Homogeneously Alloyed CdSe1-xSx Quantum Dots (0 ≤ x ≤ 1)

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Presentation transcript:

Homogeneously Alloyed CdSe1-xSx Quantum Dots (0 ≤ x ≤ 1) Tangi Aubert, Marco Cirillo, Stijn Flamee, Rik Van Deun, Holger Lange, Christian Thomsen, Zeger Hens E-MRS Spring Meeting 2013, Strasbourg, France

Tuning optical properties of QDs size dependent alloyed QDs composition dependent

Alloyed QDs II-VI alloys: Cd(Se,Te), Cd(Se,S), Cd(Te,S), (Cd,Zn)Se, … core-shell gradient homogeneous Bailey et al., J. Am. Chem. Soc. 2003, 125, 7100; Swafford et al. J. Am. Chem. Soc. 2006, 128, 12299; Gurusinghe et al. J. Phys. Chem. C 2008, 112, 12795; Zheng et al. Adv. Mater. 2007, 19, 1475.

Heterogeneous Se-ODE synthesis Synthesis of CdSe, ZnSe, CuInSe2 and Cu2(Zn,Sn)Se4 QDs TC ODE carboxylic acid CdO - open air (no flushing) - T = 260°C - 5 min reaction - nearly full yield - high solid load heterogeneous Se-ODE allow large production S. Flamee, M. Cirillo, S. Abe, K. De Nolf, R. Gomes, T. Aubert, Z. Hens, submitted. S. Flamee, R. Dierick, M. Cirillo, D. Van Genechten, T. Aubert, Z. Hens, Dalton Trans. 2013. doi10.1039/c3dt50757b S. Flamee, Z. Hens, patent n°PCT/EP2012/072428, 2012.

Heterogeneous Se-ODE synthesis Heterogeneous Se-ODE vs. Homogeneous S-ODE OR heterogeneous Se-ODE homogeneous S-ODE CdSe CdS equivalent reactivities towards Cd T. Aubert, M. Cirillo, S. Flamee, R. Van Deun, H. Lange, C. Thomsen, Z. Hens, Chem. Mater., 10.1021/cm401019t

CdSe1-xSx synthesis 1-x x AND Tunable synthesis through entire composition range (0 ≤ x ≤ 1) 1-x x AND heterogeneous Se-ODE homogeneous S-ODE CdSe1-xSx T. Aubert, M. Cirillo, S. Flamee, R. Van Deun, H. Lange, C. Thomsen, Z. Hens, Chem. Mater., 10.1021/cm401019t

size = 3 nm (myristic acid) CdSe1-xSx alloyed QDs Morphology and structure (TEM) CdSe0.5S0.5 size = 3 nm (myristic acid) size can still be tuned with acid length T. Aubert, M. Cirillo, S. Flamee, R. Van Deun, H. Lange, C. Thomsen, Z. Hens, Chem. Mater., 10.1021/cm401019t

lattice parameter follows Vegard’s law CdSe1-xSx alloyed QDs Morphology and structure (XRD) lattice parameter follows Vegard’s law T. Aubert, M. Cirillo, S. Flamee, R. Van Deun, H. Lange, C. Thomsen, Z. Hens, Chem. Mater., 10.1021/cm401019t

CdSe1-xSx alloyed QDs Morphology and structure (Raman) fitted LO bands LO frequency and FWHM - LO shifts with composition - narrow FWHM for x = 0, 0.5 and 1 - large FWHM for uneven compositions homogeneous alloying

CdSe1-xSx alloyed QDs Optical properties absorption emission T. Aubert, M. Cirillo, S. Flamee, R. Van Deun, H. Lange, C. Thomsen, Z. Hens, Chem. Mater., 10.1021/cm401019t

CdSe1-xSx/CdS core-shell QDs Synthesis: layer-by-layer (SILAR) → PL enhancement decreases with increasing S content in the core Li et al., J. Am. Chem. Soc. 2003, 125, 12567.

CdSe1-xSx/CdS core-shell QDs Confinement energy: Econf (CdSe1-xSx/CdS) = Eg (CdSe1-xSx/CdS) - Eg,∞ (CdSe1-xSx) Eg,∞ (CdSe1-xSx) = (1-x)Eg (CdSe) + xEg (CdS) - bx(1-x) T. Aubert, M. Cirillo, S. Flamee, R. Van Deun, H. Lange, C. Thomsen, Z. Hens, Chem. Mater., 10.1021/cm401019t

just accepted in Chemistry of Materials, DOI: 10.1021/cm401019t Conclusion tangi.aubert@ugent.be CdSe1-xSx alloyed QDs - fast, high yield and tunable synthesis - homogeneous alloying (Raman spectroscopy) - efficient tuning of the band gap just accepted in Chemistry of Materials, DOI: 10.1021/cm401019t

Thanks for your attention ! Aknowledgement Max Kade Foundation Thanks for your attention !