Enhancement of second-order optical nonlinearities and nanoscale periodic domain patterning in ferroelectric boron-substituted aluminum nitride thin films

Albert Suceava, John Hayden, Kyle P. Kelley, Yihuang Xiong, Benazir Fazlioglu-Yalcin, Ismaila Dabo, Susan Trolier-McKinstry, Jon Paul Maria, Venkatraman Gopalan

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

Abstract

The discovery and development of CMOS-compatible, nonlinear optical materials is essential to produce integrated photonic devices with advanced functionalities. AlN is a strong candidate for on-chip device demonstration due to its intrinsic second-order optical nonlinearities, large bandgap, and well-established fabrication techniques. However, AlN is not easily phase matched for the largest coefficient d33; the coefficients that could potentially be dispersion phase-matched, d31 and d15, have weak nonlinearities. This work investigates ferroelectric Al1−xBxN (x = 0 to 0.11) for viability as a large bandgap nonlinear optical material with unique suitability towards ultraviolet light generation using second harmonic generation. The linear and nonlinear optical properties are characterized accounting for material anisotropy. With increasing B concentration, a large enhancement from near negligible values to d31 = 0.9 ± 0.1 pm/V and d15= 1.2 ± 0.1 pm/V is observed. This compares favorably to other large bandgap materials like β-Ba(BO2)2, where the largest nonlinear coefficient is d22 ∼ 2.3 pm/V at 800 nm. This is accompanied by a change in the bandgap from 6.1 eV to 5.8 eV as B substitution goes from 0 to 11%. A periodically poled, quasi-phase-matched ferroelectric domain pattern with 400 nm domain size and a wall roughness of <16 nm is demonstrated.

Original languageEnglish
Pages (from-to)1522-1534
Number of pages13
JournalOptical Materials Express
Volume13
Issue number6
DOIs
StatePublished - Jun 1 2023

Funding

Acknowledgments. The growth, optical characterization, and first principles modeling of this material is based upon work supported by the center for 3D Ferroelectric Microelectronics (3DFeM), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences Energy Frontier Research Centers program under Award Number DE-SC0021118. The piezoresponse force microscopy research was performed at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. B.F.-Y. acknowledges the US Department of Energy, Office of Science, Basic Energy Sciences, under Award Number DE-SC0020145 as part of the Computational Materials Sciences Program. We would like to acknowledge Rui Zu for providing his personal #SHAARP code for analysis of the optical second harmonic generation data collected for this work, as well as for multiple discussions regarding modelling and interpretation of said results. J-P.M. and V.G. acknowledge valuable discussions with Joseph Mantese from Raytheon. U.S. Department of Energy (DE-SC0020145, DE-SC0021118). The growth, optical characterization, and first principles modeling of this material is based upon work supported by the center for 3D Ferroelectric Microelectronics (3DFeM), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences Energy Frontier Research Centers program under Award Number DE-SC0021118. The piezoresponse force microscopy research was performed at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. B.F.-Y. acknowledges the US Department of Energy, Office of Science, Basic Energy Sciences, under Award Number DE-SC0020145 as part of the Computational Materials Sciences Program. We would like to acknowledge Rui Zu for providing his personal #SHAARP code for analysis of the optical second harmonic generation data collected for this work, as well as for multiple discussions regarding modelling and interpretation of said results. J-P.M. and V.G. acknowledge valuable discussions with Joseph Mantese from Raytheon.

FundersFunder number
CNMS
Oak Ridge National Laboratory
Office of Basic Energy Sciences Energy Frontier Research Centers
center for 3D Ferroelectric Microelectronics
U.S. Department of EnergyDE-SC0021118
Office of Science
Basic Energy SciencesDE-SC0020145

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