Abstract
Low-dimensional chalcogenides have shown promising nonlinear optical (NLO) responses in the infrared region. Rb2Sn4Q9 (Q = S and Se) crystallizes in the noncentrosymmetric orthorhombic space group P212121. These compounds comprise an anionic layer of [Sn4Q9]2- chains separated by the Rb atoms located between the layers. Differential thermal analysis shows that Rb2Sn4Se9 melts congruently, having a melting point temperature of 472 °C and a crystallization temperature of 443 °C and no observable phase transitions, making them promising for large crystal growth. These compounds’ air- and water-stability make them more viable for application compared to the challenges faced in other promising NLO materials like γ-NaAsSe2. The Rb2Sn4S9 and Rb2Sn4Se9 have energy band gaps of 2.56 and 1.75 eV, respectively. Second harmonic generation from Rb2Sn4Q9 was found to be nonphase matchable for particle size above 75 μm, with Rb2Sn4Se9 having a χ(2) = 36.7 ± 7.4 pm/V at 1800 nm. Both materials show a high laser-induced damage threshold (LIDT) of 1.8 GW/cm2 and 0.2 GW/cm2 for the sulfide and selenide compounds, respectively, which are significantly larger than that of the benchmark reference material, AgGaSe2 (0.1 GW/cm2). The high LIDT values make these materials promising for NLO applications involving intense light-matter interactions..
Original language | English (US) |
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Pages (from-to) | 8706-8713 |
Number of pages | 8 |
Journal | Chemistry of Materials |
Volume | 35 |
Issue number | 20 |
DOIs | |
State | Published - Oct 24 2023 |
Funding
We acknowledge partial support from the Air Force Office of Scientific Research Grant number FA9550-23-1-0658. This work was also supported in part by the National Science Foundation (DMR-2305731). The IMSERC PCM facility at Northwestern University used in this work received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633) and Northwestern University. Access to facilities for high-performance computing resources at Northwestern University and of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract 477 No. DE-AC02-05CH11231 using NERSC award BES- 478 ERCAP0023827 are acknowledged. J.I.J. acknowledges the support of the Basic Science Research Programs (2021R1A2C2013625) and Basic Research Laboratory Program (2022R1S4S1033562) through the National Research Foundation of Korea (NRF), funded by the Korean government. T.S.I acknowledges the support from Materials Research Science and Engineering Centers (DMR-1720139 MRSEC).
ASJC Scopus subject areas
- General Chemistry
- General Chemical Engineering
- Materials Chemistry
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CSD 2286965: Experimental Crystal Structure Determination
Iyer, A. K. (Contributor), Ha, S. H. (Contributor), Waters, M. J. (Contributor), Ie, T. S. (Contributor), Shin, S. H. (Contributor), Rondinelli, J. M. (Contributor), Jang, J. I. (Contributor) & Kanatzidis, M. G. (Contributor), FIZ Karlsruhe - Leibniz Institute for Information Infrastructure, 2023
DOI: 10.25505/fiz.icsd.cc2grs23, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc2grs23&sid=DataCite
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