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Title: Interface disorder in large single- and multi-shell upconverting nanocrystals

The growth of core–shell nanocrystals (NCs) can lead to extended interface disorder due to the intermixing of core and shell materials. Such an issue is particularly important for large single- and multi-shell upconverting NCs, which have been considered as being relatively insusceptible to intermixing. In this work, a robust methodology – based on structure-independent local chemical analyses with nanometer-scale resolution and high-energy synchrotron X-ray powder diffraction – has been used to shed new light on the chemical and structural organization of large single-, double-, and triple-shell upconverting NCs. Furthermore, the experimental results reveal, for the first time, that significant disorder: (i) exists at the interfaces of large (20–50 nm) multi-shell upconverting NCs; (ii) reaches core–shell and shell–shell interfaces, independently of their position within the structure; (iii) can be partially controlled by the shell deposition method; and (iv) leads to the formation of multiple length-scale interfaces depending on the size of the starting seeds, the number and relative thickness of the pre-existing shells in the seeds. It is likely that the results will be beneficial in furthering the fundamental understanding of the structure–property relationships of multi-shell upconverting NCs.
Authors:
ORCiD logo [1] ;  [2] ;  [1] ;  [3] ; ORCiD logo [4] ;  [3] ;  [2] ; ORCiD logo [5] ; ORCiD logo [5]
  1. Inst. of Microstructure Technology (IMT), Eggenstein-Leopoldshafen (Germany)
  2. Karlsruhe Inst. of Technology (KIT), Karlsruhe (Germany)
  3. Univ. of Grenoble, Grenoble (France)
  4. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  5. Inst. of Microstructure Technology (IMT), Eggenstein-Leopoldshafen (Germany); Karlsruhe Inst. of Technology (KIT), Karlsruhe (Germany)
Publication Date:
Report Number(s):
BNL-211435-2019-JAAM
Journal ID: ISSN 2050-7526
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry C
Additional Journal Information:
Journal Volume: 7; Journal Issue: 5; Journal ID: ISSN 2050-7526
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1502807
Alternate Identifier(s):
OSTI ID: 1484546

Hudry, Damien, Popescu, Radian, Busko, Dmitry, Diaz-Lopez, Maria, Abeykoon, Milinda, Bordet, Pierre, Gerthsen, Dagmar, Howard, Ian A., and Richards, Bryce S.. Interface disorder in large single- and multi-shell upconverting nanocrystals. United States: N. p., Web. doi:10.1039/C8TC05130E.
Hudry, Damien, Popescu, Radian, Busko, Dmitry, Diaz-Lopez, Maria, Abeykoon, Milinda, Bordet, Pierre, Gerthsen, Dagmar, Howard, Ian A., & Richards, Bryce S.. Interface disorder in large single- and multi-shell upconverting nanocrystals. United States. doi:10.1039/C8TC05130E.
Hudry, Damien, Popescu, Radian, Busko, Dmitry, Diaz-Lopez, Maria, Abeykoon, Milinda, Bordet, Pierre, Gerthsen, Dagmar, Howard, Ian A., and Richards, Bryce S.. 2018. "Interface disorder in large single- and multi-shell upconverting nanocrystals". United States. doi:10.1039/C8TC05130E.
@article{osti_1502807,
title = {Interface disorder in large single- and multi-shell upconverting nanocrystals},
author = {Hudry, Damien and Popescu, Radian and Busko, Dmitry and Diaz-Lopez, Maria and Abeykoon, Milinda and Bordet, Pierre and Gerthsen, Dagmar and Howard, Ian A. and Richards, Bryce S.},
abstractNote = {The growth of core–shell nanocrystals (NCs) can lead to extended interface disorder due to the intermixing of core and shell materials. Such an issue is particularly important for large single- and multi-shell upconverting NCs, which have been considered as being relatively insusceptible to intermixing. In this work, a robust methodology – based on structure-independent local chemical analyses with nanometer-scale resolution and high-energy synchrotron X-ray powder diffraction – has been used to shed new light on the chemical and structural organization of large single-, double-, and triple-shell upconverting NCs. Furthermore, the experimental results reveal, for the first time, that significant disorder: (i) exists at the interfaces of large (20–50 nm) multi-shell upconverting NCs; (ii) reaches core–shell and shell–shell interfaces, independently of their position within the structure; (iii) can be partially controlled by the shell deposition method; and (iv) leads to the formation of multiple length-scale interfaces depending on the size of the starting seeds, the number and relative thickness of the pre-existing shells in the seeds. It is likely that the results will be beneficial in furthering the fundamental understanding of the structure–property relationships of multi-shell upconverting NCs.},
doi = {10.1039/C8TC05130E},
journal = {Journal of Materials Chemistry C},
number = 5,
volume = 7,
place = {United States},
year = {2018},
month = {11}
}

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Cation Exchange Reactions in Ionic Nanocrystals
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