Interplay between Surface Chemistry, Precursor Reactivity, and Temperature Determines Outcome of ZnS Shelling Reactions on CuInS2 Nanocrystals

ZnS shelling of I-III-VI2 nanocrystals (NCs) invariably leads to blue-shifts in both the absorption and photoluminescence spectra. These observations imply that the outcome of ZnS shelling reactions on I-III-VI2 colloidal NCs results from a complex interplay between several processes taking place in...

Ausführliche Beschreibung

Bibliographische Detailangaben
Veröffentlicht in:Chemistry of materials : a publication of the American Chemical Society. - 1998. - 30(2018), 7 vom: 10. Apr., Seite 2400-2413
1. Verfasser: Berends, Anne C (VerfasserIn)
Weitere Verfasser: van der Stam, Ward, Hofmann, Jan P, Bladt, Eva, Meeldijk, Johannes D, Bals, Sara, de Mello Donega, Celso
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2018
Zugriff auf das übergeordnete Werk:Chemistry of materials : a publication of the American Chemical Society
Schlagworte:Journal Article
LEADER 01000naa a22002652 4500
001 NLM283057637
003 DE-627
005 20231225035511.0
007 cr uuu---uuuuu
008 231225s2018 xx |||||o 00| ||eng c
024 7 |a 10.1021/acs.chemmater.8b00477  |2 doi 
028 5 2 |a pubmed24n0943.xml 
035 |a (DE-627)NLM283057637 
035 |a (NLM)29657360 
040 |a DE-627  |b ger  |c DE-627  |e rakwb 
041 |a eng 
100 1 |a Berends, Anne C  |e verfasserin  |4 aut 
245 1 0 |a Interplay between Surface Chemistry, Precursor Reactivity, and Temperature Determines Outcome of ZnS Shelling Reactions on CuInS2 Nanocrystals 
264 1 |c 2018 
336 |a Text  |b txt  |2 rdacontent 
337 |a ƒaComputermedien  |b c  |2 rdamedia 
338 |a ƒa Online-Ressource  |b cr  |2 rdacarrier 
500 |a Date Revised 06.03.2020 
500 |a published: Print-Electronic 
500 |a Citation Status PubMed-not-MEDLINE 
520 |a ZnS shelling of I-III-VI2 nanocrystals (NCs) invariably leads to blue-shifts in both the absorption and photoluminescence spectra. These observations imply that the outcome of ZnS shelling reactions on I-III-VI2 colloidal NCs results from a complex interplay between several processes taking place in solution, at the surface of, and within the seed NC. However, a fundamental understanding of the factors determining the balance between these different processes is still lacking. In this work, we address this need by investigating the impact of precursor reactivity, reaction temperature, and surface chemistry (due to the washing procedure) on the outcome of ZnS shelling reactions on CuInS2 NCs using a seeded growth approach. We demonstrate that low reaction temperatures (150 °C) favor etching, cation exchange, and alloying regardless of the precursors used. Heteroepitaxial shell overgrowth becomes the dominant process only if reactive S- and Zn-precursors (S-ODE/OLAM and ZnI2) and high reaction temperatures (210 °C) are used, although a certain degree of heterointerfacial alloying still occurs. Remarkably, the presence of residual acetate at the surface of CIS seed NCs washed with ethanol is shown to facilitate heteroepitaxial shell overgrowth, yielding for the first time CIS/ZnS core/shell NCs displaying red-shifted absorption spectra, in agreement with the spectral shifts expected for a type-I band alignment. The insights provided by this work pave the way toward the design of improved synthesis strategies to CIS/ZnS core/shell and alloy NCs with tailored elemental distribution profiles, allowing precise tuning of the optoelectronic properties of the resulting materials 
650 4 |a Journal Article 
700 1 |a van der Stam, Ward  |e verfasserin  |4 aut 
700 1 |a Hofmann, Jan P  |e verfasserin  |4 aut 
700 1 |a Bladt, Eva  |e verfasserin  |4 aut 
700 1 |a Meeldijk, Johannes D  |e verfasserin  |4 aut 
700 1 |a Bals, Sara  |e verfasserin  |4 aut 
700 1 |a de Mello Donega, Celso  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Chemistry of materials : a publication of the American Chemical Society  |d 1998  |g 30(2018), 7 vom: 10. Apr., Seite 2400-2413  |w (DE-627)NLM098194763  |x 0897-4756  |7 nnns 
773 1 8 |g volume:30  |g year:2018  |g number:7  |g day:10  |g month:04  |g pages:2400-2413 
856 4 0 |u http://dx.doi.org/10.1021/acs.chemmater.8b00477  |3 Volltext 
912 |a GBV_USEFLAG_A 
912 |a SYSFLAG_A 
912 |a GBV_NLM 
912 |a GBV_ILN_11 
912 |a GBV_ILN_350 
951 |a AR 
952 |d 30  |j 2018  |e 7  |b 10  |c 04  |h 2400-2413