Giant Non-Resonant Infrared Second Order Nonlinearity in γ -NaAsSe2

Jingyang He; Abishek K. Iyer; Michael J. Waters; Sumanta Sarkar; Rui Zu; James M. Rondinelli; Mercouri G. Kanatzidis; Venkatraman Gopalan

doi:10.1002/adom.202101729

Giant Non-Resonant Infrared Second Order Nonlinearity in γ -NaAsSe₂

Jingyang He, Abishek K. Iyer, Michael J. Waters, Sumanta Sarkar, Rui Zu, James M. Rondinelli, Mercouri G. Kanatzidis^*, Venkatraman Gopalan^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

Infrared laser systems are vital for applications in spectroscopy, communications, and biomedical devices, where infrared nonlinear optical (NLO) crystals are required for broadband frequency down-conversion. Such crystals need to have high non-resonant NLO coefficients, a large bandgap, low absorption coefficient, and phase-matchability among other competing demands; for example, a larger bandgap leads to smaller NLO coefficients. Here, the successful growth of single crystals of γ -NaAsSe₂ that exhibit a giant second harmonic generation (SHG) susceptibility of d₁₁ = 590 pm V⁻¹ at 2 µm wavelength is reported; this is ~18 times larger than that of commercial AgGaSe₂ while retaining a similar bandgap of ~1.87 eV, making it an outstanding candidate for quasi-phase-matched devices utilizing d₁₁. In addition, γ -NaAsSe₂ is both Type I and Type II phase-matchable, and has a transparency range up to 16 µm wavelength. Thus, γ -NaAsSe₂ is a promising bulk NLO crystal for infrared laser applications.

Original language	English (US)
Article number	2101729
Journal	Advanced Optical Materials
Volume	10
Issue number	2
DOIs	https://doi.org/10.1002/adom.202101729
State	Published - Jan 18 2022

Funding

J.H. and A.K.I. contributed equally to this work. J.H., A.K.I., S.S., M.G.K., and V.G. acknowledge the Air Force Office of Scientific Research Grant number FA9550‐18‐S‐0003. M.J.W. and J.M.R. were supported by the National Science Foundation's (NSF) MRSEC program (DMR‐1720139) at the Materials Research Center of Northwestern University. R.Z. and V.G. were supported by the NSF Materials Research Science and Engineering Center for Nanoscale Science, DMR‐2011839. Scientific discussions and advice from Gary Cook, Carl M. Liebig, Ryan K. Feaver, Sean A. McDaniel, and Rita D. Peterson from the AFRL are gratefully acknowledged. J.H. and A.K.I. contributed equally to this work. J.H., A.K.I., S.S., M.G.K., and V.G. acknowledge the Air Force Office of Scientific Research Grant number FA9550-18-S-0003. M.J.W. and J.M.R. were supported by the National Science Foundation's (NSF) MRSEC program (DMR-1720139) at the Materials Research Center of Northwestern University. R.Z. and V.G. were supported by the NSF Materials Research Science and Engineering Center for Nanoscale Science, DMR-2011839. Scientific discussions and advice from Gary Cook, Carl M. Liebig, Ryan K. Feaver, Sean A. McDaniel, and Rita D. Peterson from the AFRL are gratefully acknowledged.

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Atomic and Molecular Physics, and Optics

Access to Document

10.1002/adom.202101729

Cite this

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title = "Giant Non-Resonant Infrared Second Order Nonlinearity in γ -NaAsSe2",

abstract = "Infrared laser systems are vital for applications in spectroscopy, communications, and biomedical devices, where infrared nonlinear optical (NLO) crystals are required for broadband frequency down-conversion. Such crystals need to have high non-resonant NLO coefficients, a large bandgap, low absorption coefficient, and phase-matchability among other competing demands; for example, a larger bandgap leads to smaller NLO coefficients. Here, the successful growth of single crystals of γ -NaAsSe2 that exhibit a giant second harmonic generation (SHG) susceptibility of d11 = 590 pm V−1 at 2 µm wavelength is reported; this is ~18 times larger than that of commercial AgGaSe2 while retaining a similar bandgap of ~1.87 eV, making it an outstanding candidate for quasi-phase-matched devices utilizing d11. In addition, γ -NaAsSe2 is both Type I and Type II phase-matchable, and has a transparency range up to 16 µm wavelength. Thus, γ -NaAsSe2 is a promising bulk NLO crystal for infrared laser applications.",

author = "Jingyang He and Iyer, {Abishek K.} and Waters, {Michael J.} and Sumanta Sarkar and Rui Zu and Rondinelli, {James M.} and Kanatzidis, {Mercouri G.} and Venkatraman Gopalan",

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AU - He, Jingyang

AU - Iyer, Abishek K.

AU - Waters, Michael J.

AU - Sarkar, Sumanta

AU - Zu, Rui

AU - Rondinelli, James M.

AU - Kanatzidis, Mercouri G.

AU - Gopalan, Venkatraman

PY - 2022/1/18

Y1 - 2022/1/18

N2 - Infrared laser systems are vital for applications in spectroscopy, communications, and biomedical devices, where infrared nonlinear optical (NLO) crystals are required for broadband frequency down-conversion. Such crystals need to have high non-resonant NLO coefficients, a large bandgap, low absorption coefficient, and phase-matchability among other competing demands; for example, a larger bandgap leads to smaller NLO coefficients. Here, the successful growth of single crystals of γ -NaAsSe2 that exhibit a giant second harmonic generation (SHG) susceptibility of d11 = 590 pm V−1 at 2 µm wavelength is reported; this is ~18 times larger than that of commercial AgGaSe2 while retaining a similar bandgap of ~1.87 eV, making it an outstanding candidate for quasi-phase-matched devices utilizing d11. In addition, γ -NaAsSe2 is both Type I and Type II phase-matchable, and has a transparency range up to 16 µm wavelength. Thus, γ -NaAsSe2 is a promising bulk NLO crystal for infrared laser applications.

AB - Infrared laser systems are vital for applications in spectroscopy, communications, and biomedical devices, where infrared nonlinear optical (NLO) crystals are required for broadband frequency down-conversion. Such crystals need to have high non-resonant NLO coefficients, a large bandgap, low absorption coefficient, and phase-matchability among other competing demands; for example, a larger bandgap leads to smaller NLO coefficients. Here, the successful growth of single crystals of γ -NaAsSe2 that exhibit a giant second harmonic generation (SHG) susceptibility of d11 = 590 pm V−1 at 2 µm wavelength is reported; this is ~18 times larger than that of commercial AgGaSe2 while retaining a similar bandgap of ~1.87 eV, making it an outstanding candidate for quasi-phase-matched devices utilizing d11. In addition, γ -NaAsSe2 is both Type I and Type II phase-matchable, and has a transparency range up to 16 µm wavelength. Thus, γ -NaAsSe2 is a promising bulk NLO crystal for infrared laser applications.

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