uu.seUppsala University Publications
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
A Spectroelectrochemical Method for Locating Fluorescence Trap States in Nanoparticles and Quantum Dots
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
2013 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 117, no 10, 5497-5504 p.Article in journal (Refereed) Published
Abstract [en]

We here devise an electrochemical method for determining the absolute energetic position of trap levels involved in fluorescence. The method utilizes potentiostatic control of the Fermi level in the material, and thereby also the electronic population of the energy states involved in the fluorescence. The method is especially useful for nanoparticle semiconductor electrodes. Here we exemplify the method by determining the position of the trap levels involved in the green fluorescence in thin films of ZnO quantum dots. The exact mechanism and the absolute positions of these states have been debated in the literature. Here we show that the visible fluorescence is caused by a transition from energy levels slightly below the conduction band edge to a deep trap within the band gap. We further pinpoint the location of the upper trap level to be at 0.35 +/- 0.03 eV below the conduction band edge. Particles between 5 and 8 nm in diameter have been analyzed, which is in the quantum confined region of ZnO. We also show that the position of the upper trap level shifts with the size of the quantum dots in the same way as the conduction band.

Place, publisher, year, edition, pages
2013. Vol. 117, no 10, 5497-5504 p.
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:uu:diva-198385DOI: 10.1021/jp31190StISI: 000316308400068OAI: oai:DiVA.org:uu-198385DiVA: diva2:616184
Available from: 2013-04-15 Created: 2013-04-15 Last updated: 2017-12-06Bibliographically approved
In thesis
1. Highly Efficient CIGS Based Devices for Solar Hydrogen Production and Size Dependent Properties of ZnO Quantum Dots
Open this publication in new window or tab >>Highly Efficient CIGS Based Devices for Solar Hydrogen Production and Size Dependent Properties of ZnO Quantum Dots
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Materials and device concepts for renewable solar hydrogen production, and size dependent properties of ZnO quantum dots are the two main themes of this thesis.

ZnO particles with diameters less than 10 nm, which are small enough for electronic quantum confinement, were synthesized by hydrolysis in alkaline zinc acetate solutions. Properties investigated include: the band gap - particle size relation, phonon quantum confinement, visible and UV-fluorescence as well as photocatalytic performance. In order to determine the absolute energetic position of the band edges and the position of trap levels involved in the visible fluorescence, methods based on combining linear sweep voltammetry and optical measurements were developed.

The large band gap of ZnO prevents absorption of visible light, and in order to construct devices capable of utilizing a larger part of the solar spectrum, other materials were also investigated, like hematite , Fe2O3, and CIGS, CuIn1-xGaxSe2.

The optical properties of hematite were investigated as a function of film thickness on films deposited by ALD. For films thinner than 20 nm, a blue shift was observed for both the absorption maximum, the indirect band gap as well as for the direct transitions. The probability for the indirect transition decreased substantially for thinner films due to a suppressed photon/phonon coupling. These effects decrease the visible absorption for films thin enough for effective charge transport in photocatalytic applications.

CIGS was demonstrated to be a highly interesting material for solar hydrogen production. CIGS based photocathodes demonstrated high photocurrents for the hydrogen evolution half reaction. The electrode stability was problematic, but was solved by introducing a modular approach based on spatial separation of the basic functionalities in the device. To construct devices capable of driving the full reaction, the possibility to use cells interconnected in series as an alternative to tandem devices were investigated. A stable, monolithic device based on three CIGS cells interconnected in series, reaching beyond 10 % STH-efficiency, was finally demonstrated. With experimental support from the CIGS-devices, the entire process of solar hydrogen production was reviewed with respect to the underlying physical processes, with special focus on the similarities and differences between various device concepts.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2014. 155 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1134
Keyword
ZnO, Nanoparticles, Quanum Dots, Size Dependent Properties, Hematite, CIGS, Solar Water Splitting, Hydrogen Production, PEC, Photoelectrochemical cells, PV-electrolysis
National Category
Inorganic Chemistry Physical Chemistry Materials Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-221260 (URN)978-91-554-8918-2 (ISBN)
Public defence
2014-05-23, Häggsalen, Ångström Laboratory, Lägehydsvägen 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2014-04-24 Created: 2014-03-27 Last updated: 2014-05-27Bibliographically approved

Open Access in DiVA

No full text

Other links

Publisher's full text

Authority records BETA

Jacobsson, T. JesperEdvinsson, Tomas

Search in DiVA

By author/editor
Jacobsson, T. JesperEdvinsson, Tomas
By organisation
Inorganic Chemistry
In the same journal
The Journal of Physical Chemistry C
Natural Sciences

Search outside of DiVA

GoogleGoogle Scholar

doi
urn-nbn

Altmetric score

doi
urn-nbn
Total: 886 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf