Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites

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

doi:10.1103/PhysRevLett.121.127401

Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites

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

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Abstract

Excitations of free electrons and optical phonons are known to permit access to the negative real part of relative permittivities (μ′<0) that yield strong light-matter interactions. However, negative μ′ 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 μ′ stemming from the large exciton binding energy and sizable oscillator strength. Furthermore, hyperbolic dispersion (i.e., μ′ 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. We suggest that several other van der Waals solids may exhibit similar behaviors arising from excitonic response.

Original language	English (US)
Article number	127401
Journal	Physical review letters
Volume	121
Issue number	12
DOIs	https://doi.org/10.1103/PhysRevLett.121.127401
State	Published - Sep 19 2018

Funding

We thank Dr. Pierre Darancet and Dr. Stephen K. Gray for discussions, and Liliana Stan for sputtering efforts. This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. Work at Northwestern University was supported by Grant No. SC0012541 from the U.S. Department of Energy, Office of Science (material synthesis). We thank the Northwestern University MRSEC (NSF DMR-1720139), and Flexterra Corp. for support of this research ( evaporation and characterization). This work made use of the J. B. Cohen X-Ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205). T. X. acknowledges the support from National Science Foundation (DMR-1806152 and CBET-1150617). This material is based upon work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357.

ASJC Scopus subject areas

General Physics and Astronomy

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10.1103/PhysRevLett.121.127401

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Guo, P., Huang, W., Stoumpos, C. C., Mao, L., Gong, J., Zeng, L., Diroll, B. T., Xia, Y., Ma, X., Gosztola, D. J., Xu, T., Ketterson, J. B., Bedzyk, M. J., Facchetti, A., Marks, T. J., Kanatzidis, M. G., & Schaller, R. D. (2018). Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites. Physical review letters, 121(12), Article 127401. https://doi.org/10.1103/PhysRevLett.121.127401

@article{501cebe01ee444499fb0794047b89b23,

title = "Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites",

abstract = "Excitations of free electrons and optical phonons are known to permit access to the negative real part of relative permittivities (μ′<0) that yield strong light-matter interactions. However, negative μ′ 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 μ′ stemming from the large exciton binding energy and sizable oscillator strength. Furthermore, hyperbolic dispersion (i.e., μ′ 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. We suggest that several other van der Waals solids may exhibit similar behaviors arising from excitonic response.",

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

note = "Funding Information: We thank Dr. Pierre Darancet and Dr. Stephen K. Gray for discussions, and Liliana Stan for sputtering efforts. This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. Work at Northwestern University was supported by Grant No. SC0012541 from the U.S. Department of Energy, Office of Science (material synthesis). We thank the Northwestern University MRSEC (NSF DMR-1720139), and Flexterra Corp. for support of this research ( evaporation and characterization). This work made use of the J. B. Cohen X-Ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205). T. X. acknowledges the support from National Science Foundation (DMR-1806152 and CBET-1150617). This material is based upon work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2018 American Physical Society.",

year = "2018",

month = sep,

day = "19",

doi = "10.1103/PhysRevLett.121.127401",

language = "English (US)",

volume = "121",

journal = "Physical review letters",

issn = "0031-9007",

publisher = "American Physical Society",

number = "12",

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Guo, P, Huang, W, Stoumpos, CC, Mao, L, Gong, J, Zeng, L, Diroll, BT, Xia, Y, Ma, X, Gosztola, DJ, Xu, T, Ketterson, JB , Bedzyk, MJ, Facchetti, A, Marks, TJ , Kanatzidis, MG & Schaller, RD 2018, 'Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites', Physical review letters, vol. 121, no. 12, 127401. https://doi.org/10.1103/PhysRevLett.121.127401

TY - JOUR

T1 - Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites

AU - Guo, Peijun

AU - Huang, Wei

AU - Stoumpos, Constantinos C.

AU - Mao, Lingling

AU - Gong, Jue

AU - Zeng, Li

AU - Diroll, Benjamin T.

AU - Xia, Yi

AU - Ma, Xuedan

AU - Gosztola, David J.

AU - Xu, Tao

AU - Ketterson, John B.

AU - Bedzyk, Michael J.

AU - Facchetti, Antonio

AU - Marks, Tobin J.

AU - Kanatzidis, Mercouri G.

AU - Schaller, Richard D.

N1 - Funding Information: We thank Dr. Pierre Darancet and Dr. Stephen K. Gray for discussions, and Liliana Stan for sputtering efforts. This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. Work at Northwestern University was supported by Grant No. SC0012541 from the U.S. Department of Energy, Office of Science (material synthesis). We thank the Northwestern University MRSEC (NSF DMR-1720139), and Flexterra Corp. for support of this research ( evaporation and characterization). This work made use of the J. B. Cohen X-Ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205). T. X. acknowledges the support from National Science Foundation (DMR-1806152 and CBET-1150617). This material is based upon work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2018 American Physical Society.

PY - 2018/9/19

Y1 - 2018/9/19

N2 - Excitations of free electrons and optical phonons are known to permit access to the negative real part of relative permittivities (μ′<0) that yield strong light-matter interactions. However, negative μ′ 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 μ′ stemming from the large exciton binding energy and sizable oscillator strength. Furthermore, hyperbolic dispersion (i.e., μ′ 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. We suggest that several other van der Waals solids may exhibit similar behaviors arising from excitonic response.

AB - Excitations of free electrons and optical phonons are known to permit access to the negative real part of relative permittivities (μ′<0) that yield strong light-matter interactions. However, negative μ′ 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 μ′ stemming from the large exciton binding energy and sizable oscillator strength. Furthermore, hyperbolic dispersion (i.e., μ′ 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. We suggest that several other van der Waals solids may exhibit similar behaviors arising from excitonic response.

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U2 - 10.1103/PhysRevLett.121.127401

DO - 10.1103/PhysRevLett.121.127401

M3 - Article

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VL - 121

JO - Physical review letters

JF - Physical review letters

IS - 12

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ER -

Hyperbolic Dispersion Arising from Anisotropic Excitons in Two-Dimensional Perovskites

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