Radiative and Nonradiative Recombination in CuInS<sub>2</sub> Nanocrystals and CuInS<sub>2</sub>-Based Core/Shell Nanocrystals

Berends, Anne C.; Rabouw, Freddy T.; Spoor, Frank C. M.; Bladt, Eva; Grozema, Ferdinand C.; Houtepen, Arjan J.; Siebbeles, Laurens D. A.; Donegá, Celso de Mello

doi:10.1021/acs.jpclett.6b01668

Cited by 121 publications

(278 citation statements)

References 56 publications

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“…We also address the size-dependence of the band gap of chalcopyrite (cp) CIS QDs by reanalyzing experimental data published by several groups. 51,52,54−57 Our results demonstrate that the molar absorption coefficients of wz CIS QDs follow a power law with an exponent of 2.45 at first exciton transition energy and scale with the QD volume at 3.1 eV.…”

mentioning

confidence: 62%

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS₂ Quantum Dots

et al. 2018

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The knowledge of the quantum dot (QD) concentration in a colloidal suspension and the quantitative understanding of the size-dependence of the band gap of QDs are of crucial importance from both applied and fundamental viewpoints. In this work, we investigate the size-dependence of the optical properties of nearly spherical wurtzite (wz) CuInS2 (CIS) QDs in the 2.7 to 6.1 nm diameter range (polydispersity ≤10%). The QDs are synthesized by partial Cu+ for In3+ cation exchange in template Cu2–xS nanocrystals, which yields CIS QDs with very small composition variations (In/Cu = 0.91 ± 0.11), regardless of their sizes. These well-defined QDs are used to investigate the size-dependence of the band gap of wz CIS QDs. A sizing curve is also constructed for chalcopyrite CIS QDs by collecting and reanalyzing literature data. We observe that both sizing curves follow primarily a 1/d dependence. Moreover, the molar absorption coefficients and the absorption cross-section per CIS formula unit, both at 3.1 eV and at the band gap, are analyzed. The results demonstrate that the molar absorption coefficients of CIS QDs follow a power law at the first exciton transition energy (εE1 = 5208d2.45) and scale with the QD volume at 3.1 eV. This latter observation implies that the absorption cross-section per unit cell at 3.1 eV is size-independent and therefore can be estimated from bulk optical constants. These results also demonstrate that the molar absorption coefficients at 3.1 eV are more reliable for analytical purposes, since they are less sensitive to size and shape dispersion.

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confidence: 62%

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS₂ Quantum Dots

et al. 2018

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“…9 This leads to relatively wide peak widths, as indicated by large full-widthhalf-maxima (FWHM) of ∼300 meV, even with size selective precipitation, and a large Stokes' shift of ∼450 meV. 10,50,69 Our aqueous phase, room temperature bio-synthesized nanocrystals display similar FWHM values of 300, 590 and 430 meV, and a Stokes shift of 400, 300 and 650 meV, for the CuInS2, (CuInZn)S and CuInS2/ZnS, particle variants respectively. Our Stokes shift values are slightly larger than those reported for analogous chemically prepared materials (cf.…”

Section: Discussionmentioning

confidence: 99%

“…61 The substantial increase in the radiative decay lifetime for the CuInS2/ZnS core/shell type quantum dots is a typical result of increased surface passivation upon growth of a shell onto core nanocrystals. 10 To demonstrate that our biomineralized CuInS2/ZnS core/ shell nanocrystals could be eff ective for bio-labeling, the as-synthesized quantum dots were conjugated to IgG antibodies using EDC/NHS cross-linkers, which then bind to the epidermal growth factor receptor (EGFR) of the THP-1 leukemia cells. THP-1 is an established cell line used for biomarker detection in cancer and contains the target receptor of interest, namely EGFR.…”

Section: 10mentioning

confidence: 99%

Enzymatic biomineralization of biocompatible CuInS₂, (CuInZn)S₂and CuInS₂/ZnS core/shell nanocrystals for bioimaging

Spangler

Chu

et al. 2017

Nanoscale

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a This work demonstrates a bioenabled fully aqueous phase and room temperature route to the synthesis of CuInS2/ZnS core/shell quantum confined nanocrystals conjugated to IgG antibodies and used for fluorescent tagging of THP-1 leukemia cells. This elegant, straightforward and green approach avoids the use of solvents, high temperatures and the necessity to phase transfer the nanocrystals prior to appli-cation.Non-toxic CuInS2, (CuInZn)S2, and CuInS2/ZnS core/shell quantum confined nanocrystals are synthesized via a biomineralization process based on a single recombinant cystathionine γ-lyase (CSE) enzyme. First, soluble In-S complexes are formed from indium acetate and H2S generated by CSE, which are then stabilized by L-cysteine in solution. The subsequent addition of copper, or both copper and zinc, precursors then results in the immediate formation of CuInS2 or (CuInZn)S2 quantum dots. Shell growth is realized through subsequent introduction of Zn acetate to the preformed core nanocrystals. The size and optical properties of the nanocrystals are tuned by adjusting the indium precursor concentration and initial incubation period. CuInS2/ZnS core/shell particles are conjugated to IgG antibodies using EDC/NHS crosslinkers and then applied in the bioimaging of THP-1 cells. Cytotoxicity tests confirm that CuInS2/ ZnS core/shell quantum dots do not cause cell death during bioimaging. Thus, this biomineralization enabled approach provides a facile, low temperature route for the fully aqueous synthesis of non-toxic CuInS2/ZnS quantum dots, which are ideal for use in bioimaging applications.

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“…[70][71][72] By controlling the reaction condition, the variation of their particle sizes, structures and compositions results in the tunability of both absorption and emission spectra. However, the limited oscillator strength of these materials near their bandgap typically prevents their use as NIR selective harvester, making them more suitable for selective UV harvesting or semitransparent (colored or opaque) applications.…”

Section: Wwwadvopticalmatdementioning

confidence: 99%

Limits of Visibly Transparent Luminescent Solar Concentrators

Yang

Lunt

2017

Advanced Optical Materials

106

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surfaces into energy harvesting resources. This new approach to visibly transparent LSCs was developed by exploiting the nature of excitonic semiconductors to optimize the use of this light-exposed surface area without compromising its existing functionality, thereby avoiding the aesthetic tradeoffs that can hinder adoption. Recent work has demonstrated devices that selectively harvest different parts of the solar spectrum including i) ultraviolet (UV) absorption, with massive downconverted luminescence deeper into the NIR (>400 nm) [4] and ii) near-infrared (NIR) absorption, with even deeper luminescence in the NIR. [3] This work has been subsequently followed by a number of other groups. [8][9][10][11][12] In contrast to transparent photovoltaics, which have also been developed to exploit this untapped area, [13][14][15] this new concentrator approach offers an alternative pathway whereby energy is transported optically, offering a simple route to large-area manufacturing, high defect tolerance, angle independent performance, and low-level energy cost. In this progress report we discuss the theoretical limits of transparent LSCs, idealized configurations, scalability, and properties of enabling materials. Operating Principles of LSCsLuminescent solar concentrators operate based on the following mechanisms (see Figure 1a): a portion of solar spectrum is absorbed in a luminescent dye (or "luminophore") [16] embedded in a transparent waveguide. That absorbed solar energy is then re-emitted at another wavelength isotropically in all directions within the waveguide, provided the oscillators are not preferentially oriented. Due to the index of refraction difference between the waveguide and the ambient environment the re-emitted photons are predominately trapped by total internal reflection, causing them to be directed towards the waveguide edges where they can be converted to electrical power in an edge mounted photovoltaic cell. The overall system power conversion efficiency, η LSC , is then given by:where η Opt is the optical efficiency (number of photons reaching the waveguide edge)/(number of photons incident on the waveguide), R is the front face reflection, η Abs is the solar spectrum Visibly transparent solar harvesting surfaces are an exciting new approach to harvesting solar energy around buildings and mobile electronics to improve their efficiency and autonomy without impacting their appearance. The recent demonstration of ultraviolet (UV) and near-infrared (NIR) selective light harvesters have enabled transparent luminescent solar concentrators (LSCs) that boast unparalleled scalability, flexibility, aesthetic quality, and affordability. Consequently, the question of the efficiency limits has emerged in these new systems. In this perspective, the theoretical efficiency limits of these concentrator systems are reviewed and practical considerations are outlined to approach these limits. For UV and UV/NIR selective harvesting single-junction transparent LSCs are constrained thermodynamically to 21%, which i...

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Radiative and Nonradiative Recombination in CuInS₂ Nanocrystals and CuInS₂-Based Core/Shell Nanocrystals

Cited by 121 publications

References 56 publications

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS₂ Quantum Dots

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS₂ Quantum Dots

Enzymatic biomineralization of biocompatible CuInS₂, (CuInZn)S₂and CuInS₂/ZnS core/shell nanocrystals for bioimaging

Limits of Visibly Transparent Luminescent Solar Concentrators

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Radiative and Nonradiative Recombination in CuInS2 Nanocrystals and CuInS2-Based Core/Shell Nanocrystals

Cited by 121 publications

References 56 publications

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS2 Quantum Dots

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS2 Quantum Dots

Enzymatic biomineralization of biocompatible CuInS2, (CuInZn)S2and CuInS2/ZnS core/shell nanocrystals for bioimaging

Limits of Visibly Transparent Luminescent Solar Concentrators

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Product

Resources

About

Radiative and Nonradiative Recombination in CuInS₂ Nanocrystals and CuInS₂-Based Core/Shell Nanocrystals

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS₂ Quantum Dots

Size-Dependent Band-Gap and Molar Absorption Coefficients of Colloidal CuInS₂ Quantum Dots

Enzymatic biomineralization of biocompatible CuInS₂, (CuInZn)S₂and CuInS₂/ZnS core/shell nanocrystals for bioimaging