1.9 Poling and periodic poling
L1 Writing domains
To pole is to set the polarization with a field. A uniform field across a whole wafer makes one domain; a field applied through a comb of electrodes flips only the stripes under the teeth. The result, periodically poled lithium niobate (PPLN), alternates the sign of the crystal’s nonlinear and electro-optic coefficients every few micrometres. That alternation lets light waves of different colours stay in step over centimetres of crystal (quasi-phase-matching, Chapter 02).
Every flipped domain moves a fixed charge: twice the spontaneous polarization times its area. Flipping one square centimetre takes 142 microcoulombs with Ps = 0.71 C/m2 (160 with 0.80 C/m2 conflict) derived, so the current trace of a poling pulse is a direct record of how much crystal has switched.
comb, +z ============= ============= =============
16 um+ #############..................##############...................##############..................
|#############..................##############...................#############+.................#
|#############..................+#############...................#############...................
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12 um+ #############...................#############...................#############...................
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|#############...................#############+..................#############..................+
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8 um+ ##############..................#############...................#############...................
|##############+.................#############...................#############...................
|###############.................#############...................#############...................
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|###############.................#############...................#############..................+
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4 um+ #############..................##############...................#############..................#
|#############.................+##############...................#############...................
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|#############..................+#############...................#############...................
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|#############..................##############...................#############+..................
0 um+ +----------------------+----------------------+----------------------+----------------------+---
x, um 0 5 10 15 20 V kV 13+ ********************************************************* |
|********** *************************** |
0+ **
I nA 80+ |
| ** |
| ** * |
| ** : * |
| ****************************** *** * *********** * * |
0+*****------------------------------**---*-**---------------------*******************************
−20+ |
Q pC 472+ |
| |
| *************************************
0+*********************************************************** |
X 1+ |
| |
|- - - - - - - - - - - - - - - - - - - - - - - - - - - - - - - -*********************************
| ooo******oooo |
0+********************************************************* |
++---------'-------------'---------+---------'------------'---------+----------'------------'----
t, ms log 0.1 1 10 | State | done | |
| Time, voltage | t 70.00 ms V 0.00 kV | template |
| I = 2Ps dA/dt + C dV/dt | 0.0 nA | derived |
| Q = ∫(I − C dV/dt) dt | 197.0 pC | derived |
| 2PsA of the map | 197.0 pC | derived |
| Reversed area A | 138.7 µm² | template |
| Q / A | 142.0 µC/cm² | derived |
| Switched fraction X | 0.417 | derived |
| Domain duty / comb w/Λ | 0.42 / 0.41 | derived |
| Backswitched | 0.00 | template |
| KAI fit | n 2.06 | template |
| t₀ 6.81 ms r² 0.88 |
P, C/m² : | :
0.71 + | ooo
| : | :o
| |
| : | :
| | o
0 +--------:-------------|----------------:----
| @******************
| : | :*
| | *
| : | o:*
−0.71 +oooooooooooooooooooooo*******************
| : | :
++-------+-------------+----------------+---+
E kV/mm −26 −16 0 21 26 - State
- done
- Time, voltage
- t 70.00 ms V 0.00 kV
- Current I derived
- 0.0 nA
- Charge Q derived
- 197.0 pC
- 2PsA of the map
- 197.0 pC
- Q / A
- 142.0 µC/cm²
- Switched fraction X derived
- 0.417
- Comb w/Λ
- 0.41
- Backswitched template
- 0.00
- KAI fit template
- n 2.06
- t₀ 6.81 ms r² 0.88
Press Pulse: domains nucleate on the +z face, mostly at the finger edges, grow as hexagons, touch and merge into stripes while the current trace draws itself; the integrated charge Q equals 2Ps times the reversed area at every step. Set the field to 0 after the pulse and press again: the fresh domains shrink back (backswitching, a negative current) template; hold Ec/2 and they stay. A longer pulse spreads domains past the fingers (domain merging) and lifts the duty cycle above w/Λ. The P–E panel plots P = −Ps + Q/A against the applied field as the pulse plays: a unipolar pulse drives only the forward branch, so the return branch, at −(Ec − 2Eint) = −16 kV/mm, is never reached and is not drawn. Any parameter change loads a fresh single-domain patch; the same seed replays the same run. Rates are template values; Ps, Ec, Eint, the hexagon facets and nucleation at +z are sourced.
L2 Charge, history, practice
| Quantity | Value | Status |
|---|---|---|
| Switched charge per area, Q/A = 2Ps | 1.42 C/m2 = 142 µC/cm2 (Ps = 0.71 C/m2); 160 µC/cm2 (Ps = 0.80 C/m2) conflict | derived |
| Charge to invert a whole 76.2 mm (3 inch) wafer | 6.5 mC (Ps = 0.71 C/m2); 7.3 mC (0.80 C/m2); area π (38.1 mm)2 | derived |
| Optimum duty cycle for first-order QPM | 0.5 | P-comp |
Milestones of domain engineering, dates as published (Chapter 07 holds the full chronology):
| Year | Step | Source |
|---|---|---|
| 1962 | Periodic reversal of the nonlinear coefficient proposed for phase matching | P |
| 1965 | Domains revealed by etching | P |
| 1966 | Preparation of single-domain crystals | P |
| 1979 | Ti in-diffusion inverts a surface layer on the +c face | P(abs) |
| 1980 | Periodic laminar domains grown in by Czochralski growth striations; SHG enhanced by QPM on d33; Y-doped, period 7 µm | P(abs) P-comp |
| 1993 | First-order QPM waveguide poled by an external field at room temperature; 20.7 mW blue, 600 %/(W cm2); pulse 24 kV/mm, 100 µs, period 2.8 µm | P(abs) P-comp |
| 1994–1995 | Liquid-electrode poling, period from 9 µm to 4.5 µm; deff from 2 to 19 pm/V against a 22 pm/V limit | P-comp |
| 1995 | Bulk PPLN optical parametric oscillators; backswitching found and controlled | P P-comp |
Poling practice reported for bulk congruent crystal P-comp:
- Backswitching. If the pulse is too short the new domains flip back; at 25 kV/mm the critical time was at least 50 ms. Remedies: hold at about Ec/2 after the pulse, or use ramped fields.
- Domain merging. Domains spread beyond the electrode, so the electrode duty cycle is set below the target.
- Electrodes. Al stripes on +z under photoresist (or resist openings under a conductor), contacted through LiCl electrolyte; electrolyte on −z.
- Stability. PPLN survived heating to 800 °C.
L3 Kinetics and current
Kinetics. Switching proceeds by nucleation (at the +z surface in undoped crystal), forward growth along c, and sideways wall motion; wall motion itself proceeds by nucleation of steps on the existing wall, which accounts for the activation-type field dependence P-comp P. In congruent crystal the walls run parallel to the yz glide planes P-comp; DFT finds Y-walls lower in energy than X-walls, so domains are hexagons bounded by Y-walls, and antisite–wall interactions in congruent LiNbO3 are too weak to change that P(abs). A Kolmogorov–Avrami–Ishibashi switched fraction is the fit form used below:
In the bench above all rates are template values; only Ps, the Ec anchor, Eint and the domain shape are sourced. Fitted to the default pulse, the automaton gives n = 2.06, t0 = 6.81 ms (r2 = 0.88) template: a property of the template, not of LiNbO3.
What the switching current measures. The current through the electrodes is the switching term plus the charging of the electrode capacitance:
Integrated current minus the capacitive part equals 2PsA of the switched area. In the bench, Q = 196.992 pC against 2PsA = 196.992 pC for the default pulse derived; the displacement term uses C = 0.067 fF derived. The Ps disagreement (0.71 vs 0.80 C/m2 conflict) is therefore an 11% uncertainty in any area inferred from charge derived.
Thin films. Poling of x-cut and z-cut thin-film LN (TFLN; coplanar electrodes, sub-micrometre periods, incomplete depth) is treated with process detail in Chapter 05.
How the bench is computed. Stochastic cellular automaton on a triangular lattice in the z-cut top view, seeded generator, synchronous update. Nearest neighbours lie at 30° + k · 60° from x, so facets run along y and ±60° from y, the traces of the three mirror planes. Untouched sites under a finger nucleate (edge sites 50 times more often than interior ones); sites next to reversed ones switch at step rates (1 or 2 reversed neighbours) or kink rates (3 or more), each with the activation form of Volk & Wöhlecke 2008 Eq. (7.32) referenced to Ec − Eint. Domains younger than the stabilization age revert from their boundary while E < Ec/2. The map has no depth: domains are assumed through the thickness.
| Parameter | Value | Status |
|---|---|---|
| Spontaneous polarization Ps | 0.71 C/m2 (0.80 offered) | P-comp conflict |
| Coercive field Ec, congruent | 21 kV/mm | P-comp |
| Internal field Eint, congruent | 2.5 kV/mm | P(abs) |
| Hold level that suppresses backswitching | 0.5 Ec | reported |
| Stabilization age | 50 ms | template |
| Nucleation rate at Ec, finger-edge site; interior factor; α | 200 s−1; 0.02; 10 | template |
| Step rates, 1 / 2 reversed neighbours | 20 / 100 s−1 | template |
| Kink rate, 3 or more reversed neighbours; wall α | 2 × 104 s−1; 6 | template |
| Backswitching rate at domain boundaries | 200 s−1 | template |
| Field between fingers / applied | 0.7 | template |
| Lattice spacing; patch; time step | 0.25 µm; 20.8 × 16.0 µm; 0.05 ms | template |
| Electrode capacitance (displacement term) | 0.067 fF | derived |
Sources
- Volk & Wöhlecke 2008T. Volk, M. Woehlecke, Lithium Niobate: Defects, Photorefraction and Ferroelectric Switching, Springer Series in Materials Science 115 (Springer, Berlin Heidelberg, 2008). doi:10.1007/978-3-540-70766-0
- Hsu et al. 1997R. Hsu, E. N. Maslen, D. du Boulay, N. Ishizawa, "Synchrotron X-ray studies of LiNbO3 and LiTaO3", Acta Cryst. B 53, 420-428 (1997). doi:10.1107/S010876819600777X
- Gopalan et al. 1998V. Gopalan, T. E. Mitchell, Y. Furukawa, K. Kitamura, "The role of nonstoichiometry in 180 ° domain switching of LiNbO3 crystals", Appl. Phys. Lett. 72, 1981-1983 (1998). doi:10.1063/1.121491
- Kitamura et al. 1998K. Kitamura, Y. Furukawa, K. Niwa, V. Gopalan, T. E. Mitchell, "Crystal growth and low coercive field 180 ° domain switching characteristics of stoichiometric LiTaO3", Appl. Phys. Lett. 73, 3073-3075 (1998). doi:10.1063/1.122676
- Armstrong et al. 1962J. A. Armstrong, N. Bloembergen, J. Ducuing, P. S. Pershan, "Interactions between light waves in a nonlinear dielectric", Phys. Rev. 127, 1918-1939 (1962). doi:10.1103/PhysRev.127.1918
- Nassau et al. 1965K. Nassau, H. J. Levinstein, G. M. Loiacono, "The domain structure and etching of ferroelectric lithium niobate", Appl. Phys. Lett. 6, 228-229 (1965). doi:10.1063/1.1754147
- Nassau et al. 1966bK. Nassau, H. J. Levinstein, G. M. Loiacono, "Ferroelectric lithium niobate. 2. Preparation of single domain crystals", J. Phys. Chem. Solids 27, 989-996 (1966). doi:10.1016/0022-3697(66)90071-0
- Miyazawa 1979S. Miyazawa, "Ferroelectric domain inversion in Ti-diffused LiNbO3 optical waveguide", J. Appl. Phys. 50, 4599-4603 (1979). doi:10.1063/1.326568
- Feng et al. 1980D. Feng, N.-B. Ming, J.-F. Hong, Y.-S. Yang, J.-S. Zhu, Z. Yang, Y.-N. Wang, "Enhancement of second-harmonic generation in LiNbO3 crystals with periodic laminar ferroelectric domains", Appl. Phys. Lett. 37, 607-609 (1980). doi:10.1063/1.92035
- Yamada et al. 1993M. Yamada, N. Nada, M. Saitoh, K. Watanabe, "First-order quasi-phase matched LiNbO3 waveguide periodically poled by applying an external field for efficient blue second-harmonic generation", Appl. Phys. Lett. 62, 435-436 (1993). doi:10.1063/1.108925
- Myers et al. 1995L. E. Myers, R. C. Eckardt, M. M. Fejer, R. L. Byer, W. R. Bosenberg, J. W. Pierce, "Quasi-phase-matched optical parametric oscillators in bulk periodically poled LiNbO3", J. Opt. Soc. Am. B 12(11), 2102 (1995). doi:10.1364/JOSAB.12.002102
- Shur 2006V. Ya. Shur, "Kinetics of ferroelectric domains: Application of general approach to LiNbO3 and LiTaO3", J. Mater. Sci. 41, 199-210 (2006). doi:10.1007/s10853-005-6065-7
- Lee et al. 2011D. Lee, H. Xu, V. Dierolf, V. Gopalan, S. R. Phillpot, "Shape of ferroelectric domains in LiNbO3 and LiTaO3 from defect/domain-wall interactions", Appl. Phys. Lett. 98, 092903 (2011). doi:10.1063/1.3560343