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Voltage-Controlled Switching of Strong Light-Matter Interactions using Liquid Crystals.

ABSTRACT: We experimentally demonstrate a fine control over the coupling strength of vibrational light-matter hybrid states by controlling the orientation of a nematic liquid crystal. Through an external voltage, the liquid crystal is seamlessly switched between two orthogonal directions. Using these features, for the first time, we demonstrate electrical switching and increased Rabi splitting through transition dipole moment alignment. The C-Nstr vibration on the liquid crystal molecule is coupled to a cavity mode, and FT-IR is used to probe the formed vibropolaritonic states. A switching ratio of the Rabi splitting of 1.78 is demonstrated between the parallel and the perpendicular orientation. Furthermore, the orientational order increases the Rabi splitting by 41?% as compared to an isotropic liquid. Finally, by examining the influence of molecular alignment on the Rabi splitting, the scalar product used in theoretical modeling between light and matter in the strong coupling regime is verified.

SUBMITTER: Hertzog M

PROVIDER: S-EPMC5814857 | biostudies-other | 2017 Dec

REPOSITORIES: biostudies-other

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Voltage-Controlled Switching of Strong Light-Matter Interactions using Liquid Crystals.

Hertzog Manuel M Rudquist Per P Hutchison James A JA George Jino J Ebbesen Thomas W TW Börjesson Karl K

Chemistry (Weinheim an der Bergstrasse, Germany) 20171207 72

We experimentally demonstrate a fine control over the coupling strength of vibrational light-matter hybrid states by controlling the orientation of a nematic liquid crystal. Through an external voltage, the liquid crystal is seamlessly switched between two orthogonal directions. Using these features, for the first time, we demonstrate electrical switching and increased Rabi splitting through transition dipole moment alignment. The C-N<sub>str</sub> vibration on the liquid crystal molecule is cou ...[more]

PMID: 29155469

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Project description:Soft matter that undergoes programmed macroscopic responses to molecular analytes has potential utility in a range of health and safety-related contexts. In this study, we report the design of a nematic liquid crystal (LC) composition that forms through dimerization of carboxylic acids and responds to the presence of vapors of organoamines by undergoing a visually distinct phase transition to an isotropic phase. Specifically, we screened mixtures of two carboxylic acids, 4-butylbenzoic acid and trans-4-pentylcyclohexanecarboxylic acid, and found select compositions that exhibited a nematic phase from 30.6 to 111.7 °C during heating and 110.6 to 3.1 °C during cooling. The metastable nematic phase formed at ambient temperatures was found to be long-lived (>5 days), thus enabling the use of the LC as a chemoresponsive optical material. By comparing experimental infrared (IR) spectra of the LC phase with vibrational frequencies calculated using density functional theory (DFT), we show that it is possible to distinguish between the presence of monomers, homodimers and heterodimers in the mixture, leading us to conclude that a one-to-one heterodimer is the dominant species within this LC composition. Further support for this conclusion is obtained by using differential scanning calorimetry. Exposure of the LC to 12 ppm triethylamine (TEA) triggers a phase transition to an isotropic phase, which we show by IR spectroscopy to be driven by an acid-base reaction, leading to the formation of ammonium carboxylate salts. We characterized the dynamics of the phase transition and found that it proceeds via a characteristic spatiotemporal pathway involving the nucleation, growth, and coalescence of isotropic domains, thus amplifying the atomic-scale acid-base reaction into an information-rich optical output. In contrast to TEA, we determined via both experiment and computation that neither hydrogen bonding donor or acceptor molecules, such as water, dimethyl methylphosphonate, ethylene oxide or formaldehyde, disrupt the heterodimers formed in the LC, hinting that the phase transition (including spatial-temporal characteristics of the pathway) induced in this class of hydrogen bonded LC may offer the basis of a facile and chemically selective way of reporting the presence of volatile amines. This proposal is supported by exploratory experiments in which we show that it is possible to trigger a phase transition in the LC by exposure to volatile amines emitted from rotting fish. Overall, these results provide new principles for the design of chemoresponsive soft matter based on hydrogen bonded LCs that may find use as the basis of low-cost visual indicators of chemical environments.

Dataset Information

Voltage-Controlled Switching of Strong Light-Matter Interactions using Liquid Crystals.

Publications

Voltage-Controlled Switching of Strong Light-Matter Interactions using Liquid Crystals.

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