Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

Shi, Wenqin; Eijt, Stephan W.  H.; Suchand Sandeep, C. S.; Siebbeles, Laurens D.  A.; Houtepen, Arjan J.; Kinge, Sachin; Brück, Ekkes; Barbiellini, Bernardo; Bansil, Arun

doi:10.1063/1.4942609

Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

Journal Article · Wed Feb 24 00:00:00 EST 2016 · Applied Physics Letters

DOI:https://doi.org/10.1063/1.4942609· OSTI ID:1470084

Shi, Wenqin ^[1]; Eijt, Stephan W. H. ^[2]; Suchand Sandeep, C. S. ^[3]; Siebbeles, Laurens D. A. ^[3]; Houtepen, Arjan J. ^[3]; Kinge, Sachin ^[4]; Brück, Ekkes ^[2]; Barbiellini, Bernardo ^[5]; Bansil, Arun ^[5]

Delft Univ. of Technology (Netherlands). Dept. of Radiation Science and Technology. Faculty of Applied Sciences; Delft Univ. of Tech., Delft (Netherlands)
Delft Univ. of Technology (Netherlands). Dept. of Radiation Science and Technology. Faculty of Applied Sciences
Delft Univ. of Technology (Netherlands). Dept. of Chemical Engineering. Faculty of Applied Sciences
Toyota Motor Europe, Zaventem (Belgium). Materials Research and Development
Northeastern Univ., Boston, MA (United States). Dept. of Physics

Positron Two Dimensional Angular Correlation of Annihilation Radiation (2D-ACAR) measurements reveal modifications of the electronic structure and composition at the surfaces of PbSe quantum dots (QDs), deposited as thin films, produced by various ligands containing either oxygen or nitrogen atoms. In particular, the 2D-ACAR measurements on thin films of colloidal PbSe QDs capped with oleic acid ligands yield an increased intensity in the electron momentum density (EMD) at high momenta compared to PbSe quantum dots capped with oleylamine. Moreover, the EMD of PbSe QDs is strongly affected by the small ethylenediamine ligands, since these molecules lead to small distances between QDs and favor neck formation between near neighbor QDs, inducing electronic coupling between neighboring QDs. The high sensitivity to the presence of oxygen atoms at the surface can be also exploited to monitor the surface oxidation of PbSe QDs upon exposure to air. Finally, our study clearly demonstrates that positron annihilation spectroscopy applied to thin films can probe surface transformations of colloidal semiconductor QDs embedded in functional layers.

View Accepted Manuscript (DOE)

Research Organization:: Delft Univ. of Technology (Netherlands); Northeastern Univ., Boston, MA (United States); Toyota Motor Europe, Zaventem (Belgium)

Sponsoring Organization:: China Scholarship Council (CSC); Ministry of Economic Affairs (Netherlands); Toyota Motor Europe; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; FG02-07ER46352

OSTI ID:: 1470084

Alternate ID(s):: OSTI ID: 1239170

Journal Information:: Applied Physics Letters, Journal Name: Applied Physics Letters Journal Issue: 8 Vol. 108; ISSN 0003-6951

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

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