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  Exciton-driven change of phonon modes causes strong temperature dependent bandgap shift in nanoclusters

Muckel, F., Lorenz, S., Yang, J., Nugraha, T. A., Scalise, E., Hyeon, T., et al. (2020). Exciton-driven change of phonon modes causes strong temperature dependent bandgap shift in nanoclusters. Nature Communications, 11(1): 4127. doi:10.1038/s41467-020-17563-0.

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Exciton-driven change of phonon modes causes strong temperature dependent bandgap shift in nanoclusters - s41467-020-17563-0.pdf (Publisher version), 3MB
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Exciton-driven change of phonon modes causes strong temperature dependent bandgap shift in nanoclusters - s41467-020-17563-0.pdf
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 Creators:
Muckel, Franziska1, Author
Lorenz, Severin1, Author
Yang, Jiwoong2, 3, Author
Nugraha, Taufik Adi4, Author           
Scalise, Emilio4, Author           
Hyeon, Taeghwan2, 5, Author
Wippermann, Stefan Martin4, Author           
Bacher, Gerd1, Author           
Affiliations:
1Werkstoffe der Elektrotechnik and CENIDE, Universität Duisburg-Essen, 47057 Duisburg, Germany, ou_persistent22              
2Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul, 08826, Republic of Korea, ou_persistent22              
3Department of Energy Science & Engineering, Daegu Gyeongbuk Institute of Science & Technology (DGIST), Daegu, 42988, Republic of Korea, ou_persistent22              
4Atomistic Modelling, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863350              
5School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul, 08826, Republic of Korea, ou_persistent22              

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Free keywords: oleic acid, crystal structure; entropy; experimental study; optical property; temperature; transition element; vibration, Article; atomic emission spectrometry; circular dichroism; dispersity; energy absorption; energy dispersive X ray spectroscopy; entropy; Fourier transform; freeze drying; gas chromatography; human; hydrogen bond; infrared spectroscopy; molecular dynamics; nanotechnology; photoluminescence; photothermal therapy; simulation; temperature; X ray diffraction
 Abstract: The fundamental bandgap Eg of a semiconductor—often determined by means of optical spectroscopy—represents its characteristic fingerprint and changes distinctively with temperature. Here, we demonstrate that in magic sized II-VI clusters containing only 26 atoms, a pronounced weakening of the bonds occurs upon optical excitation, which results in a strong exciton-driven shift of the phonon spectrum. As a consequence, a drastic increase of dEg/dT (up to a factor of 2) with respect to bulk material or nanocrystals of typical size is found. We are able to describe our experimental data with excellent quantitative agreement from first principles deriving the bandgap shift with temperature as the vibrational entropy contribution to the free energy difference between the ground and optically excited states. Our work demonstrates how in small nanoparticles, photons as the probe medium affect the bandgap—a fundamental semiconductor property. © 2020, The Author(s).

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Language(s): eng - English
 Dates: 2020-08-17
 Publication Status: Issued
 Pages: -
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 Identifiers: DOI: 10.1038/s41467-020-17563-0
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 11 (1) Sequence Number: 4127 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723