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Records |
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Author |
Xia, C.; Pedrazo-Tardajos, A.; Wang, D.; Meeldijk, J.D.; Gerritsen, H.C.; Bals, S.; de Donega, C.M. |
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Title |
Seeded growth combined with cation exchange for the synthesis of anisotropic Cu2-xS/ZnS, Cu2-xS, and CuInS2 nanorods |
Type |
A1 Journal article |
| |
Year  |
2021 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
33 |
Issue |
1 |
Pages |
102-116 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal copper(I) sulfide (Cu2-xS) nanocrystals (NCs) have attracted much attention for a wide range of applications because of their unique optoelectronic properties, driving scientists to explore the potential of using Cu2-xS NCs as seeds in the synthesis of heteronanocrystals to achieve new multifunctional materials. Herein, we developed a multistep synthesis strategy toward Cu2-xS/ZnS heteronanorods. The Janus-type Cu2-xS/ZnS heteronanorods are obtained by the injection of hexagonal high-chalcocite Cu2-xS seed NCs in a hot zinc oleate solution in the presence of suitable surfactants, 20 s after the injection of sulfur precursors. The Cu2-xS seed NCs undergo rapid aggregation and coalescence in the first few seconds after the injection, forming larger NCs that act as the effective seeds for heteronucleation and growth of ZnS. The ZnS heteronucleation occurs on a single (100) facet of the Cu2-xS seed NCs and is followed by fast anisotropic growth along a direction that is perpendicular to the c-axis, thus leading to Cu2-xS/ZnS Janus-type heteronanorods with a sharp heterointerface. Interestingly, the high-chalcocite crystal structure of the injected Cu2-xS seed NCs is preserved in the Cu2-xS segments of the heteronanorods because of the highthermodynamic stability of this Cu2-xS phase. The Cu2-xS/ZnS heteronanorods are subsequently converted into single-component Cu2-xS and CuInS2 nanorods by postsynthetic topotactic cation exchange. This work expands the possibilities for the rational synthesis of colloidal multicomponent heteronanorods by allowing the design principles of postsynthetic heteroepitaxial seeded growth and nanoscale cation exchange to be combined, yielding access to a plethora of multicomponent heteronanorods with diameters in the quantum confinement regime. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Editor |
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Wos |
000610984700009 |
Publication Date |
2020-12-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
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ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
C.X. acknowledges China Scholarship Council (CSC) for the financial support (grant number 201406330055). C.d.M.D. acknowledges funding from the European Commission for access to the EMAT facilities (grant number EUSMI E180900184). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. acknowledges support by means of the ERC Consolidator grant no. 815128 REALNANO. The authors thank Donglong Fu for XRD measurements.; sygma |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:176587 |
Serial |
6732 |
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| Permanent link to this record |
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Author |
Hinterding, S.O.M.; Berends, A.C.; Kurttepeli, M.; Moret, M.-E.; Meeldijk, J.D.; Bals, S.; van der Stam, W.; de Donega, C.M. |
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Title |
Tailoring Cu+ for Ga3+ cation exchange in Cu2-xS and CuInS2 nanocrystals by controlling the Ga precursor chemistry |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
13 |
Issue |
13 |
Pages |
12880-12893 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoscale cation exchange (CE) has resulted in colloidal nanomaterials that are unattainable by direct synthesis methods. Aliovalent CE is complex and synthetically challenging because the exchange of an unequal number of host and guest cations is required to maintain charge balance. An approach to control aliovalent CE reactions is the use of a single reactant to both supply the guest cation and extract the host cation. Here, we study the application of GaCl3-L complexes [L = trioctylphosphine (TOP), triphenylphosphite (TPP), diphenylphosphine (DPP)] as reactants in the exchange of Cu+ for Ga3+ in Cu2-xS nanocrystals. We find that noncomplexed GaCl3 etches the nanocrystals by S2- extraction, whereas GaCl3-TOP is unreactive. Successful exchange of Cu+ for Ga3+ is only possible when GaCl3 is complexed with either TPP or DPP. This is attributed to the pivotal role of the Cu2-xS-GaCl3-L activated complex that forms at the surface of the nanocrystal at the onset of the CE reaction, which must be such that simultaneous Ga3+ insertion and Cu+ extraction can occur. This requisite is only met if GaCl3 is bound to a phosphine ligand, with a moderate bond strength, to allow facile dissociation of the complex at the nanocrystal surface. The general validity of this mechanism is demonstrated by using GaCl3-DPP to convert CuInS2 into (Cu,Ga,In)S-2 nanocrystals, which increases the photoluminescence quantum yield 10 -fold, while blue -shifting the photoluminescence into the NIR biological window. This highlights the general applicability of the mechanistic insights provided by our work. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000500650000061 |
Publication Date |
2019-10-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
27 |
Open Access |
OpenAccess |
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Notes |
; S.O.M.H., W.v.d.S., A.C.B., and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant Nos. ECHO.712.012.0001 and ECHO.712.014.001. S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant No. 815128-REALNANO). S.O.M.H. is supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. DFT calculations were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. This work was sponsored by NWO Physical Sciences for the use of supercomputer facilities. The authors thank Jessi van der Hoeven for EDS and TEM measurements. ; sygma |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:165149 |
Serial |
6324 |
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Author |
Brodu, A.; Ballottin, M.V.; Buhot, J.; van Harten, E.J.; Dupont, D.; La Porta, A.; Prins, P.T.; Tessier, M.D.; Versteegh, M.A.M.; Zwiller, V.; Bals, S.; Hens, Z.; Rabouw, F.T.; Christianen, P.C.M.; de Donega, C.M.; Vanmaekelbergh, D. |
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Title |
Exciton Fine Structure and Lattice Dynamics in InP/ZnSe Core/Shell Quantum Dots |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS Photonics |
Abbreviated Journal |
Acs Photonics |
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Volume |
5 |
Issue |
5 |
Pages |
3353-3362 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanocrystalline InP quantum dots (QDs) hold promise for heavy-metal-free optoelectronic applications due to their bright and size tunable emission in the visible range. Photochemical stability and high photoluminescence (PL) quantum yield are obtained by a diversity of epitaxial shells around the InP core. To understand and optimize the emission line shapes, the exciton fine structure of InP core/shell QD systems needs be investigated. Here, we study the exciton fine structure of InP/ZnSe core/shell QDs with core diameters ranging from 2.9 to 3.6 nm (PL peak from 2.3 to 1.95 eV at 4 K). PL decay measurements as a function of temperature in the 10 mK to 300 K range show that the lowest exciton fine structure state is a dark state, from which radiative recombination is assisted by coupling to confined acoustic phonons with energies ranging from 4 to 7 meV, depending on the core diameter. Circularly polarized fluorescence line-narrowing (FLN) spectroscopy at 4 K under high magnetic fields (up to 30 T) demonstrates that radiative recombination from the dark F = +/- 2 state involves acoustic and optical phonons, from both the InP core and the ZnSe shell. Our data indicate that the highest intensity FLN peak is an acoustic phonon replica rather than a zero-phonon line, implying that the energy separation observed between the F = +/- 1 state and the highest intensity peak in the FLN spectra (6 to 16 meV, depending on the InP core size) is larger than the splitting between the dark and bright fine structure exciton states. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000442185900049 |
Publication Date |
2018-07-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2330-4022 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.756 |
Times cited |
40 |
Open Access |
OpenAccess |
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Notes |
; We acknowledge the support of the HFML-RU/FOM, member of the European Magnetic Field Laboratory (EMFL). D.V. and Z.H. acknowledge support by the European Commission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656) and the Marie Sklodowska-Curie Action Compass (H2020 MSCA-RISE-691185). Z.H. acknowledges the Research Foundation Flanders (project 17006602) and Ghent University (GOA no. 01G01513). Z.H. and S.B. acknowledge SIM vzw (SBO-QDOCCO). F.T.R. acknowledges financial support from The Netherlands Organisation for Scientific Research NWO (Gravitation program Multiscale Catalytic Energy Conversion and VENI grant number 722.017.002). This work was also supported by the Dutch NWO-Physics Program DDC13, ERC Advanced Grant 692691 “First step”, and ERC Starting Grant 335078 “COLOURATOM”. ; ecas_sara |
Approved |
Most recent IF: 6.756 |
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Call Number |
UA @ lucian @ c:irua:153753UA @ admin @ c:irua:153753 |
Serial |
5100 |
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| Permanent link to this record |
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Author |
Berends, A.C.; van der Stam, W.; Hofmann, J.P.; Bladt, E.; Meeldijk, J.D.; Bals, S.; de Donega, C.M. |
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Title |
Interplay between surface chemistry, precursor reactivity, and temperature determines outcome of ZnS shelling reactions on CuInS2 nanocrystals |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
30 |
Issue |
30 |
Pages |
2400-2413 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
ZnS shelling of I-III-VI(2 )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 degrees 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 degrees 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. |
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Corporate Author |
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Thesis |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
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Language |
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Wos |
000430023700027 |
Publication Date |
2018-03-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
85 |
Open Access |
OpenAccess |
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Notes |
; Annelies van der Bok is gratefully acknowledged for performing the ICP measurements. A.C.B. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant No. ECHO.712.014.001. S.B. and E.B. acknowledge financial support from European Research Council (ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara |
Approved |
Most recent IF: 9.466 |
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Call Number |
UA @ lucian @ c:irua:150772UA @ admin @ c:irua:150772 |
Serial |
4972 |
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Author |
Berends, A.C.; Rabouw, F.T.; Spoor, F.C.M.; Bladt, E.; Grozema, F.C.; Houtepen, A.J.; Siebbeles, L.D.A.; de Donega, C.M. |
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Title |
Radiative and nonradiative recombination in CuInS2 nanocrystals and CuInS2-based core/shell nanocrystals |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
The journal of physical chemistry letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
7 |
Issue |
7 |
Pages |
3503-3509 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Luminescent copper indium sulfide (CIS) nanocrystals are a potential solution to the toxicity issues associated with Cd- and Pb-based nanocrystals. However, the development of high-quality CIS nanocrystals has been complicated by insufficient knowledge of the electronic structure and of the factors that lead to luminescence quenching. Here we investigate the exciton decay pathways in CIS nanocrystals using time resolved photoluminescence and transient absorption spectroscopy. Core-only CIS nanocrystals with low quantum yield are compared to core/shell nanocrystals (CIS/ZnS and CIS/CdS) with higher quantum yield. Our measurements support the model of photoluminescence by radiative recombination of a conduction band electron with a localized hole. Moreover, we find that photoluminescence quenching in low-quantum-yield nanocrystals involves initially uncoupled decay pathways for the electron and hole. The electron decay pathway determines whether the exciton recombines radiatively or nonradiatively. The development of high-quality CIS nanocrystals should therefore focus on the elimination of electron traps. |
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Corporate Author |
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Thesis |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
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Language |
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Wos |
000382603300037 |
Publication Date |
2016-08-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1948-7185 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.353 |
Times cited |
67 |
Open Access |
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Notes |
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Approved |
Most recent IF: 9.353 |
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Call Number |
UA @ lucian @ c:irua:135715 |
Serial |
4308 |
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Author |
van der Stam, W.; Berends, A.C.; Rabouw, F.T.; Willhammar, T.; Ke, X.; Meeldijk, J.D.; Bals, S.; de Donega, C.M. |
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Title |
Luminescent CuInS2 quantum dots by partial cation exchange in Cu2-xS nanocrystals |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
27 |
Issue |
27 |
Pages |
621-628 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Here, we show successful partial cation exchange reactions in Cu2-xS nanocrystals (NCs) yielding luminescent CuInS2 (CIS) NCs. Our approach of mild reaction conditions ensures slow Cu extraction rates, which results in a balance with the slow In incorporation rate. With this method, we obtain CIS NCs with photoluminescence (PL) far in the near-infrared (NIR), which cannot be directly synthesized by currently available synthesis protocols. We discuss the factors that favor partial, self-limited cation exchange from Cu2-xS to CIS NCs, rather than complete cation exchange to In2S3. The product CIS NCs have the wurtzite crystal structure, which is understood in terms of conservation of the hexagonal close packing of the anionic sublattice of the parent NCs into the product NCs. These results are an important step toward the design of CIS NCs with sizes and shapes that are not attainable by direct synthesis protocols and may thus impact a number of potential applications. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000348618400028 |
Publication Date |
2014-12-29 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
119 |
Open Access |
OpenAccess |
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Notes |
335078 Colouratom; 262348 Esmi; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:125291 |
Serial |
1858 |
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Author |
van der Stam, W.; Akkerman, Q.A.; Ke, X.; van Huis, M.A.; Bals, S.; de Donega, C.M. |
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Title |
Solution-processable ultrathin size- and shape-controlled colloidal Cu2-xS nanosheets |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
27 |
Issue |
27 |
Pages |
283-291 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Ultrathin two-dimensional (2D) nanosheets (NSs) possess extraordinary properties that are attractive for both fundamental studies and technological devices. Solution-based bottom-up methods are emerging as promising routes to produce free-standing NSs, but the synthesis of colloidal NSs with well-defined size and shape has remained a major challenge. In this work, we report a novel method that yields 2 nm thick colloidal Cu2-xS NSs with well-defined shape (triangular or hexagonal) and size (100 nm to 3 mu m). The key feature of our approach is the use of a synergistic interaction between halides (Br or Cl) and copper-thiolate metal-organic frameworks to create a template that imposes 2D constraints on the Cu-catalyzed C-S thermolysis, resulting in nucleation and growth of colloidal 2D Cu2-xS NSs. Moreover, the NS composition can be postsynthetically tailored by exploiting topotactic cation exchange reactions. This is illustrated by converting the Cu2-xS NSs into ZnS and CdS NSs while preserving their size and shape. The method presented here thus holds great promise as a route to solution-processable compositionally diverse ultrathin colloidal NSs with well-defined shape and size. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000348085300036 |
Publication Date |
2014-12-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
68 |
Open Access |
OpenAccess |
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Notes |
335078 Colouratom; 246791 Countatoms; 312483 Esteem2; esteem2ta; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:123865 c:irua:123865 |
Serial |
3052 |
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| Permanent link to this record |
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Author |
Hutter, E.M.; Bladt, E.; Goris, B.; Pietra, F.; van der Bok, J.C.; Boneschanscher, M.P.; de Donega, C.M.; Bals, S.; Vanmaekelbergh, D. |
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Title |
Conformal and atomic characterization of ultrathin CdSe platelets with a helical shape |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Nano letters |
Abbreviated Journal |
Nano Lett |
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Volume |
14 |
Issue |
11 |
Pages |
6257-6262 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Currently, ultrathin colloidal CdSe semiconductor nanoplatelets (NPLs) with a uniform thickness that is controllable up to the atomic scale can be prepared. The optical properties of these 2D semiconductor systems are the subject of extensive research. Here, we reveal their natural morphology and atomic arrangement. Using cryo-TEM (cryo-transmission electron microscopy), we show that the shape of rectangular NPLs in solution resembles a helix. Fast incorporation of these NPLs in silica preserves and immobilizes their helical shape, which allowed us to perform an in-depth study by high angle annular dark field scanning transmission electron microscopy (HAADF-STEM). Electron tomography measurements confirm and detail the helical shape of these systems. Additionally, high-resolution HAADF-STEM shows the thickness of the NPLs on the atomic scale and furthermore that these are consistently folded along a ?110? direction. The presence of a silica shell on both the top and bottom surfaces shows that Cd atoms must be accessible for silica precursor (and ligand) molecules on both sides. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington |
Editor |
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Language |
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Wos |
000345723800036 |
Publication Date |
2014-10-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1530-6984 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.712 |
Times cited |
43 |
Open Access |
OpenAccess |
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Notes |
Dariusz Mitoraj, Hans Meeldijk, Relinde van Dijk-Moes, and Stephan Zevenhuizen are acknowledged for technical support and help with some experiments. The research leading to these results has received funding from the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement no. 291667. The authors acknowledge financial support from FOM and NOW [FOM program Functional NanoParticle Solids (FNPS)]. S.B. acknowledges financial support from European Research Council (ERC Starting Grant #335078- COLOURATOMS). E.B. and B.G. gratefully acknowledge financial support by the Flemish Fund for Scientific Research (FWO Vlaanderen).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 12.712; 2014 IF: 13.592 |
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Call Number |
UA @ lucian @ c:irua:122209 |
Serial |
490 |
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| Permanent link to this record |
