Probing nearby molecular vibrations with lanthanide-doped nanocrystals.

Autor:	Mangnus MJJ; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl.; Soft Condensed Matter group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Benning VRM; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl.; Soft Condensed Matter group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Baumgartner B; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl., Prins PT; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl., van Swieten TP; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl.; Condensed Matter and Interfaces group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Dekker AJH; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl.; Soft Condensed Matter group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., van Blaaderen A; Soft Condensed Matter group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Weckhuysen BM; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl., Meijerink A; Condensed Matter and Interfaces group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Rabouw FT; Inorganic Chemistry and Catalysis group, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands. f.t.rabouw@uu.nl.; Soft Condensed Matter group, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
Jazyk:	angličtina
Zdroj:	Nanoscale [Nanoscale] 2023 Oct 26; Vol. 15 (41), pp. 16601-16611. Date of Electronic Publication: 2023 Oct 26.
DOI:	10.1039/d3nr02997b
Abstrakt:	The photoluminescence (PL) of lanthanide-doped nanocrystals can be quenched by energy transfer to vibrations of molecules located within a few nanometers from the dopants. Such short-range electronic-to-vibrational energy transfer (EVET) is often undesired as it reduces the photoluminescence efficiency. On the other hand, EVET may be exploited to extract information about molecular vibrations in the local environment of the nanocrystals. Here, we investigate the influence of solvent and gas environments on the PL properties of NaYF 4 :Er 3+ ,Yb 3+ upconversion nanocrystals. We relate changes in the PL spectrum and excited-state lifetimes in different solvents and their deuterated analogues to quenching of specific lanthanide levels by EVET to molecular vibrations. Similar but weaker changes are induced when we expose a film of nanocrystals to a gas environment with different amounts of H 2 O or D 2 O vapor. Quenching of green- and red-emitting levels of Er 3+ can be explained in terms of EVET-mediated quenching that involves molecular vibrations with energies resonant with the gap between the energy levels of the lanthanide. Quenching of the near-infrared-emitting level is more complex and may involve EVET to combination-vibrations or defect-mediated quenching. EVET-mediated quenching holds promise as a mechanism to probe the local chemical environment-both for nanocrystals dispersed in a liquid and for nanocrystals exposed to gaseous molecules that adsorb onto the nanocrystal surface.
Databáze:	MEDLINE
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