Excitonic effects from geometric order and disorder explain broadband optical absorption in eumelanin
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Eumelanin is a ubiquitous biological pigment, and the origin of its broadband absorption spectrum has long been a topic of scientific debate. Here, we report a first-principles computational investigation to explain its broadband absorption feature. These computations are complemented by experimental results showing a broadening of the absorption spectra of dopamine solutions upon their oxidation. We consider a variety of eumelanin molecular structures supported by experiments or theoretical studies, and calculate the absorption spectra with proper account of the excitonic couplings based on the Frenkel exciton model. The interplay of geometric order and disorder of eumelanin aggregate structures broadens the absorption spectrum and gives rise to a relative enhancement of absorption intensity at the higher-energy end, proportional to the cube of absorption energy. These findings show that the geometric disorder model is as able as the chemical disorder model, and complements this model, to describe the optical properties of eumelanin.
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DHI melanin gives a nearly monotonic absorption profile, while the DHICA polymer displays an intense absorption band in the UV region around 320 nm.
“While DHI melanin gives a nearly monotonic profile [35], the DHICA polymer displays an intense absorption band in the UV region around 320 nm [36].”
From “Fifty Shades” of Black and Red or How Carboxyl Groups Fine Tune Eumelanin and Pheomelanin Properties (2016) · cites this paper as [35]
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- Authors
- Chen, C.-T., Chuang, C., Cao, J., Ball, V., Ruch, D., & Buehler, M. J.
- Affiliations
- Massachusetts Institute of Technology (US)
- Inserm (FR)
- Centre de recherche public Henri-Tudor (LU)
- Corresponding author
- Buehler, Markus J.
- Venue
- Nature Communications
- Published
- 2014-05-22
- Volume
- 5
- Issue
- 1
- Pages
- 3859-3859
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2012184523
- Cited by
- 199
- References
- 56
- Citations by year
- 2026: 17 · 2025: 11 · 2024: 16 · 2023: 9 · 2022: 30 · 2021: 18 · 2020: 22 · 2019: 22 · 2018: 17 · 2017: 15 · 2016: 12 · 2015: 9 · 2014: 1
- FWCI
- 6.14
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Funders
- U.S. Department of Energy (DESC0001088)
- Topics
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Cell Biology › melanin and skin pigmentation
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Keywords
- eumelanin, broadband light absorption, excitonic coupling, Frenkel excitons, geometric disorder, chemical disorder, aggregate structure, dopamine oxidation, stacking interactions, biological pigments
- MeSH terms
- Dopamine, Electrons, Melanins, Oxidation-Reduction, Solutions, Spectrum Analysis, Optical Phenomena, Molecular Dynamics Simulation, Absorption, Physicochemical
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