Abstract

Exciton polaritons are quasiparticles of photons coupled strongly to bound electron-hole pairs, manifesting as an anti-crossing light dispersion near an exciton resonance. Highly anisotropic semiconductors with opposite-signed permittivities along different crystal axes are predicted to host exotic modes inside the anti-crossing called hyperbolic exciton polaritons (HEPs), which confine light subdiffractionally with enhanced density of states. Here, we show observational evidence of steady-state HEPs in the van der Waals magnet chromium sulfide bromide (CrSBr) using a cryogenic near-infrared near-field microscope. At low temperatures, in the magnetically-ordered state, anisotropic exciton resonances sharpen, driving the permittivity negative along one crystal axis and enabling HEP propagation. We characterize HEP momentum and losses in CrSBr, also demonstrating coupling to excitonic sidebands and enhancement by magnetic order: which boosts exciton spectral weight via wavefunction delocalization. Our findings open new pathways to nanoscale manipulation of excitons and light, including routes to magnetic, nonlocal, and quantum polaritonics.

Hyperbolic exciton polaritons (HEPs) are anisotropic light-matter excitations with promising applications, but their steady-state observation is challenging. Here, the authors report experimental evidence of HEPs in a van der Waals magnet, CrSBr, via cryogenic infrared near-field microscopy.

Details

Title
Hyperbolic exciton polaritons in a van der Waals magnet
Author
Ruta, Francesco L. 1   VIAFID ORCID Logo  ; Zhang, Shuai 2   VIAFID ORCID Logo  ; Shao, Yinming 2   VIAFID ORCID Logo  ; Moore, Samuel L. 2   VIAFID ORCID Logo  ; Acharya, Swagata 3 ; Sun, Zhiyuan 2   VIAFID ORCID Logo  ; Qiu, Siyuan 2 ; Geurs, Johannes 4 ; Kim, Brian S. Y. 5   VIAFID ORCID Logo  ; Fu, Matthew 2 ; Chica, Daniel G. 6 ; Pashov, Dimitar 7   VIAFID ORCID Logo  ; Xu, Xiaodong 8 ; Xiao, Di 8   VIAFID ORCID Logo  ; Delor, Milan 6 ; Zhu, X-Y. 6   VIAFID ORCID Logo  ; Millis, Andrew J. 9   VIAFID ORCID Logo  ; Roy, Xavier 6   VIAFID ORCID Logo  ; Hone, James C. 10   VIAFID ORCID Logo  ; Dean, Cory R. 2   VIAFID ORCID Logo  ; Katsnelson, Mikhail I. 11   VIAFID ORCID Logo  ; van Schilfgaarde, Mark 3 ; Basov, D. N. 2   VIAFID ORCID Logo 

 Columbia University, Department of Physics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729); Columbia University, Department of Applied Physics and Applied Mathematics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729) 
 Columbia University, Department of Physics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729) 
 National Renewable Energy Laboratory, Golden, USA (GRID:grid.419357.d) (ISNI:0000 0001 2199 3636) 
 Columbia University, Department of Physics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729); Columbia University, Columbia Nano Initiative, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729) 
 Columbia University, Department of Physics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729); Columbia University, Department of Mechanical Engineering, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729) 
 Columbia University, Department of Chemistry, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729) 
 King’s College London, Theory and Simulation of Condensed Matter, London, UK (GRID:grid.13097.3c) (ISNI:0000 0001 2322 6764) 
 University of Washington, Department of Physics, Seattle, USA (GRID:grid.34477.33) (ISNI:0000 0001 2298 6657); University of Washington, Department of Materials Science and Engineering, Seattle, USA (GRID:grid.34477.33) (ISNI:0000 0001 2298 6657) 
 Columbia University, Department of Physics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729); Flatiron Institute, Center for Computational Quantum Physics, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 7411 3681) 
10  Columbia University, Department of Mechanical Engineering, New York, USA (GRID:grid.21729.3f) (ISNI:0000 0004 1936 8729) 
11  Radboud University, Institute for Molecules and Materials, Nijmegen, Netherlands (GRID:grid.5590.9) (ISNI:0000 0001 2293 1605) 
Pages
8261
Publication year
2023
Publication date
2023
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2900961711
Copyright
© The Author(s) 2023. corrected publication 2024. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.