Near-infrared photon upconversion and solar synthesis using lead-free nanocrystals

Nie, Chengming; Du, Jun; Han, Yaoyao; Zhao, Guoqing; Yang, Fan; Liang, Guijie; Wu, Kaifeng

doi:10.26434/chemrxiv-2022-1hnt6-v2

Cited by 2 publications

(4 citation statements)

References 51 publications

(82 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…3,13,[50][51]111 We extract Ith=3.1 W/cm 2 from the inflection point in our excitation-density-dependent measurements (Figure 6c), which is comparable to reported systems with less-toxic NC sensitizers. 55,[108][109][110] However, only one of these systems has generated photochemically-active deep-blue light (0-0 shoulder of DPA at λ: 415 nm) from red excitation (λ: 637 nm) 13 -thus achieving a beneficially larger anti-Stokes shift (Δ𝐸=1.04 eV) relative to yellow/green excitation (λ<590nm)-and our system breaks new ground with a threshold intensity more than 10x lower. Thus, our upconversion platform built on ultra-small AZTS NCs stands as a strong candidate among the rising tide of less-toxic NC-sensitized tripletfusion systems.…”

Section: Azts Nanocrystals Sensitize Red-to-blue Triplet-fusion Upcon...mentioning

confidence: 93%

See 1 more Smart Citation

A Stepwise Reaction Achieves Emissive, Ultra-Small Ag2ZnSnS4 Nanocrystals

Villanueva

Hasham

Green

et al. 2023

Preprint

View full text Add to dashboard Cite

Pirquitasite Ag2ZnSnS4 (AZTS) nanocrystals (NCs) are emergent, lead-free emissive materials in the coinage chalcogenide family with applications in optoelectronic technologies. Like many multinary nanomaterials, their phase-pure synthesis is complicated by the generation of e.g. binary/ternary chalcogenide and metallic impurities. Here, we develop a stepwise synthetic procedure that controls the size, morphology, and transformations of acanthite (Ag2S) and canfieldite (Ag8SnS6) intermediates. This reaction scheme improves size-dispersity and grants the production of small AZTS NCs (d: 2.1-4.0 nm) that have not been achieved through established single-injection procedures expanding the accessible quantum-confined AZTS emission to shorter wavelengths (650-740 nm). We show that the initial sulfur stoichiometry is the key handle for template-size tunability and reveal that temporally separating transformation steps is crucial to obtaining <740 nm emitting AZTS NCs. We then use NMR and optical spectroscopies to demonstrate that the installation of thiol ligands improves colloidal stability and photoluminescence, while carboxylate ligands do not. Finally, facilitated by this enhanced synthetic control, we show that our ultra-small AZTS NCs can act as effective and less-toxic sensitizers for red-to-blue triplet fusion upconversion. Our results highlight transferrable insights for the synthesis and post-synthetic treatment of complex less-toxic quaternary nanocrystalline systems.

show abstract

Section: Azts Nanocrystals Sensitize Red-to-blue Triplet-fusion Upcon...mentioning

confidence: 93%

“…107 Thus, we conclude that ultra-small AZTS NCs can sensitize red-to-blue triplet fusion upconversion, adding to the short list of solution-based upconversion facilitated by less-toxic NC sensitizers. 55,[108][109][110] Scheme 2. Cartoon of the proposed upconversion mechanism.…”

Section: Azts Nanocrystals Sensitize Red-to-blue Triplet-fusion Upcon...mentioning

confidence: 99%

A Stepwise Reaction Achieves Emissive, Ultra-Small Ag2ZnSnS4 Nanocrystals

Villanueva

Hasham

Green

et al. 2023

Preprint

View full text Add to dashboard Cite

show abstract

Section: Azts Nanocrystals Sensitize Red-to-blue Triplet-fusion Upcon...mentioning

confidence: 93%

Section: Azts Nanocrystals Sensitize Red-to-blue Triplet-fusion Upcon...mentioning

confidence: 99%

A Stepwise Reaction Achieves Emissive, Ultra-Small Ag2ZnSnS4 Nanocrystals

Villanueva

Hasham

Green

et al. 2023

Preprint

View full text Add to dashboard Cite

Pirquitasite Ag2ZnSnS4 (AZTS) nanocrystals (NCs) are emergent, lead-free emissive materials in the coinage chalcogenide family with applications in optoelectronic technologies. Like many multinary nanomaterials, their phase-pure synthesis is complicated by the generation of e.g. binary/ternary chalcogenide and metallic impurities. Here, we develop a stepwise synthetic procedure that controls the size, morphology, and transformations of acanthite (Ag2S) and canfieldite (Ag8SnS6) intermediates. This reaction scheme improves size-dispersity and grants the production of small AZTS NCs (d: 2.1-4.0 nm) that have not been achieved through established single-injection procedures expanding the accessible quantum-confined AZTS emission to shorter wavelengths (650-740 nm). We show that the initial sulfur stoichiometry is the key handle for template-size tunability and reveal that temporally separating transformation steps is crucial to obtaining <740 nm emitting AZTS NCs. We then use NMR and optical spectroscopies to demonstrate that the installation of thiol ligands improves colloidal stability and photoluminescence, while carboxylate ligands do not. Finally, facilitated by this enhanced synthetic control, we show that our AZTS NCs can act as effective and less-toxic sensitizers for red-to-blue triplet fusion upconversion. Our results highlight transferrable insights for the synthesis and post-synthetic treatment of complex less-toxic quaternary nanocrystalline systems.

show abstract

Near-infrared photon upconversion and solar synthesis using lead-free nanocrystals

Cited by 2 publications

References 51 publications

A Stepwise Reaction Achieves Emissive, Ultra-Small Ag2ZnSnS4 Nanocrystals

A Stepwise Reaction Achieves Emissive, Ultra-Small Ag2ZnSnS4 Nanocrystals

A Stepwise Reaction Achieves Emissive, Ultra-Small Ag2ZnSnS4 Nanocrystals

Contact Info

Product

Resources

About