@article{e96e1cd056834145bff6131663e57366,
title = "Effects of disorder on two-photon absorption in amorphous semiconductors",
abstract = "Structural disorder inherent to amorphous materials affords them unique, tailorable properties desirable for diverse applications, but our ability to exploit these phenomena is limited by a lack of understanding of complex structure-property relationships. Here we focus on nonlinear optical absorption and derive a relationship between disorder and the two-photon absorption (2PA) coefficient. We employ an open-aperture Z-scan to measure the 2PA spectra of arsenic (III) sulfide (As2S3) chalcogenide glass films processed with two solvents that impart different levels of structural disorder. We find that the effect of solvent choice on 2PA depends on the energy of the exciting photons and explain this as a consequence of bonding disorder and electron state localization. Our results demonstrate how optical nonlinearities in As2S3 can be enhanced through informed processing and present a fundamental relationship between disorder and 2PA for a generalized amorphous solid.",
author = "Dutta, {Nikita S.} and Almeida, {Juliana M.P.} and Mendon{\c c}a, {Cleber R.} and Arnold, {Craig B.}",
note = "Funding Information: The authors acknowledge useful discussions with A. Biella, G. Piccitto, R. Rota, M. Wauters, and W. Verstraelen. F.M. is supported by the FY2018 JSPS Postdoctoral Fellowship for Research in Japan. F.N. is supported in part by: NTT Research, Army Research Office (ARO) (Grant No. W911NF-18-1-0358), Japan Science and Technology Agency (JST) (via the CREST Grant No. JPMJCR1676), Japan Society for the Promotion of Science (JSPS) (via the KAKENHI Grant No. JP20H00134, JSPS-RFBR Grant No. JPJSBP120194828, and JSPS-FWO Grant No. VS.059.18N), and the Grant No. FQXi-IAF19-06 from the Foundational Questions Institute Fund (FQXi), a donor advised fund of the Silicon Valley Community Foundation. D.H. is supported by UAntwerpen/DOCPRO/34878. Part of the computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation-Flanders (FWO) and the Flemish Government department EWI. Funding Information: The authors gratefully acknowledge Leonardo de Boni, Lino Misoguti, and Andr{\'e} Romero for assistance and insight on Z-scan measurements, as well as Caitlin Azar for work on sample preparation. The authors acknowledge the use of Princeton{\textquoteright}s Imaging and Analysis Center. Princeton University & S{\~a}o Paulo Partnership Grant; Princeton University; National Science Foundation (DMR-1420541); Funda{\c c}{\~a}o de Amparo {\`a} Pesquisa do Publisher Copyright: {\textcopyright} 2020 Optical Society of America",
year = "2020",
month = jun,
day = "15",
doi = "10.1364/OL.391197",
language = "English (US)",
volume = "45",
pages = "3228--3231",
journal = "Optics Letters",
issn = "0146-9592",
publisher = "The Optical Society",
number = "12",
}