Abstract:We report the first observation of the reversible transformations that occur among three types of CdTe magic-size clusters (MSCs) in dispersion at room temperature and discuss our understanding of the transformation pathway. The reversible transformations were achieved with CdTe prenucleation stage samples, which were prepared with reactions of cadmium oleate [Cd(OA) 2 ] and tri-n-octylphosphine telluride in 1-octadecene and were then dispersed in mixtures of toluene and a primary amine at room temperature. Th… Show more
“…This is due to CdTeP C-371 contained in the CdTeI Ps ample added. [4,[7][8][9] CdTeM SC-371 disappeared afterwards.F rom 60 to 300 min, the change for both MSC-399 and MSC-422 was negligible as compared that shown in Part b.…”
Ararely studied transformation in colloidal ternary magic-size clusters (MSCs) is addressed. We report the first observation of the transformation from ternary CdTeSe MSC-399 to MSC-422, whichoccurs at room temperature.These two MSC types displaysharp optical absorption resonances at 399 and 422 nm, respectively,and are related in that they are quasi isomers,together with their counterpart precursor compounds (PCs). Binary CdTea nd CdSe samples were prepared in the prenucleation stage also called the induction period (IP). After they were mixed and placed in am ixture of toluene and octylamine,the transformation was found to take place and to be assisted by the addition of the CdSe IP sample.Abinary IP sample contains corresponding binary PCs and monomers (Mo) and fragments (Fr). We argue that the transformation pathway is enabled by the corresponding ternary PCs,involving the substitution reaction, namely CdTeSe PC-399 + CdSe (Mo/Fr)-1 ) CdTeSe PC-422 + CdSe (Mo/Fr)-2. The present study provides an in-depth understanding of the formation characteristics of the MSCs.
“…This is due to CdTeP C-371 contained in the CdTeI Ps ample added. [4,[7][8][9] CdTeM SC-371 disappeared afterwards.F rom 60 to 300 min, the change for both MSC-399 and MSC-422 was negligible as compared that shown in Part b.…”
Ararely studied transformation in colloidal ternary magic-size clusters (MSCs) is addressed. We report the first observation of the transformation from ternary CdTeSe MSC-399 to MSC-422, whichoccurs at room temperature.These two MSC types displaysharp optical absorption resonances at 399 and 422 nm, respectively,and are related in that they are quasi isomers,together with their counterpart precursor compounds (PCs). Binary CdTea nd CdSe samples were prepared in the prenucleation stage also called the induction period (IP). After they were mixed and placed in am ixture of toluene and octylamine,the transformation was found to take place and to be assisted by the addition of the CdSe IP sample.Abinary IP sample contains corresponding binary PCs and monomers (Mo) and fragments (Fr). We argue that the transformation pathway is enabled by the corresponding ternary PCs,involving the substitution reaction, namely CdTeSe PC-399 + CdSe (Mo/Fr)-1 ) CdTeSe PC-422 + CdSe (Mo/Fr)-2. The present study provides an in-depth understanding of the formation characteristics of the MSCs.
“…It is established that colloidal semiconductor compound magic-size clusters (MSCs) have particular precursor compounds (PCs). [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16] Thef ormer (MSC-A) exhibits distinct optical absorption peaking at ac onstant wavelength A expressed in nanometers (nm), while the latter (PC-A) is usually transparent at this wavelength Aa nd to longer wavelengths.T he MSCs and their counterpart PCs are quasi isomers and transform mutually via reversible intramolecular reorganization. Furthermore,t he transformation between types of MSCs has been observed, [1][2][3][4][5][6][7][8][9][10] following ap athway that appears to be PC-enabled comprising three key steps (Scheme S1).…”
Section: Introductionmentioning
confidence: 99%
“…[1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16] Thef ormer (MSC-A) exhibits distinct optical absorption peaking at ac onstant wavelength A expressed in nanometers (nm), while the latter (PC-A) is usually transparent at this wavelength Aa nd to longer wavelengths.T he MSCs and their counterpart PCs are quasi isomers and transform mutually via reversible intramolecular reorganization. Furthermore,t he transformation between types of MSCs has been observed, [1][2][3][4][5][6][7][8][9][10] following ap athway that appears to be PC-enabled comprising three key steps (Scheme S1). ForaMSC-A to MSC-B transformation, the three steps are MSC-A to PC-A, PC-A to PC-B,and PC-B to MSC-B.However,the reported transformations are limited to those between two binary MSCs, [3][4][5][6][7][8][9][10] or between ab inary MSC and at ernary MSC.…”
Section: Introductionmentioning
confidence: 99%
“…Furthermore,t he transformation between types of MSCs has been observed, [1][2][3][4][5][6][7][8][9][10] following ap athway that appears to be PC-enabled comprising three key steps (Scheme S1). ForaMSC-A to MSC-B transformation, the three steps are MSC-A to PC-A, PC-A to PC-B,and PC-B to MSC-B.However,the reported transformations are limited to those between two binary MSCs, [3][4][5][6][7][8][9][10] or between ab inary MSC and at ernary MSC. [1,2,5] Before the present study, transformations in ternary MSCs have not been reported.…”
Section: Introductionmentioning
confidence: 99%
“…[30][31][32] Fors emiconductor binary systems,a nI Ps ample typically contains av ariety of species,i ncluding the corresponding ME PCs, monomers (Mo), and fragments (Fr) (Scheme S2). [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16] After two binary IP samples of CdTea nd CdSe were mixed with each other, ternary CdTeSe MSC-399 was seen to evolve at room temperature when the mixture was incubated or placed in mixtures of toluene (Tol) and octylamine (OTA). [1,2] The formation of the counterpart PC for MSC-399, PC-399, occurred as described by the monomer substitution reaction given in Equation (1): [1] CdTe PC-371 þ CdSe ðMo=FrÞ)…”
Ararely studied transformation in colloidal ternary magic-size clusters (MSCs) is addressed. We report the first observation of the transformation from ternary CdTeSe MSC-399 to MSC-422, whichoccurs at room temperature.These two MSC types displaysharp optical absorption resonances at 399 and 422 nm, respectively,and are related in that they are quasi isomers,together with their counterpart precursor compounds (PCs). Binary CdTea nd CdSe samples were prepared in the prenucleation stage also called the induction period (IP). After they were mixed and placed in am ixture of toluene and octylamine,the transformation was found to take place and to be assisted by the addition of the CdSe IP sample.Abinary IP sample contains corresponding binary PCs and monomers (Mo) and fragments (Fr). We argue that the transformation pathway is enabled by the corresponding ternary PCs,involving the substitution reaction, namely CdTeSe PC-399 + CdSe (Mo/Fr)-1 ) CdTeSe PC-422 + CdSe (Mo/Fr)-2. The present study provides an in-depth understanding of the formation characteristics of the MSCs.
A fundamental understanding of formation pathways is critical to the controlled synthesis of colloidal semiconductor nanocrystals. As ultrasmall‐size quantum dots (QDs) sometimes emerge in reactions along with magic‐size clusters (MSCs), distinguishing their individual pathway of evolution is important, but has proven difficult. To decouple the evolution of QDs and MSCs, an unconventional, selective approach has been developed, along with a two‐pathway model that provides a fundamental understanding of production selectivity. For on‐demand production of either ultrasmall QDs or MSCs, the key enabler is in how to allow a reaction to proceed in the time prior to nucleation and growth of QDs. In this prenucleation stage, an intermediate compound forms, which is the precursor compound (PC) to the MSC. Here, the two‐pathway model and the manipulation of such PCs to synthesize either ultrasmall QDs or binary and ternary MSCs are highlighted. The two‐pathway model will assist the development of nucleation theory as well as provide a basis for a mechanism‐enabled design and predictive synthesis of functional nanomaterials.
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