Issue 7, 2023

Melilite oxychalcogenide Sr2FeGe2OS6: a phase-matching IR nonlinear optical material realized by isomorphous substitution

Abstract

Transition-metal-based chalcogenides have recently emerged as greatly promising infrared nonlinear optical (IR-NLO) candidates due to their unique structural chemistries and rich optical properties. However, Fe-based IR-NLO chalcogenides with phase-matching (PM) features have not yet been reported. In this work, a new non-centrosymmetric (NCS) melilite oxychalcogenide, Sr2FeGe2OS6, has been prepared by an isomorphous substitution method, and the relationships between the microscopic crystal structure and macroscopic NLO activity were systematically investigated. Sr2FeGe2OS6 adopts the tetragonal space group of P[4 with combining macron]21m (no. 113) and features a unique two-dimensional structure with Cairo pentagonal tiling layers formed by the alternating connection of [Ge2OS6] dimers and [FeS4] tetrahedra via corner-sharing and with the charge-balanced Sr2+ cations between these layers. Excitingly, Sr2FeGe2OS6 is the first Fe-based example capable of achieving PM in the IR-NLO chalcogenide system and displays an outstanding IR-NLO comprehensive performance, including a wide energy gap (Eg = 2.24 eV), sufficient second-harmonic-generation (SHG) efficiency (deff = 5.89 pm V−1 at 2050 nm) and strong laser-induced damage threshold (LIDT = 14.42 MW cm−2). Deeper structural and theoretical analysis suggests that the ordered arrangement of NLO-active motifs, [Ge2OS6] dimers and [FeS4] tetrahedra, makes significant contributions to the strong deff and large birefringence (Δn). This work not only demonstrates a PM Fe-based NCS material for the first time but also puts forward a new design avenue for high-performance IR-NLO materials.

Graphical abstract: Melilite oxychalcogenide Sr2FeGe2OS6: a phase-matching IR nonlinear optical material realized by isomorphous substitution

Supplementary files

Article information

Article type
Research Article
Submitted
24 Dec 2022
Accepted
18 Feb 2023
First published
20 Feb 2023
This article is Open Access
Creative Commons BY-NC license

Inorg. Chem. Front., 2023,10, 2030-2038

Melilite oxychalcogenide Sr2FeGe2OS6: a phase-matching IR nonlinear optical material realized by isomorphous substitution

H. Yang, S. Zhou, M. Ran, X. Wu, H. Lin and Q. Zhu, Inorg. Chem. Front., 2023, 10, 2030 DOI: 10.1039/D2QI02733J

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. You can use material from this article in other publications, without requesting further permission from the RSC, provided that the correct acknowledgement is given and it is not used for commercial purposes.

To request permission to reproduce material from this article in a commercial publication, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party commercial publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements