Efficient High-Order Harmonic Generation from the van der Waals Layered Crystal Copper Indium Thiophosphate.

Autor: Mushtaq A; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States., Journigan T; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States., Turkowski V; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States., Siebenaller R; Department of Materials Science and Engineering, The Ohio State University, 140W 19th Avenue, Columbus, Ohio 43210, United States.; Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States., Jeff DA; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States.; NanoScience Technology Center, University of Central Florida, Orlando, Florida 32826, United States., Truong TC; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States., Noor MY; Department of Materials Science and Engineering, The Ohio State University, 140W 19th Avenue, Columbus, Ohio 43210, United States., Khatri D; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States., Lantigua C; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States., Harrison K; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States.; NanoScience Technology Center, University of Central Florida, Orlando, Florida 32826, United States., Khondaker SI; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States.; NanoScience Technology Center, University of Central Florida, Orlando, Florida 32826, United States., Rowe E; Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States.; National Research Council, Washington, District of Columbia 20001, United States., Goldstein JT; Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States., Susner MA; Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States., Chowdhury E; Department of Materials Science and Engineering, The Ohio State University, 140W 19th Avenue, Columbus, Ohio 43210, United States., Chini M; Department of Physics, University of Central Florida, Orlando, Florida 32816, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2024 Sep 04; Vol. 146 (35), pp. 24288-24295. Date of Electronic Publication: 2024 Aug 22.
DOI: 10.1021/jacs.4c04515
Abstrakt: Layered metal thio- and selenophosphates (MTPs) are a family of van der Waals gapped materials that exhibit a multitude of functionalities in terms of magnetic, ferroelectric, and optical properties. Despite the recent progress in terms of understanding the material properties of these compounds, the potential of MTPs as a material class yet needs further scrutiny, especially in terms of nonlinear optical properties. Recent reports of efficient low-order harmonic generation and extremely high third-order nonlinear optical properties in MTPs suggest the potential application of these materials in integrated nanophotonics. In this article, we investigate the high-order nonlinear response of bulk and exfoliated thin-film crystals of copper indium thiophosphate (CIPS) to intense mid-infrared fields through experimental and computational studies of high-order harmonic generation (HHG). From a driving laser source with a 3.2 μm wavelength, we generate odd and even harmonics up to the 10th order, exceeding the bandgap of the material. We note conversion efficiencies as high as 10 -7 measured for the fifth and seventh harmonics and observe that the harmonic intensities follow a power law scaling with the driving laser intensity, suggesting a perturbative nonlinear optical origin of the observed harmonics for both bulk and thin flakes. Furthermore, first-principles calculations suggest that the generation of the highest harmonic orders results from electron-electron interactions, suggesting a correlation-mediated enhancement of the high-order optical nonlinearity.
Databáze: MEDLINE
Externí odkaz: