Growth kinetics determine the polydispersity and size of PbS and PbSe nanocrystals
A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range ( = 10 to 10 s ), at several temperatures (80-120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate) ] = 10.8 mM, [chalcogenourea] = 9.0...
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| Published in | Chemical science (Cambridge) Vol. 13; no. 16; pp. 4555 - 4565 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Royal Society of Chemistry
20.04.2022
The Royal Society of Chemistry Royal Society of Chemistry (RSC) |
| Subjects | |
| Online Access | Get full text |
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| Abstract | A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (
= 10
to 10
s
), at several temperatures (80-120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate)
] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay (
) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using
X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb
(μ
-S)
(Pb(O
CR)
)
structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. |
|---|---|
| AbstractList | A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (kr = 10−1 to 10−4 s−1), at several temperatures (80–120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate)2] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay (tind) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using in situ X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb2(μ2-S)2(Pb(O2CR)2)2 structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range ( = 10 to 10 s ), at several temperatures (80-120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate) ] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay ( ) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb (μ -S) (Pb(O CR) ) structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (kr = 10−1 to 10−4 s−1), at several temperatures (80–120 °C), under a standard set of conditions (Pb[thin space (1/6-em)]:[thin space (1/6-em)]E = 1.2[thin space (1/6-em)]:[thin space (1/6-em)]1, [Pb(oleate)2] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay (tind) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using in situ X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb2(μ2-S)2(Pb(O2CR)2)2 structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range ( k r = 10 −1 to 10 −4 s −1 ), at several temperatures (80–120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate) 2 ] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay ( t ind ) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using in situ X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb 2 (μ 2 -S) 2 (Pb(O 2 CR) 2 ) 2 structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. Colloidal lead chalcogenide nanocrystals nucleate slowly throughout their synthesis rather than in a burst. There is no correlation between the temporal width of the nucleation phase and the polydispersity. A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (k r = 10-1 to 10-4 s-1), at several temperatures (80-120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate)2] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay (t ind) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using in situ X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb2(μ2-S)2(Pb(O2CR)2)2 structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures.A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (k r = 10-1 to 10-4 s-1), at several temperatures (80-120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate)2] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay (t ind) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using in situ X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb2(μ2-S)2(Pb(O2CR)2)2 structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range ( k r = 10 −1 to 10 −4 s −1 ), at several temperatures (80–120 °C), under a standard set of conditions (Pb : E = 1.2 : 1, [Pb(oleate) 2 ] = 10.8 mM, [chalcogenourea] = 9.0 mM). An induction delay ( t ind ) is observed prior to the onset of nanocrystal absorption during which PbE solute is observed using in situ X-ray total scattering. Density functional theory models fit to the X-ray pair distribution function (PDF) support a Pb 2 (μ 2 -S) 2 (Pb(O 2 CR) 2 ) 2 structure. Absorption spectra of aliquots reveal a continuous increase in the number of nanocrystals over more than half of the total reaction time at low temperatures. A strong correlation between the width of the nucleation phase and reaction temperature is observed that does not correlate with the polydispersity. These findings are antithetical to the critical concentration dependence of nucleation that underpins the La Mer hypothesis and demonstrates that the duration of the nucleation period has a minor influence on the size distribution. The results can be explained by growth kinetics that are size dependent, more rapid at high temperature, and self limiting at low temperatures. Colloidal lead chalcogenide nanocrystals nucleate slowly throughout their synthesis rather than in a burst. There is no correlation between the temporal width of the nucleation phase and the polydispersity. |
| Author | Hendricks, Mark P Bennett, Ellie Sfeir, Matthew Y Abécassis, Benjamin McMurtry, Brandon M Ghose, Sanjit K Greenberg, Matthew W Owen, Jonathan S De Roo, Jonathan Saenz, Natalie Campos, Michael P |
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| CitedBy_id | crossref_primary_10_1021_acs_jpclett_3c02005 crossref_primary_10_1021_jacs_2c07423 crossref_primary_10_1021_acs_chemmater_2c03761 crossref_primary_10_1038_s41598_022_16666_6 crossref_primary_10_1021_acsnanoscienceau_3c00057 crossref_primary_10_1039_D3SC03384H crossref_primary_10_1107_S1600577523007300 crossref_primary_10_1021_acs_chemmater_2c01058 crossref_primary_10_1021_acsnano_3c13159 crossref_primary_10_1021_acsnano_3c02149 crossref_primary_10_1038_s44160_022_00210_5 crossref_primary_10_1021_acsnano_3c05138 crossref_primary_10_1021_acs_chemrev_3c00097 crossref_primary_10_1039_D2CC05012A crossref_primary_10_1021_acs_chemmater_1c03432 crossref_primary_10_1080_02603594_2023_2200174 crossref_primary_10_1063_5_0133809 crossref_primary_10_1021_acs_jpcc_2c06036 |
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| Snippet | A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (
= 10
to 10
s... A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range ( k r = 10 −1 to... A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (kr = 10−1 to... A library of thio- and selenourea derivatives is used to adjust the kinetics of PbE (E = S, Se) nanocrystal formation across a 1000-fold range (k r = 10-1 to... Colloidal lead chalcogenide nanocrystals nucleate slowly throughout their synthesis rather than in a burst. There is no correlation between the temporal width... |
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| SubjectTerms | Absorption spectra Chemical Sciences Chemistry Density functional theory Distribution functions High temperature Kinetics Lead selenides Low temperature Nanocrystals Nucleation Polydispersity Reaction time Size distribution |
| Title | Growth kinetics determine the polydispersity and size of PbS and PbSe nanocrystals |
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