Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites

Guo, Peijun; Huang, Wei; Stoumpos, Constantinos C.; Mao, Lingling; Gong, Jue; Zeng, Li; Diroll, Benjamin T.; Xia, Yi; Ma, Xuedan; Gosztola, David J.; Xu, Tao; Ketterson, John B.; Bedzyk, Michael J.; Facchetti, Antonio; Marks, Tobin J.; Kanatzidis, Mercouri G.; Schaller, Richard D.

doi:10.1103/PhysRevLett.121.127401

Title: Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites

Journal Article · 18 September 2018 · Physical Review Letters

DOI: https://doi.org/10.1103/PhysRevLett.121.127401 · OSTI ID:1477741

Guo, Peijun ^[1]; Huang, Wei ^[2]; Stoumpos, Constantinos C. ^[2]; Mao, Lingling ^[2]; Gong, Jue ^[3]; Zeng, Li ^[2]; Diroll, Benjamin T. ^[1]; Xia, Yi ^[1]; Ma, Xuedan ^[1]; Gosztola, David J. ^[1]; Xu, Tao ^[3]; Ketterson, John B. ^[2]; Bedzyk, Michael J. ^[2]; Facchetti, Antonio ^[4]; Marks, Tobin J. ^[2]; Kanatzidis, Mercouri G. ^[2]; Schaller, Richard D. ^[5]

Argonne National Lab. (ANL), Lemont, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Northern Illinois Univ., DeKalb, IL (United States)
Northwestern Univ., Evanston, IL (United States); Flexterra Corp., Skokie, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)

Excitations of free electrons and optical phonons are known to permit access to the negative real part of relative permittivities (ϵ' < 0) that yield strong light-matter interactions. However, negative ϵ' arising from excitons has been much less explored. Via development of a dielectric-coating based technique described herein, we report fundamental optical properties of two-dimensional hybrid perovskites (2DHPs), composed of alternating layers of inorganic and organic sublattices. Low members of 2DHPs (N = 1 and N = 2) exhibit negative ϵ' stemming from the large exciton binding energy and sizable oscillator strength. Furthermore, hyperbolic dispersion (i.e., ϵ' changes sign with directions) occurs in the visible range, which has been previously achieved only with artificial metamaterials. Such naturally occurring, exotic dispersion stems from the extremely anisotropic excitonic behaviors of 2DHPs, and can intrinsically support a large photonic density of states. Here, we suggest that several other van der Waals solids may exhibit similar behaviors arising from excitonic response.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Air Force Research Laboratory (AFRL), Air Force Office of Scientific Research (AFOSR); Northwestern University, Materials Research Science and Engineering Center (NU-MRSEC); Flexterra, Inc.

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1477741

Alternate ID(s):: OSTI ID: 1471446

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 12 Vol. 121; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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