, “The domain structure and etching of freeoelectric lithium niobate,” Appl. Phys. Lett. 6(11), 228–229 (1965). [CrossRef]

], optical imaging [3

3. M. Müller, E. Soergel, and K. Buse, “Visualization of ferroelectric domains with coherent light,” Opt. Lett. 28(24), 2515–2517 (2003). [CrossRef] [PubMed]

5

5. G. Fogarty, B. Steiner, M. Cronin-Golomb, U. Laor, M. H. Garrett, J. Martin, and R. Uhrin, “Antiparallel ferroelectric domains in photorefractive barium titanate and strontium barium niobate observed by high-resolution x-ray diffraction imaging,” J. Opt. Soc. Am. B 13(11), 2636–2643 (1996). [CrossRef]

] and scanning microscopy techniques [6

6. S. Zhu and W. Cao, “Direct observation of ferroelectric domains in LiTaO3 using environmental scanning electron microscopy,” Phys. Rev. Lett. 79(13), 2558–2561 (1997). [CrossRef]

9

9. M. Flörsheimer, R. Paschotta, U. Kubitscheck, C. Brillert, D. Hofmann, L. Heuer, G. Schreiber, C. Verbeek, W. Sohler, and H. Fuchs, “Second-harmonic imaging of ferroelectric domains in LiNbO3 with micron resolution in lateral and axial directions,” Appl. Phys. B 67(5), 593–599 (1998). [CrossRef]

]. Chemical etching is the most widely utilized method because of its high resolution and comparative ease of use. The disadvantage is also obvious that it is destructive. Optical imaging is comparatively simple and can be used to acquire real-time or in situ information about the domain structures, but diffraction limits the resolution. Scanning microscopy is non-destructive and of high resolution. However, it cannot give real-time information and strongly depends on the surface patterns.

In this paper, we propose a new optical method that can characterize domain walls through Cherenkov second harmonic generation (CSHG) by using localized nonlinearities. This method is not only non-destructive and in situ, but also gives domain wall information with high precision, such as wall width and orientation. Moreover, this method can be used to acquire the information of domain structures buried inside a crystal other than on the surface since it has strong response to domain walls anywhere in a transparent crystal.

2. Cherenkov second harmonic generation by localized nonlinearities in domain wall

3. Experiments and analysis

By utilizing CSHG method, we can measure the orientation of domain wall with high precision as well as the width of domain wall. Figure 3
Fig. 3 CSHG patterns which reveal the fine structures of the domain wall. The spatial angular resolution is about 10mrad.
gives a pair of CSHGs which contains the information of the fine structures of the domain wall. Since smaller numerical aperture of the focused FB can provide higher angular resolution, here the FB is still loosely focused to about 10μm on the input facet, whose small numerical aperture will provide higher angular resolution. The domain wall covered by the FB spot has tiny difference in its orientation, which can generate CSHGs with tiny angular difference. The spatial angular resolution of the CSHGs is about 10mrad. Such tiny difference of the domain wall orientation is hard to detect by other optical methods, but it can be easily visualized by CSHG method with high precision. As well, with the decreasing of the FB spot size and its divergence, the precision of measurement can be further improved. This high spatial angular resolution may be meaningful in domain engineering of fine structures.

When the domain walls’ scale is smaller than the FB spot size and the domain walls have complex patterns, CSHG method can still be used to determine the orientations of the domain walls and show a first glance at the geometry of the domain wall structures. Due to the point-group structure and the nonstoichiometry, domain inversions in LiTaO3 crystals are trigonal [15

15. D. A. Scrymgeour, V. Gopalan, A. Itagi, A. Saxena, and P. J. Swart, “Phenomenological theory of a single domain wall in uniaxial trigonal ferroelectrics: Lithium niobate and lithium tantalate,” Phys. Rev. B 71(18), 184110 (2005). [CrossRef]

]. We fabricate such trigonal micro domain inversions with averaged size of 7~8μm in the 1mm z-cut LiTaO3 sample as shown in Fig. 4(a)
Fig. 4 (a) Trigonal domain wall patterns on the + z surface of the sample; (b) corresponding CSHG patterns.
and the 10μm FB spot can coves it totally. The generated CSHGs are hexagonally distributed as shown in Fig. 4(b). They are obviously three pairs of CSHGs symmetrical to the trigonal walls respectively. Since the FB spot size does not impact the CSHG, this method is valid even when domain inversions are smaller than the FB spot. For a more complex domain wall pattern, more complex CSHGs are expected, through whose intensities we can also determine the relative importance of the domain walls. Since CSHGs are quite sensitive to domain walls, it can also be used to monitor domain inversions inside any ferroelectrics.

CSHG by localized nonlinearities has been demonstrated in a variety of ferroelectrics, such as PPKTP [12

12. A. Fragemann, V. Pasiskevicius, and F. Laurell, “Second-order nonlinearities in domain walls of periodically poled KTiOPO4,” Appl. Phys. Lett. 85(3), 375–377 (2004). [CrossRef]

], PPLN and PPLT [16

16. S. M. Saltiel, D. N. Neshev, W. Krolikowski, A. Arie, O. Bang, and Y. S. Kivshar, “Multiorder nonlinear diffraction in frequency doubling processes,” Opt. Lett. 34(6), 848–850 (2009). [CrossRef] [PubMed]

], SBN [17

17. P. Molina, M. O. Ramírez, and L. E. Bausá, “Stronitium Barium Niobate as a multifunctional two-dimensional nonlinear ‘photonic glass’,” Adv. Funct. Mater. 18(5), 709–715 (2008). [CrossRef]

] and so on. Since the localized nonlinearities should exist in domain wall regions of all ferroelectrics, this CSHG method can be used in all ferroelectrics and even other nonlinear materials with domain structures.

4. Conclusion

In conclusion, we propose a new method to characterize domain walls in ferroelectrics by using localized nonlinearities. By this method, we estimate that the width of the domain walls in LiTaO3 is less than 10nm. The symmetry of the CSHGs is used to measure the orientation of domain walls and the spatial resolution is as high as 10mrad in our experiments. It is also demonstrated that even when the measured domain inversion is smaller than the FB spot can the CSHGs reveal the information of the domain walls of such tiny domain inversions. Combined with scanning techniques, CSHG method can reconstruct the domain wall patterns with high precision. This method has advantages of nondestructive, noncontact, in situ and of high resolution. Since CSHG by localized nonlinearities exist in domain wall regions of all ferroelectrics, this method should work in general in all ferroelectrics and even some other materials with domain wall structures.

Acknowledgement

This research was supported by the National Natural Science Foundation of China (No. 60508015 and No.10574092), the National Basic Research Program “973” of China (2006CB806000), and the Shanghai Leading Academic Discipline Project (B201).

References and links

1.

M. M. Fejer, G. A. Magel, D. H. Jundt, and R. L. Byer, “Quasi-phase-matched second harmonic generation: tuning and tolerances,” IEEE J. Quantum Electron. 28(11), 2631–2654 (1992). [CrossRef]

2.

K. Nassau, H. J. Levinstein, and G. M. Loiacono, “The domain structure and etching of freeoelectric lithium niobate,” Appl. Phys. Lett. 6(11), 228–229 (1965). [CrossRef]

3.

M. Müller, E. Soergel, and K. Buse, “Visualization of ferroelectric domains with coherent light,” Opt. Lett. 28(24), 2515–2517 (2003). [CrossRef] [PubMed]

4.

S. I. Bozhevolnyi, J. M. Hvam, K. Pedersen, F. Laurell, H. Karlsson, T. Skettrup, and M. Belmonte, “Second harmonic imaging of ferroelectric domain walls,” Appl. Phys. Lett. 73(13), 1814–1816 (1998). [CrossRef]

5.

G. Fogarty, B. Steiner, M. Cronin-Golomb, U. Laor, M. H. Garrett, J. Martin, and R. Uhrin, “Antiparallel ferroelectric domains in photorefractive barium titanate and strontium barium niobate observed by high-resolution x-ray diffraction imaging,” J. Opt. Soc. Am. B 13(11), 2636–2643 (1996). [CrossRef]

6.

S. Zhu and W. Cao, “Direct observation of ferroelectric domains in LiTaO3 using environmental scanning electron microscopy,” Phys. Rev. Lett. 79(13), 2558–2561 (1997). [CrossRef]

7.

F. Augereau, G. Despaux, and P. Saint-Gr’egoire, “Imaging ferroic domain structures with an acoustic microscope: example of PPLN,” Ferroelectrics 290(1), 29–38 (2003). [CrossRef]

8.

O. Tikhomirov, B. Red’kin, A. Trivelli, and J. Levy, “Visualization of 180° domain structures in uniaxial ferroelectrics using confocal scanning optical microscopy,” J. Appl. Phys. 87(4), 1932–1936 (2000). [CrossRef]

9.

M. Flörsheimer, R. Paschotta, U. Kubitscheck, C. Brillert, D. Hofmann, L. Heuer, G. Schreiber, C. Verbeek, W. Sohler, and H. Fuchs, “Second-harmonic imaging of ferroelectric domains in LiNbO3 with micron resolution in lateral and axial directions,” Appl. Phys. B 67(5), 593–599 (1998). [CrossRef]

10.

P. K. Tien, R. Ulrich, and R. J. Martin, “Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide,” Appl. Phys. Lett. 17(10), 447–450 (1970). [CrossRef]

11.

A. Zembrod, H. Puell, and J. Giordmaine, “Surface radiation from nonlinear optical polarization,” Opt. Quantum Electron. 1(1), 64–66 (1969).

12.

A. Fragemann, V. Pasiskevicius, and F. Laurell, “Second-order nonlinearities in domain walls of periodically poled KTiOPO4,” Appl. Phys. Lett. 85(3), 375–377 (2004). [CrossRef]

13.

D. A. Scrymgeour and V. Gopalan, “Nanoscale piezoelectric response across a single antiparallel ferroelectric domain wall,” Phys. Rev. B 72(2), 024103 (2005). [CrossRef]

14.

J. Wittborn, C. Canalias, K. V. Rao, R. Clemens, H. Karlsson, and F. Laurell, “Nanoscale imaging of domains and domain walls in periodically poled ferroelectrics using atomic force microscopy,” Appl. Phys. Lett. 80(9), 1622–1624 (2002). [CrossRef]

15.

D. A. Scrymgeour, V. Gopalan, A. Itagi, A. Saxena, and P. J. Swart, “Phenomenological theory of a single domain wall in uniaxial trigonal ferroelectrics: Lithium niobate and lithium tantalate,” Phys. Rev. B 71(18), 184110 (2005). [CrossRef]

16.

S. M. Saltiel, D. N. Neshev, W. Krolikowski, A. Arie, O. Bang, and Y. S. Kivshar, “Multiorder nonlinear diffraction in frequency doubling processes,” Opt. Lett. 34(6), 848–850 (2009). [CrossRef] [PubMed]

17.

P. Molina, M. O. Ramírez, and L. E. Bausá, “Stronitium Barium Niobate as a multifunctional two-dimensional nonlinear ‘photonic glass’,” Adv. Funct. Mater. 18(5), 709–715 (2008). [CrossRef]

OCIS Codes
(160.2260) Materials : Ferroelectrics
(190.1900) Nonlinear optics : Diagnostic applications of nonlinear optics
(190.2620) Nonlinear optics : Harmonic generation and mixing
(190.4400) Nonlinear optics : Nonlinear optics, materials

ToC Category:
Nonlinear Optics

History
Original Manuscript: March 19, 2010
Revised Manuscript: May 9, 2010
Manuscript Accepted: June 7, 2010
Published: July 8, 2010

Citation
Xuewei Deng and Xianfeng Chen, "Domain wall characterization in ferroelectrics by using localized nonlinearities," Opt. Express 18, 15597-15602 (2010)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-18-15-15597


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References

  1. M. M. Fejer, G. A. Magel, D. H. Jundt, and R. L. Byer, “Quasi-phase-matched second harmonic generation: tuning and tolerances,” IEEE J. Quantum Electron. 28(11), 2631–2654 (1992). [CrossRef]
  2. K. Nassau, H. J. Levinstein, and G. M. Loiacono, “The domain structure and etching of freeoelectric lithium niobate,” Appl. Phys. Lett. 6(11), 228–229 (1965). [CrossRef]
  3. M. Müller, E. Soergel, and K. Buse, “Visualization of ferroelectric domains with coherent light,” Opt. Lett. 28(24), 2515–2517 (2003). [CrossRef] [PubMed]
  4. S. I. Bozhevolnyi, J. M. Hvam, K. Pedersen, F. Laurell, H. Karlsson, T. Skettrup, and M. Belmonte, “Second harmonic imaging of ferroelectric domain walls,” Appl. Phys. Lett. 73(13), 1814–1816 (1998). [CrossRef]
  5. G. Fogarty, B. Steiner, M. Cronin-Golomb, U. Laor, M. H. Garrett, J. Martin, and R. Uhrin, “Antiparallel ferroelectric domains in photorefractive barium titanate and strontium barium niobate observed by high-resolution x-ray diffraction imaging,” J. Opt. Soc. Am. B 13(11), 2636–2643 (1996). [CrossRef]
  6. S. Zhu and W. Cao, “Direct observation of ferroelectric domains in LiTaO3 using environmental scanning electron microscopy,” Phys. Rev. Lett. 79(13), 2558–2561 (1997). [CrossRef]
  7. F. Augereau, G. Despaux, and P. Saint-Gr’egoire, “Imaging ferroic domain structures with an acoustic microscope: example of PPLN,” Ferroelectrics 290(1), 29–38 (2003). [CrossRef]
  8. O. Tikhomirov, B. Red’kin, A. Trivelli, and J. Levy, “Visualization of 180° domain structures in uniaxial ferroelectrics using confocal scanning optical microscopy,” J. Appl. Phys. 87(4), 1932–1936 (2000). [CrossRef]
  9. M. Flörsheimer, R. Paschotta, U. Kubitscheck, C. Brillert, D. Hofmann, L. Heuer, G. Schreiber, C. Verbeek, W. Sohler, and H. Fuchs, “Second-harmonic imaging of ferroelectric domains in LiNbO3 with micron resolution in lateral and axial directions,” Appl. Phys. B 67(5), 593–599 (1998). [CrossRef]
  10. P. K. Tien, R. Ulrich, and R. J. Martin, “Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide,” Appl. Phys. Lett. 17(10), 447–450 (1970). [CrossRef]
  11. A. Zembrod, H. Puell, and J. Giordmaine, “Surface radiation from nonlinear optical polarization,” Opt. Quantum Electron. 1(1), 64–66 (1969).
  12. A. Fragemann, V. Pasiskevicius, and F. Laurell, “Second-order nonlinearities in domain walls of periodically poled KTiOPO4,” Appl. Phys. Lett. 85(3), 375–377 (2004). [CrossRef]
  13. D. A. Scrymgeour and V. Gopalan, “Nanoscale piezoelectric response across a single antiparallel ferroelectric domain wall,” Phys. Rev. B 72(2), 024103 (2005). [CrossRef]
  14. J. Wittborn, C. Canalias, K. V. Rao, R. Clemens, H. Karlsson, and F. Laurell, “Nanoscale imaging of domains and domain walls in periodically poled ferroelectrics using atomic force microscopy,” Appl. Phys. Lett. 80(9), 1622–1624 (2002). [CrossRef]
  15. D. A. Scrymgeour, V. Gopalan, A. Itagi, A. Saxena, and P. J. Swart, “Phenomenological theory of a single domain wall in uniaxial trigonal ferroelectrics: Lithium niobate and lithium tantalate,” Phys. Rev. B 71(18), 184110 (2005). [CrossRef]
  16. S. M. Saltiel, D. N. Neshev, W. Krolikowski, A. Arie, O. Bang, and Y. S. Kivshar, “Multiorder nonlinear diffraction in frequency doubling processes,” Opt. Lett. 34(6), 848–850 (2009). [CrossRef] [PubMed]
  17. P. Molina, M. O. Ramírez, and L. E. Bausá, “Stronitium Barium Niobate as a multifunctional two-dimensional nonlinear ‘photonic glass’,” Adv. Funct. Mater. 18(5), 709–715 (2008). [CrossRef]

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