A 2D chiral microcavity based on apparent circular dichroism

Tzu Ling Chen; Andrew Salij; Katherine A. Parrish; Julia K. Rasch; Francesco Zinna; Paige J. Brown; Gennaro Pescitelli; Francesco Urraci; Laura A. Aronica; Abitha Dhavamani; Michael S. Arnold; Michael R. Wasielewski; Lorenzo di Bari; Roel Tempelaar; Randall H. Goldsmith

doi:10.1038/s41467-024-47411-4

A 2D chiral microcavity based on apparent circular dichroism

Tzu Ling Chen, Andrew Salij, Katherine A. Parrish, Julia K. Rasch, Francesco Zinna, Paige J. Brown, Gennaro Pescitelli, Francesco Urraci, Laura A. Aronica, Abitha Dhavamani, Michael S. Arnold, Michael R. Wasielewski, Lorenzo di Bari, Roel Tempelaar^*, Randall H. Goldsmith^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Engineering asymmetric transmission between left-handed and right-handed circularly polarized light in planar Fabry–Pérot (FP) microcavities would enable a variety of chiral light-matter phenomena, with applications in spintronics, polaritonics, and chiral lasing. Such symmetry breaking, however, generally requires Faraday rotators or nanofabricated polarization-preserving mirrors. We present a simple solution requiring no nanofabrication to induce asymmetric transmission in FP microcavities, preserving low mode volumes by embedding organic thin films exhibiting apparent circular dichroism (ACD); an optical phenomenon based on 2D chirality. Importantly, ACD interactions are opposite for counter-propagating light. Consequently, we demonstrated asymmetric transmission of cavity modes over an order of magnitude larger than that of the isolated thin film. Through circular dichroism spectroscopy, Mueller matrix ellipsometry, and simulation using theoretical scattering matrix methods, we characterize the spatial, spectral, and angular chiroptical responses of this 2D chiral microcavity.

Original language	English (US)
Article number	3072
Journal	Nature communications
Volume	15
Issue number	1
DOIs	https://doi.org/10.1038/s41467-024-47411-4
State	Published - Dec 2024

Funding

Research was primarily supported as part of the Center for Molecular Quantum Transduction, an Energy Frontier Research Center funded by U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award DE-SC0021314 (microcavity fabrication, characterization, and theory). In addition, L.D.B. acknowledges support from PRIN 2017 project \u201CCHIRALAB\u201D, grant number 20172M3K5N given by the Italian Ministry (MIUR) (PTPO synthesis), and M.S.A. acknowledges support from the Air Force Office of Scientific Research award number FA9550-23-1-0181 (apparatus for sample preparation). The authors thank Bart Kahr and Jonah Greenberg for discussions regarding the Berreman 4-by-4 matrix method and Monte Carlo simulations, respectively. We thank Dr. Nina Hong and J.A. Woollam Company for assistance with Mueller matrix spectroscopic ellipsometry measurements.

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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Chen, T. L., Salij, A., Parrish, K. A., Rasch, J. K., Zinna, F., Brown, P. J., Pescitelli, G., Urraci, F., Aronica, L. A., Dhavamani, A., Arnold, M. S., Wasielewski, M. R., di Bari, L., Tempelaar, R., & Goldsmith, R. H. (2024). A 2D chiral microcavity based on apparent circular dichroism. Nature communications, 15(1), Article 3072. https://doi.org/10.1038/s41467-024-47411-4

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title = "A 2D chiral microcavity based on apparent circular dichroism",

abstract = "Engineering asymmetric transmission between left-handed and right-handed circularly polarized light in planar Fabry–P{\'e}rot (FP) microcavities would enable a variety of chiral light-matter phenomena, with applications in spintronics, polaritonics, and chiral lasing. Such symmetry breaking, however, generally requires Faraday rotators or nanofabricated polarization-preserving mirrors. We present a simple solution requiring no nanofabrication to induce asymmetric transmission in FP microcavities, preserving low mode volumes by embedding organic thin films exhibiting apparent circular dichroism (ACD); an optical phenomenon based on 2D chirality. Importantly, ACD interactions are opposite for counter-propagating light. Consequently, we demonstrated asymmetric transmission of cavity modes over an order of magnitude larger than that of the isolated thin film. Through circular dichroism spectroscopy, Mueller matrix ellipsometry, and simulation using theoretical scattering matrix methods, we characterize the spatial, spectral, and angular chiroptical responses of this 2D chiral microcavity.",

author = "Chen, {Tzu Ling} and Andrew Salij and Parrish, {Katherine A.} and Rasch, {Julia K.} and Francesco Zinna and Brown, {Paige J.} and Gennaro Pescitelli and Francesco Urraci and Aronica, {Laura A.} and Abitha Dhavamani and Arnold, {Michael S.} and Wasielewski, {Michael R.} and {di Bari}, Lorenzo and Roel Tempelaar and Goldsmith, {Randall H.}",

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doi = "10.1038/s41467-024-47411-4",

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AU - Chen, Tzu Ling

AU - Salij, Andrew

AU - Parrish, Katherine A.

AU - Rasch, Julia K.

AU - Zinna, Francesco

AU - Brown, Paige J.

AU - Pescitelli, Gennaro

AU - Urraci, Francesco

AU - Aronica, Laura A.

AU - Dhavamani, Abitha

AU - Arnold, Michael S.

AU - Wasielewski, Michael R.

AU - di Bari, Lorenzo

AU - Tempelaar, Roel

AU - Goldsmith, Randall H.

PY - 2024/12

Y1 - 2024/12

N2 - Engineering asymmetric transmission between left-handed and right-handed circularly polarized light in planar Fabry–Pérot (FP) microcavities would enable a variety of chiral light-matter phenomena, with applications in spintronics, polaritonics, and chiral lasing. Such symmetry breaking, however, generally requires Faraday rotators or nanofabricated polarization-preserving mirrors. We present a simple solution requiring no nanofabrication to induce asymmetric transmission in FP microcavities, preserving low mode volumes by embedding organic thin films exhibiting apparent circular dichroism (ACD); an optical phenomenon based on 2D chirality. Importantly, ACD interactions are opposite for counter-propagating light. Consequently, we demonstrated asymmetric transmission of cavity modes over an order of magnitude larger than that of the isolated thin film. Through circular dichroism spectroscopy, Mueller matrix ellipsometry, and simulation using theoretical scattering matrix methods, we characterize the spatial, spectral, and angular chiroptical responses of this 2D chiral microcavity.

AB - Engineering asymmetric transmission between left-handed and right-handed circularly polarized light in planar Fabry–Pérot (FP) microcavities would enable a variety of chiral light-matter phenomena, with applications in spintronics, polaritonics, and chiral lasing. Such symmetry breaking, however, generally requires Faraday rotators or nanofabricated polarization-preserving mirrors. We present a simple solution requiring no nanofabrication to induce asymmetric transmission in FP microcavities, preserving low mode volumes by embedding organic thin films exhibiting apparent circular dichroism (ACD); an optical phenomenon based on 2D chirality. Importantly, ACD interactions are opposite for counter-propagating light. Consequently, we demonstrated asymmetric transmission of cavity modes over an order of magnitude larger than that of the isolated thin film. Through circular dichroism spectroscopy, Mueller matrix ellipsometry, and simulation using theoretical scattering matrix methods, we characterize the spatial, spectral, and angular chiroptical responses of this 2D chiral microcavity.

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A 2D chiral microcavity based on apparent circular dichroism

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