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Exceptional Two-Photon Absorption in Alkynylruthenium-Gold Nanoparticle Hybrids
摘要： Ruthenium alkynyl “star” complexes with tri(2-thienyl)-, tris(1,2,3-triazolyl)-, or triphenyl-benzene cores stabilize gold nanoparticles (AuNPs). Cyclic voltammetry, transmission electron microscopy, molecular modeling, dynamic light scattering, X-ray photoelectron spectroscopy, and energy-dispersive X-ray spectroscopy studies are consistent with ca. 5 trithienyl- or triazolyl-benzene-cored star complexes decorating the exterior of each AuNP. The ca. 2.5 nm diameter (by TEM) trithienylbenzene-cored gold nanoparticle hybrids are significantly less absorbing than classical Brust nanoparticles stabilized by 1-dodecanethiol; with femtosecond pulsed radiation, they exhibit exceptionally strong saturable absorption and two-photon absorption across the visible range and into the NIR region (3,000,000 GM at 500 nm, 46,000 GM at 750 nm; 1 GM = 10-50 cm4 s photon-1).
关键词： Gold nanoparticles,nonlinear optics,inorganic materials,metal alkynyl complexes,organometallics.
更新于2025-09-23 15:23:52
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Ether-soluble Cu53 Nanoclusters as an Effective Precursor of High-quality CuI Films for Optoelectronic Applications
摘要： An effective strategy is developed to synthesize high-nuclearity Cu clusters, [Cu53(RCOO)10(C≡CtBu)20Cl2H18]+ (Cu53), which is the largest Cu(I)/Cu(0) cluster reported to date. Cu powder and Ph2SiH2 are employed as the reducing agents in the synthesis. As revealed by single-crystal diffraction, Cu53 is arranged as a four-concentric-shell Cu3@Cu10Cl2@Cu20@Cu20 structure, possessing an atomic arrangement of concentric M12 icosahedral and M20 dodecahedral shells which popularly occurs in Au/Ag nanoclusters. Surprisingly, Cu53 can be dissolved in diethyl ether and spin coated to form uniform nanoclusters film on organo-lead halide perovskite. The cluster film can subsequently be converted into high-quality CuI film via in-situ iodination at room temperature. The as-fabricated CuI film proves to be an excellent hole-transport layer for fabricating highly stable CuI-based perovskite solar cells (PSCs) with 14.3% of efficiency.
关键词： CuI film,Cu nanocluster,Alkynyl,Perovskite solar cells,Superatoms
更新于2025-09-23 15:21:21
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Ether-soluble Cu53 Nanoclusters as an Effective Precursor of High-quality CuI Films for Optoelectronic Applications
摘要： An effective strategy is developed to synthesize high-nuclearity Cu clusters, [Cu53(RCOO)10(C≡CtBu)20Cl2H18]+ (Cu53), which is the largest Cu(I)/Cu(0) cluster reported to date. Cu powder and Ph2SiH2 are employed as the reducing agents in the synthesis. As revealed by single-crystal diffraction, Cu53 is arranged as a four-concentric-shell Cu3@Cu10Cl2@Cu20@Cu20 structure, possessing an atomic arrangement of concentric M12 icosahedral and M20 dodecahedral shells which popularly occurs in Au/Ag nanoclusters. Surprisingly, Cu53 can be dissolved in diethyl ether and spin coated to form uniform nanoclusters film on organo-lead halide perovskite. The cluster film can subsequently be converted into high-quality CuI film via in-situ iodination at room temperature. The as-fabricated CuI film proves to be an excellent hole-transport layer for fabricating highly stable CuI-based perovskite solar cells (PSCs) with 14.3% of efficiency.
关键词： CuI film,Cu nanocluster,Alkynyl,Perovskite solar cells,Superatoms
更新于2025-09-09 09:28:46
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Same Magic Number but Different Arrangement: Alkynyl-Protected Au25 with D3 Symmetry Jiao-Jiao Li, Zong-Jie Guan, Zhen Lei, Feng Hu, and Quan-Ming Wang*
摘要： We synthesize two homoleptic alkynyl-protected gold clusters Na[Au25(C≡CAr)18] and (Ph4P)[Au25(C≡CAr)18] (Ar = 3,5-bis(trifluoromethyl)phenyl) via direct reduction method. 1 is a magic cluster analogous to [Au25(SR)18]- in terms of electron counts and metal-to-ligand ratio. Single crystal structure analysis reveals that 1 has identical Au13 kernel to [Au25(SR)18]-, but adopts distinctly different arrangement of the six peripheral dimer staple motifs. The steric hindrance of alkynyl ligands is responsible for the D3 arrangement of Au25. The introduction of alkynyl also significantly changes the optical absorption features of the nanocluster as supported by DFT calculations. This magic cluster confirms that there is a similar but quite different parallel alkynyl-protected metal cluster universe in comparison to the thiolated one.
关键词： optical properties,gold,alkynyl ligands,cluster compounds,structure determination
更新于2025-09-09 09:28:46
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Synthesis and Photophysical Properties of Rhenium(I)-Alkynyl Molecular Rectangles
摘要： A series of highly conjugated, rigid Re(I)-based molecular rectangles {[fac-Re(CO)3Br]2(μ-bpy) (μ-L)}2 (1, L = 1,4-bis(42 -pyridylethynyl)benzene, bpeb; 2, L = 1,4-bis(42 -pyridylethynyl)naphthalene, bpen; 3, L = 1,4-bis(42 -pyridylethynyl)anthracene, bpea; and bpy = 4,42 -bipyridine) containing two different types of pyridyl ligands were synthesized, characterized and their photophysical properties studied. Successful emission color tuning was achieved by incorporating rigid alkynyl ligands into the Re(I) rectangles. Complexes 1-3 exhibited an intense absorption bands with a high e value at > 340 nm in THF solution, which is attributed to mixed two metal-to-ligand charge transfer dp(Re) → p*(bpy) and dp(Re) → p*(alkynyl)) along with ligand-to-ligand charge transfer (1LLCT)/ and intraligand charge transfer (1ILCT) transitions. Compound 1 featured a broad and structureless emission band at 619 nm, which was attributed to the emission of 3MLCT dp(Re) → p*(bpy) and/or [dp(Re) → p*(alkynyl)] characteristics with an additional luminescence at 431 nm. Whereas complexes 2 and 3 displayed an intraligand (IL) emission at 445 and 489(sh), 521 nm. These compounds represent a new class of visible light-harvesting materials that exhibit greatly enhanced emission decay lifetimes as a result of intervening ligand triplet states (3LLCT/3ILCT) present on the alkynyl appended naphthalene and anthracene chromophores, as evidenced by transient absorption spectra.
关键词： rhenium,quenching,Rectangles,alkynyl ligands,luminescence
更新于2025-09-09 09:28:46