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

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.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [3] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [3] ;  [2] ;  [2] ;  [4] ;  [2] ;  [2] ;  [5]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Northern Illinois Univ., DeKalb, IL (United States)
  4. Northwestern Univ., Evanston, IL (United States); Flexterra Corp., Skokie, IL (United States)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357; SC0012541
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 12; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
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.
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1477741
Alternate Identifier(s):
OSTI ID: 1471446

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., and Schaller, Richard D.. Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites. United States: N. p., Web. doi:10.1103/PhysRevLett.121.127401.
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.. Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites. United States. doi:10.1103/PhysRevLett.121.127401.
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., and Schaller, Richard D.. 2018. "Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites". United States. doi:10.1103/PhysRevLett.121.127401.
@article{osti_1477741,
title = {Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites},
author = {Guo, Peijun and Huang, Wei and Stoumpos, Constantinos C. and Mao, Lingling and Gong, Jue and Zeng, Li and Diroll, Benjamin T. and Xia, Yi and Ma, Xuedan and Gosztola, David J. and Xu, Tao and Ketterson, John B. and Bedzyk, Michael J. and Facchetti, Antonio and Marks, Tobin J. and Kanatzidis, Mercouri G. and Schaller, Richard D.},
abstractNote = {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.},
doi = {10.1103/PhysRevLett.121.127401},
journal = {Physical Review Letters},
number = 12,
volume = 121,
place = {United States},
year = {2018},
month = {9}
}

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