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| Citation: |
Chakkoria JJ, Dubey A, Mitchell A et al. Ferroelectric domain engineering of lithium niobate. Opto-Electron Adv 8, 240139 (2025). doi: 10.29026/oea.2025.240139
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Abstract
Lithium niobate (LN) has remained at the forefront of academic research and industrial applications due to its rich material properties, which include second-order nonlinear optic, electro-optic, and piezoelectric properties. A further aspect of LN’s versatility stems from the ability to engineer ferroelectric domains with micro and even nano-scale precision in LN, which provides an additional degree of freedom to design acoustic and optical devices with improved performance and is only possible in a handful of other materials. In this review paper, we provide an overview of the domain engineering techniques developed for LN, their principles, and the typical domain size and pattern uniformity they provide, which is important for devices that require high-resolution domain patterns with good reproducibility. It also highlights each technique's benefits, limitations, and adaptability for an application, along with possible improvements and future advancement prospects. Further, the review provides a brief overview of domain visualization methods, which is crucial to gain insights into domain quality/shape and explores the adaptability of the proposed domain engineering methodologies for the emerging thin-film lithium niobate on an insulator platform, which creates opportunities for developing the next generation of compact and scalable photonic integrated circuits and high frequency acoustic devices. -
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References
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Chakkoria JJ, Dubey A, Mitchell A et al. Ferroelectric domain engineering of lithium niobate. Opto-Electron Adv 8, 240139 (2025). doi: 10.29026/oea.2025.240139
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Figure 1.
(a) Top view of the relative arrangement of oxygen atoms about the Li and Nb atoms in LN, corresponding to the sequence of the unit cell. (b) Side view illustration of the LN unit cell crystal structure. (c) The relative position of the cations (Li and Nb) in the crystal structure in relation to the oxygen plane is represented by black lines. The dashed lines indicate the center position between two oxygen planes. Figures redrawn from: (a) ref.34, CRC Press ; (b, c) ref.35, Elsevier.
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Figure 2.
(a, b) Movement of the Li and Nb ions during domain inversion. The Nb ions undergo a small displacement within their oxygen octahedrons, whereas the Li ions undergo a larger displacement through the close-packed oxygen planes into the adjacent, vacant oxygen octahedrons. Figure redrawn from ref.33, Annual Reviews.
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Figure 3.
(a) Illustration of the domain visualization process using selective chemical etching. (b) Periodically poled bulk LN (Z-cut) viewed under an optical microscope. (c) Image of etched LNOI (X-cut) sample observed with an SEM.
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Figure 4.
(a) Schematic for contact-mode scanning probe microscopy used for PFM. (b) Illustration of the PFM signal, resulting from the orientation of the spontaneous polarization and the applied external voltage to the conductive cantilever. (c) PFM image of a periodically poled LN crystal.
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Figure 5.
(a) Schematic of transmission interference SHG microscopy. (b) Illustration of interference process that is used for imaging the domain pattern, redrawn from ref.53, IOP Publishing. (c) Example of an interference SHG microscopy image of a periodically poled LN crystal. Figure reproduced with permission from ref.54, Optical Society of America.
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Figure 6.
(a) Schematic of transmission non-interference SHG microscopy. (b) Illustration of interference of SH signals at the domain boundary, causing the disappearance of the SH signal. (c) Example of a non-interference SHG microscopy image of a periodically poled LN crystal. Figure reproduced with permission from ref.54, Optical Society of America.
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Figure 7.
(a) Schematic of Cerenkov second harmonic generation microscopy. (b) Only a collinear (forward) second harmonic signal is generated in a homogeneous sample. (c) a conical Cerenkov signal is generated when ferroelectric domain walls are present. (d) Three-dimensional visualization of a square pattern of inverted domains by Cerenkov second harmonic microscopy58. Figure reproduced with permission from ref.63, Optical Society of America.
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Figure 8.
(a) Schematic of the electro-optic imaging microscopy setup. (b) Optical setup with cross polarizers to inspect the poled domains. (c) Microscope Image of poled domains analyzed using polarization contract microscopy on an X-cut 600 nm thin film LNOI with an LN substrate. Figure redawn from: (a) ref.64, AIP Publishing; (b) ref.ref.67, Optical Society of America.
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Figure 9.
Schematic of (a) single crystal and single domain Czochralski growth technique by applying electric field redrawn from ref.3, and (b) off-centered Czochralski growth technique for PPLN.
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Figure 10.
(a) Evaporation of metallic titanium and spin coating of photoresist, (b) patterning and development of resist, (c) wet etching of titanium, (d) removal of photoresist, (e) titanium indiffusion by heating in a furnace and domain inversion, and (f) etched-surface micrograph of inverted domains. Figure reproduced with permission from ref.72, AIP Publishing.
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Figure 11.
Illustration of the six stages of domain kinetics during electric field periodic poling. (a) Domain nucleation at the electrode edges. (b) Domain tip propagation toward the opposite face of the crystal. (c) Termination of the domain tips at the opposite side of the crystal. (d) Rapid coalescence under the electrodes. (e) Lateral domain growth. (f) Stabilization of the inverted domains. Illustration redrawn from ref.89.
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Figure 12.
(a–d) Schematic illustration of the evolution of inverted domain using a single long poling pulse. (e–h) Schematic illustration of the evolution of inverted domains using multi-pulse waveforms with short pulse durations. (i) Schematic of cross section of the device obtained after ion milling to visualize the periodically poled region. (j) Top-view micrograph of the cross section of a poled device after 10 min 48% HF etch at room temperature. The dashed line corresponds to the cross section in which the bright part is the poled area. (k) SEM image of inverted domain. (l) Schematic illustration of poling process in X-cut LNOI. (m) Schematic illustration of poling process in Z-cut LNOI. Figure reproduced with permission from (a–k) ref 92, Optical Society of America.
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Figure 13.
Schematic illustration of the AFM-tip domain writing process for (a) bulk LN; (c) helium implanted bulk LN; and (e) thin-film LNOI. (b) Electrostatic force microscopy image of inverted domains in Bulk LN. (d) PFM image of inverted domains in He-implanted bulk LN. (f) PFM image of inverted domains in thin-film LNOI. Figure reproduced with permission from: (b) ref.98, (d) ref.100, AIP Publishing; ref.102, Optical Society of America.
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Figure 14.
Schematic illustration of (a) electron beam and (c) ion beam poling process, and (b, d) PFM image of inverted domain108,120. Figure reproduced with permission from: (b) ref.108, AIP Publishing; (d) ref.120, Taylor & Francis Ltd.
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Figure 15.
(a) Schematic of a light-assisted poling setup, showing the focusing of the illuminating laser beam on the +Z face of a LN crystal held between liquid electrodes (W) using fused silica (FS) plates, replotted from ref.131 . The white light (WL) is used only for visualization of the poling process via the crossed polarizer and CCD camera. (P = crossed polarizers; L = lens; F = filter to block the laser beam; M = dielectric mirror; HV = high voltage; O = O-ring). (b) SEM image of inverted domains. Figure reproduced with permission from (b) ref.130, Taylor & Francis Ltd.
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Figure 16.
Illustration of the poling inhibition process. The focused UV light is strongly absorbed at the crystal surface, generating a local heat profile (a), which causes Li diffusion into the colder adjacent crystal (b). The coercive depends on the Li concentration (c). When a poling step is applied (d), the domains prefer to nucleate at the Li enriched region next to the UV-irradiated area (e). The Li deficient region on the other hand is poling inhibited, resulting in a surface domain when the poling step is completed (f). SEM image of poling inhibited domain cross-section after HF-etching (g). Figure reprinted with the permission from (g) ref.135, AIP Publishing.
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Figure 17.
Illustration of the laser direct writing process on the +Z face (a–c), −Z face (d–f), and X and Y cut crystal (g–i). Domain inversion occurs when the thermoelectric field is higher than the coercive field of the Lithium Niobate (LN) crystal. PFM images of inverted domains on the Z face. In the PFM image −Z domains appear black and +Z domains appear white (j) and Y-cut134, where the direction of irradiation is in chronology (1 to 4) (k). Figure reproduced with permission from: (j) ref.137, Optical Society of America; (k) ref.134, AIP Publishing.
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Figure 18.
Illustration of the fabrication steps for visible light irradiation of a Cr pattern: (a) Cr pattern on the surface of a LN crystal, (b) generation of the surface domains by laser light irradiation, and (c) Cr pattern removal by Cr etchant, and (d–f) SEM images of domain patterns with period of 300nm. Figure reproduced with permission from (d–f) ref.139, AIP Publishing.
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Figure 19.
(a) Schematic of direct writing ferroelectric domain patterns in a LN crystal using femtosecond infrared pulses, and (b) 3D profile of inverted domains using Cerenkov second-harmonic microscopy. Figure reproduced from (b) ref.59, AIP Publishing.
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Figure 20.
(a–d) Illustration of energy level diagram describing second harmonic generation (SHG), sum frequency generation (SFG), difference frequency generation (DFG), and spontaneous parametric down conversion (SPDC). (e) Illustration of the relative phase matching efficiencies for non-phase matching (NPM), quasi-phase matching (QPM) and perfect phase matching (PPM). The sign of the nonlinear susceptibility χ(2) is inverted after each coherence length lc for QPM. Figure redrawn from: (a–d) ref.162, Elsevier; (e) ref.28.
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Figure 21.
(a) Illustration of the EO modulator with open-circuited-end microstrip electrode and inversion sections. (b) The modulation index as a function of interaction length in the case of velocity matching, quasi-matching and mismatching. Figure redrawn from: (a) ref.180, (b) ref.178, IEEE.
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Figure 22.
(a) Schematic of an IDT on a LN substrate. (b) Basic structure of ASL based-on ZX-cut PPLN with coplanar electrodes. (c) Schematic of the integrated AO polarization converter based on ASL on Z-cut PPLN with coplanar uniform electrodes. Figure redrawn from: (a) ref.193, (b) ref.194, AIP Publishing; (c) ref.16, Optical Society of America.
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Figure 23.
(a) Illustration of a surface phonon cavity with a bandgap structure consisting of regular poling with period a, and with an included defect of width D. (b) Microscope image of the fabricated surface phonon cavity and the IDTs used to generate the SAW. The poled bandgap region is indicated by the larger white dashed rectangle and the region with the defect is indicated by the smaller dark dashed rectangle. (c) Schematic of the surface phonon-polariton phononic crystal formed from domain-inverted hexagonal inclusions. (d) An optical micrograph of the back side of the substrate after HF etching, with a scanning electron microscope image inset showing the hexagonal domain-inverted inclusion. Figure reproduced with permission from: (a, b) ref.199, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim; (c, d) ref.15, American Physical Society.
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Figure 24.
(a) SEM image (tilted at 45°) of large aspect ratio surface structures in LN produced by extended etching of a domain pattern for tens of hours. The long sections of the slabs are aligned along the y-axis of the crystal thus producing X-face sidewall surfaces which etch much slower than −Z face. (b) SEM 45˚ angle view image of a fabricated nanopillar phononic crystals in LN. (c) SEM images of the micro-structured LN crystal surface (45° tilted) after deep etching of a 2D lattice of inverted ferroelectric domains. (d) shows the micro-structured LN crystal after thermal treatment. Figure reproduced with permission from: (a) ref.125, John Wiley and Sons; (b) ref. 201, American Physical Society; (c, d) ref.202, Optical Society of America.
