Molecular polariton electroabsorption

Chiao-Yu Cheng, Nina Krainova, Alyssa N. Brigeman, Ajay Khanna, Sapana Shedge, Christine Isborn, Joel Yuen-Zhou and Noel C. Giebink ()
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Chiao-Yu Cheng: The Pennsylvania State University
Nina Krainova: The Pennsylvania State University
Alyssa N. Brigeman: The Pennsylvania State University
Ajay Khanna: University of California Merced
Sapana Shedge: University of California Merced
Christine Isborn: University of California Merced
Joel Yuen-Zhou: University of California San Diego
Noel C. Giebink: The Pennsylvania State University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract We investigate electroabsorption (EA) in organic semiconductor microcavities to understand whether strong light-matter coupling non-trivially alters their nonlinear optical [ $${\chi }^{(3)}\left(\omega,{{{{\mathrm{0,0}}}}}\right)$$ χ ( 3 ) ω , 0, 0 ] response. Focusing on strongly-absorbing squaraine (SQ) molecules dispersed in a wide-gap host matrix, we find that classical transfer matrix modeling accurately captures the EA response of low concentration SQ microcavities with a vacuum Rabi splitting of $$\hslash \Omega \approx 200$$ ℏ Ω ≈ 200 meV, but fails for high concentration cavities with $$\hslash \Omega \approx 420$$ ℏ Ω ≈ 420 meV. Rather than new physics in the ultrastrong coupling regime, however, we attribute the discrepancy at high SQ concentration to a nearly dark H-aggregate state below the SQ exciton transition, which goes undetected in the optical constant dispersion on which the transfer matrix model is based, but nonetheless interacts with and enhances the EA response of the lower polariton mode. These results indicate that strong coupling can be used to manipulate EA (and presumably other optical nonlinearities) from organic microcavities by controlling the energy of polariton modes relative to other states in the system, but it does not alter the intrinsic optical nonlinearity of the organic semiconductor inside the cavity.

Date: 2022
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DOI: 10.1038/s41467-022-35589-4

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