Multidegree fluorescence–optical rotatory dispersion (F-ORD) from submonolayer interfacial chiral films
- 1Department of Chemistry, Purdue University, West Lafayette, IN 47907, USA.
Abstract
Homochiral monomolecular thin films adsorbed to fused silica produced fluorescence-optical rotatory dispersion (F-ORD; i.e., optical rotation of the fluorescence emission relative to the excitation beam) more than seven orders of magnitude greater than anticipated by conventional origins of optical rotatory dispersion (i.e., optical rotation of the excitation beam after passing through a chiral film relative to its initial plane of polarization). Optical rotation of -4.5 ± 0.5° was observed in the principal axis of fluorescence emission relative to that of excitation for submonolayer dip-coated thin films of (S)-naproxen, with the sign of the rotation inverting for comparable films of (R)-naproxen. The chiral-specific F-ORD response was nonreciprocal, inverting in sign upon flipping of the sample orientation (i.e., source-facing versus detector-facing), suggesting selectivity to chiral molecules oriented at the interface. The interface selectivity, chiral selectivity, and large magnitude of the response were in excellent agreement with a fully electric-dipole-allowed orientational mechanism for chiral-specific fluorescence in uniaxial systems. These observations elevate fluorescence as a novel chiral-specific probe with exquisite sensitivity to chirality and interface specificity akin to that normally reserved for even-ordered nonlinear optical interactions, such as second harmonic and sum-frequency spectroscopy.
Related
- Lignin-Assisted Dispersion and Iohexol Retention in Lead-Free Bi2O3/Iohexol-Loaded Waterborne Polyurethane Sheets for Diagnostic X-Ray Attenuation
- Near-Infrared Fluorescence Probes for Fluorescence-Guided Surgery: Current Clinical Probes and Emerging Candidates
- Broadband chromatic-aberration-corrected metalens integrating a 1D grating structure for spectral dispersion and focusing
- Avoided-crossing engineering of quasi-BIC resonances for flat-band metadevices with suppressed angular dispersion
- Addition and Correction to “Numerical Investigation of LPG Leakage Dispersion and Explosion Consequences in a Spherical Tank with Safety Walls”
BibTeX
@article{murati2026multidegree,
title = {{Multidegree fluorescence–optical rotatory dispersion (F-ORD) from submonolayer interfacial chiral films}},
author = {Kevin Murati and Matthew R. Wilson and Isabela Capelozi de Freitas and TJ Pinedo and Benjamin W. Cerjan and Patrizia Polichetti and Alexander J. Higgins and Ethan T. Cox and Osama Abuhammad and Lyudmila V. Slipchenko and Garth J. Simpson},
journal = {Science Advances},
year = {2026},
month = oct,
doi = {10.1126/sciadv.aed0661},
url = {https://www.science.org/doi/10.1126/sciadv.aed0661},
note = {CC BY-NC},
}
RIS
TY - JOUR
TI - Multidegree fluorescence–optical rotatory dispersion (F-ORD) from submonolayer interfacial chiral films
AU - Kevin Murati
AU - Matthew R. Wilson
AU - Isabela Capelozi de Freitas
AU - TJ Pinedo
AU - Benjamin W. Cerjan
AU - Patrizia Polichetti
AU - Alexander J. Higgins
AU - Ethan T. Cox
AU - Osama Abuhammad
AU - Lyudmila V. Slipchenko
AU - Garth J. Simpson
PY - 2026
DA - 2026/10/09
JO - Science Advances
DO - 10.1126/sciadv.aed0661
UR - https://www.science.org/doi/10.1126/sciadv.aed0661
AB - Homochiral monomolecular thin films adsorbed to fused silica produced fluorescence-optical rotatory dispersion (F-ORD; i.e., optical rotation of the fluorescence emission relative to the excitation beam) more than seven orders of magnitude greater than anticipated by conventional origins of optical rotatory dispersion (i.e., optical rotation of the excitation beam after passing through a chiral film relative to its initial plane of polarization). Optical rotation of -4.5 ± 0.5° was observed in the principal axis of fluorescence emission relative to that of excitation for submonolayer dip-coated thin films of (S)-naproxen, with the sign of the rotation inverting for comparable films of (R)-naproxen. The chiral-specific F-ORD response was nonreciprocal, inverting in sign upon flipping of the sample orientation (i.e., source-facing versus detector-facing), suggesting selectivity to chiral molecules oriented at the interface. The interface selectivity, chiral selectivity, and large magnitude of the response were in excellent agreement with a fully electric-dipole-allowed orientational mechanism for chiral-specific fluorescence in uniaxial systems. These observations elevate fluorescence as a novel chiral-specific probe with exquisite sensitivity to chirality and interface specificity akin to that normally reserved for even-ordered nonlinear optical interactions, such as second harmonic and sum-frequency spectroscopy.
SN - 2375-2548
ER -