Reversible and Tunable Second‐Order Nonlinear Optical Susceptibility in PZT Thin Films for Integrated Optics

Feutmba, Gilles Freddy; Hermans, Artur; George, John P.; Rijckaert, Hannes; Ansari, Irfan; Thourhout, Dries Van; Beeckman, Jeroen

doi:10.1002/adom.202100149

Cited by 7 publications

(5 citation statements)

References 42 publications

(47 reference statements)

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“…SHG and THG susceptibilities, χ (2) and χ (3) , respectively, were obtained by a relative intensity method based on nonlinear Maxwell’s equation. − For calculating χ (2) and χ (3) , commercial betabarium borate (BBO) and 2D (BA) 2 PbI 4 single crystals were used as reference materials, respectively, as shown in Figure b. The reported value of χ (2) , for BBO is 4.162 pm V –1 at 1550 nm wavelength, and the χ (3) of (BA) 2 PbI 4 is 3.5 × 10 –18 m 2 V –2 at 1500 nm. , The obtained effective χ (2) = 5.73 pm V –1 at 1580 nm and χ (3) = 3.45 × 10 –18 m 2 V –2 at 1500 nm for (MIPA) 2 PbI 4 indicate that the second and third-order nonlinear susceptibilities of (MIPA) 2 PbI 4 are significantly high and hence have promising potential in lasing applications in a wide wavelength range. It should be, however, noted that the BBO is ideal as the reference for 800 nm up-conversion.…”

Section: Resultsmentioning

confidence: 99%

“…The reported value of χ (2) , for BBO is 4.162 pm V −1 at 1550 nm wavelength, and the χ (3) of (BA) 2 PbI 4 is 3.5 × 10 −18 m 2 V −2 at 1500 nm. 40,46 The obtained effective χ (2) = 5.73 pm V −1 at 1580 nm and χ (3) = 3.45 × 10 −18 m 2 V −2 at 1500 nm for (MIPA) 2 PbI 4 indicate that the second and third-order nonlinear susceptibilities of (MIPA) 2 PbI 4 are significantly high and hence have promising potential in lasing applications in a wide wavelength range. It should be, however, noted that the BBO is ideal as the reference for 800 nm upconversion.…”

Section: ■ Introductionmentioning

confidence: 84%

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Rational Design of Non-Centrosymmetric Hybrid Halide Perovskites

et al. 2023

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Structural non-centrosymmetry in semiconducting organic–inorganic hybrid halide perovskites can introduce functionalities like anomalous photovoltaics and nonlinear optical properties. Here we introduce a design principle to prepare Pb- and Bi-based two- and one-dimensional hybrid perovskites with polar non-centrosymmetric space groups. The design principle relies on creating dissimilar hydrogen and halogen bonding non-covalent interactions at the organic–inorganic interface. For example, in organic cations like I–(CH2)3–NH2(CH3)+ (MIPA), −CH3 is substituted by −CH2I at one end, and −NH3 + is substituted by −NH2(CH3)+ at the other end. These substitutions of two −H atoms by −I and −CH3 reduce the rotational symmetry of MIPA at both ends, compared to an unsubstituted cation, for example, H3C–(CH2)3–NH3 +. Consequently, the dissimilar hydrogen–iodine and iodine–iodine interactions at the organic–inorganic interface of (MIPA)2PbI4 2D perovskites break the local inversion symmetries of Pb–I octahedra. Owing to this non-centrosymmetry, (MIPA)2PbI4 displays visible to infrared tunable nonlinear optical properties with second and third harmonic generation susceptibility values of 5.73 pm V–1 and 3.45 × 10–18 m2 V–2, respectively. Also, the single crystal shows photocurrent on shining visible light at no external bias, exhibiting anomalous photovoltaic effect arising from the structural asymmetry. The design strategy was extended to synthesize four new non-centrosymmetric hybrid perovskite compounds. Among them, one-dimensional (H3N–(CH2)3–NH(CH3)2)BiI5 shows a second harmonic generation susceptibility of 7.3 pm V–1 and a high anomalous photovoltaic open-circuit voltage of 22.6 V.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 84%

Rational Design of Non-Centrosymmetric Hybrid Halide Perovskites

et al. 2023

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“…21 Using the results from Figure 8e, a half-wave voltagelength product of V π L = 2.019 V cm and r wg = 94.50 pm V −1 are obtained, yielding comparable results to those reported in state-of-the-art Pb(Zr,Ti)O 3 thin films. 13,54 In addition, the poling is stable and there have been no indications of decay of much longer periods of time.…”

Section: ■ Results and Discussionmentioning

confidence: 98%

Solution-Processed Pb(Zr,Ti)O₃Thin Films with Strong Remnant Pockels Coefficient

Picavet,

De Geest,

Lievens

et al. 2024

ACS Appl. Mater. Interfaces

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In contrast to the widely studied electrical properties of Pb(Zr,Ti)O 3 thin films, which have led to their applicability in various application areas such as thin film capacitors, microelectronics, and ferroelectric memories, the electro-optic (EO) properties are far less studied, which hinders the applicability of Pb(Zr,Ti)O 3 films for EO applications such as heterogeneously integrated phase modulators in silicon (Si) photonics. Therefore, the EO properties of Pb(Zr,Ti)O 3 films need to be further investigated to pave the way for the applicability of Pb(Zr,Ti)O 3 films in EO applications. As the EO properties of ferroelectric thin films strongly depend on their crystal phase and texture, which in turn are influenced by the method of film fabrication. Therefore, in this work, we investigate the EO properties of a promising solution process using a La 2 O 2 CO 3 template film. We successively characterize the precursor ink, microstructure and EO properties of the solution-processed Pb(Zr,Ti)O 3 film. The Pb(Zr,Ti)O 3 film exhibits a fiber texture and has a large maximum and remnant Pockels coefficient (r eff ) of 69 pm V −1 and 66 pm V −1 , respectively. The integration into a ring resonator-based modulator shows a V π L of 2.019 V cm. The determination of these promising EO properties could further pave the way for the applicability of Pb(Zr,Ti)O 3 thin films in Si photonics.

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“…The high quality of this PZT film has been proven through the demonstration of electro-optic modulators with very low optical loss (<1 dB/cm) on both SiN and Si photonic platforms . Additionally, we also demonstrated that this film exhibits a high second-order nonlinearity (χ zzz 2 128 pm/V) . Therefore, a detailed investigation of the piezoelectric effect and acousto-optic modulation with this PZT film is warranted. − …”

Section: Introductionmentioning

confidence: 97%

Light Modulation in Silicon Photonics by PZT Actuated Acoustic Waves

et al. 2022

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Tailoring the interaction between light and sound has opened new possibilities in photonic integrated circuits (PICs) that range from achieving quantum control of light to high-speed information processing. However, the actuation of sound waves in Si PICs usually requires integration of a piezoelectric thin film. Lead zirconate titanate (PZT) is a promising material due to its strong piezoelectric and electromechanical coupling coefficient. Unfortunately, the traditional methods to grow PZT on silicon are detrimental for photonic applications due to the presence of an optical lossy intermediate layer. In this work, we report integration of a high quality PZT thin film on a silicon-on-insulator (SOI) photonic chip using an optically transparent buffer layer. We demonstrate acousto-optic modulation in silicon waveguides with the PZT actuated acoustic waves. We fabricate interdigital transducers (IDTs) on the PZT film with a contact photolithography and electron-beam lithography to generate the acoustic waves in MHz and GHz ranges, respectively. We obtain a V π L ∼ 3.35 V•cm at 576 MHz from a 350 nm thick gold (Au) IDT with 20 finger-pairs. After taking the effect of mass-loading and grating reflection into account, we measured a V π L ∼ 3.60 V•cm at 2 GHz from a 100 nm thick aluminum (Al) IDT consisting of only four finger-pairs. Thus, without patterning the PZT film nor suspending the device, we obtained figures-of-merit comparable to state-of-the-art modulators based on SOI, making it a promising candidate for a broadband and efficient acousto-optic modulator for future integration.

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Reversible and Tunable Second‐Order Nonlinear Optical Susceptibility in PZT Thin Films for Integrated Optics

Cited by 7 publications

References 42 publications

Rational Design of Non-Centrosymmetric Hybrid Halide Perovskites

Rational Design of Non-Centrosymmetric Hybrid Halide Perovskites

Solution-Processed Pb(Zr,Ti)O₃Thin Films with Strong Remnant Pockels Coefficient

Light Modulation in Silicon Photonics by PZT Actuated Acoustic Waves

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Reversible and Tunable Second‐Order Nonlinear Optical Susceptibility in PZT Thin Films for Integrated Optics

Cited by 7 publications

References 42 publications

Rational Design of Non-Centrosymmetric Hybrid Halide Perovskites

Rational Design of Non-Centrosymmetric Hybrid Halide Perovskites

Solution-Processed Pb(Zr,Ti)O3Thin Films with Strong Remnant Pockels Coefficient

Light Modulation in Silicon Photonics by PZT Actuated Acoustic Waves

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Product

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Solution-Processed Pb(Zr,Ti)O₃Thin Films with Strong Remnant Pockels Coefficient