Luminescence and photoelectrochemical properties of size-selected aqueous copper-doped Ag–In–S quantum dots

Raevskaya, A. E.; Rozovik, O. P.; Novikovа, A. S.; Selyshchev, Oleksandr; Stroyuk, A. L.; Dzhagan, Volodymyr; Goryacheva, Irina Yu.; Gaponik, Nikolai; Zahn, Dietrich R. T.; Eychmüller, Alexander

doi:10.1039/c8ra00257f

Cited by 55 publications

(76 citation statements)

References 41 publications

(124 reference statements)

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“…8. Summarizing, the complex of XPS and XRD data discussed show that the size selection yields a series of colloidal CZTS NCs with very similar composition but a different average size varying from 2 to 3 nm, similar to the earlier observation on the MA-capped Ag-In-S and Ag-In-S/ZnS NCs 57,58 .…”

Section: Resultssupporting

confidence: 84%

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“Green” Aqueous Synthesis and Advanced Spectral Characterization of Size-Selected Cu2ZnSnS4 Nanocrystal Inks

Stroyuk

Raevskaya

Selyshchev

et al. 2018

Sci Rep

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Structure, composition, and optical properties of colloidal mercaptoacetate-stabilized Cu2ZnSnS4 (CZTS) nanocrystal inks produced by a “green” method directly in aqueous solutions were characterized. A size-selective precipitation procedure using 2-propanol as a non-solvent allows separating a series of fractions of CZTS nanocrystals with an average size (bandgap) varying from 3 nm (1.72 eV) to 2 nm (2.04 eV). The size-selected CZTS nanocrystals revealed also phonon confinement, with the main phonon mode frequency varying by about 4 cm−1 between 2 nm and 3 nm NCs.

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Section: Resultssupporting

confidence: 84%

“…Recently, we showed the feasibility of the size-selective fractionation of MA-capped 57,58 and glutathione-capped 59 aqueous Ag-In-S/ZnS NCs into a series of bright luminophors with different emission colors using 2-propanol as a non-solvent. Here, we extend this methodology to the MA-capped CZTS NCs.…”

Section: Resultsmentioning

confidence: 99%

“Green” Aqueous Synthesis and Advanced Spectral Characterization of Size-Selected Cu2ZnSnS4 Nanocrystal Inks

Stroyuk

Raevskaya

Selyshchev

et al. 2018

Sci Rep

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“…We should note that in contrast to the ultra‐small CdS NCs, both absorption and PL excitation spectra of AIS and AIS/ZnS NCs reveal no distinct excitonic features and show the presence of broad subbandgap “tails” . Such structure of the absorption spectra makes the assessment of the bandgap quite tricky and prohibits the evaluation of the thermally‐induced shifts in the absorption/PL excitation spectra of ternary NCs.…”

Section: Resultsmentioning

confidence: 98%

“…In the present work, we tested two models for the description of the PL decay curves. The first is a conventional description of PL decay curves with linear combinations of three single‐exponential functions . It allows the average PL lifetime to be evaluated and the representative values of rate constants of radiative and non‐radiative recombination (provided the PL QY values are known) to be calculated without any assumptions on the exact emission mechanism.…”

Section: Resultsmentioning

confidence: 99%

“…We should note that in contrast to the ultra-small CdS NCs, both absorption and PL excitation spectra of AIS and AIS/ZnS NCs reveal no distinct excitonic features and show the presence of broad subbandgap "tails". [18,19,35] Such structure of the absorption spectra makes the assessment of the bandgap quite tricky and prohibits the evaluation of the thermally-induced shifts in the absorption/PL excitation spectra of ternary NCs. At the same time, we argued [16] that the broadband PL of AIS NCs can be described by a model of self-trapped excitons implying the PL band position to be directly dependent on the bandgap energy and, therefore, the changes of the PL band maximum energy can be taken as directly reflecting the temperatureinduced changes of the bandgap of AIS NCs.…”

Section: Variations Of the Pl Band Maximum Positionmentioning

confidence: 99%

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Temperature‐Dependent Photoluminescence of Silver‐Indium‐Sulfide Nanocrystals in Aqueous Colloidal Solutions

et al. 2019

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The temperature dependence of the photoluminescence (PL) intensity of colloidal semiconductor nanocrystals (NCs) makes them an appealing option in bio‐sensing applications. Here, we probed the temperature‐dependent PL behavior of aqueous glutathione (GSH)‐capped Ag−In−S (AIS) NCs and their core/shell AIS/ZnS heterostructures. We show that both core and core‐shell materials reveal strong PL quenching upon heating from 10 to 80 °C, which is completely reversible upon cooling. The PL quenching is assigned to the thermally activated dissociation of complexes formed by ligands with the metal cations on the NC surface and the introduction of water into the NC coordination sphere. This unique mechanism of the thermal PL quenching results in a much higher temperature sensitivity of the aqueous colloidal AIS (AIS/ZnS) NCs as compared with previously reported analogs capped by covalently bound ligands. Our results are expected to stimulate further studies on aqueous ternary NCs as colloidal luminescent nano‐thermometers applicable for ratiometric temperature sensing.

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Role of Copper Doping in Heavy Metal‐Free InP/ZnSe Core/Shell Quantum Dots for Highly Efficient and Stable Photoelectrochemical Cell

Zhao

Cai

et al. 2021

Advanced Energy Materials

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the emerging global energy crisis. [1] To boost the hydrogen production efficiency, the rational design and fabrication of semiconductor photoelectrodes with broad light absorption, adequate exciton generation, efficient charge separation/transfer, and long-term stability are highly desired. [2] Recently, semiconductors quantum dots (QDs) have demonstrated huge potential as light sensitizers in photoanodes for high efficiency solar-driven PEC application due to their size/shape/composition-tunable optical properties that features considerable overlap with solar spectrum. [3] However, the state-of-the-art QDs used in current PEC systems still suffer from major limitations including highly toxic heavy metal elements (Pb, Cd etc.), insufficient charge separation/transfer, and low photo-stability. [1b,4] Developing eco-friendly core/shell structured QDs is a promising strategy to address these issues, while a proper selection of core and shell materials is necessary to obtain core/shell QDs with tailored band structure, optimized optical properties/ charge dynamics, and enhanced photo/chemical stability for high performance and stable solar-to-hydrogen conversion.Among various semiconductor QDs, heavy metal-free InP QDs have recently attracted great attention due to their large absorption coefficient, narrow band gap (≈1.34 eV in bulk), and wide wavelength tunability. [5] Nevertheless, bare InP QDs can exhibit abundant surface defect states, resulting in severe non-radiative recombination for largely reduced quantum yield (QY, usually <5%) and photo/chemical stability. [6] Generally, inorganic shell (such as ZnS and ZnSe) were coated on InP core QDs to form type I band alignment with improved radiative emission and photo/chemical stability. [7] Considering the stress-induced defects at the core/shell interface, the ZnSe shell with a lower lattice mismatch (3.4%) as compared to ZnS (7.6%) is more appropriate to coat on InP core for optimized optical characteristics. [8] In 2019, Jang et al. synthesized InP/ZnSe/ZnS QDs to fabricate a red QDs-light-emitting diode (QLED) with an external quantum efficiency of 21.4%, which is considered as a milestone for the display application based on environmentally friendly QDs, demonstrating the huge potential of InP-based core/shell QDs as building blocks in optoelectronic devices. [9] However, to date, most of the investigations regarding InP-based core-shell QDs are mainly focused on enhancing As emerging eco-friendly alternatives to traditional Cd/Pb-based quantum dots (QDs), InP/ZnSe(S) core/shell QDs have demonstrated huge potential in light-emitting technologies. So far, these QDs have been rarely employed in solar energy conversion applications due to their type-I band structure offering limited photo-induced charge carrier separation and transfer. Here, a controllable Cu shell doping approach is reported to engineer the optoelectronic properties of InP/ZnSe core/shell QDs and realize high performance and stable solar-driven photoelectrochemical (PEC) hydrogen evol...

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Luminescence and photoelectrochemical properties of size-selected aqueous copper-doped Ag–In–S quantum dots

Abstract: Colloidal size-selected copper-doped Ag–In–S quantum dots were produced directly in aqueous solutions by fractionation/redispersion with a plethora of emission colors and a top luminescence quantum yield of around 60%.

Cited by 55 publications

References 41 publications

“Green” Aqueous Synthesis and Advanced Spectral Characterization of Size-Selected Cu2ZnSnS4 Nanocrystal Inks

“Green” Aqueous Synthesis and Advanced Spectral Characterization of Size-Selected Cu2ZnSnS4 Nanocrystal Inks

Temperature‐Dependent Photoluminescence of Silver‐Indium‐Sulfide Nanocrystals in Aqueous Colloidal Solutions

Role of Copper Doping in Heavy Metal‐Free InP/ZnSe Core/Shell Quantum Dots for Highly Efficient and Stable Photoelectrochemical Cell

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