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Three-orders-of-magnitude variation of carrier lifetimes with crystal phase of gold nanoclusters

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Science  19 Apr 2019:
Vol. 364, Issue 6437, pp. 279-282
DOI: 10.1126/science.aaw8007

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Atomic packing controls exciton lifetime

Like semiconductors, small metallic clusters can absorb light and create excitons (electron-hole pairs). In ligand-capped gold clusters of 30 to 40 atoms (Au30 to Au40) that adopt the usual face-centered cubic packing, the lifetime of these excitons is ∼100 nanoseconds. Zhou et al. found that atomic packing and molecular orbital overlap can greatly affect carrier lifetimes. Despite having similar bandgaps to those of face-centered cubic clusters, a hexagonal close-packed Au30 cluster had a much shorter lifetime (∼1 nanosecond), and a body-centered cubic Au38 cluster had a lifetime of ∼5 microseconds, which is comparable to bulk silicon.

Science, this issue p. 279

Abstract

We report a three-orders-of-magnitude variation of carrier lifetimes in exotic crystalline phases of gold nanoclusters (NCs) in addition to the well-known face-centered cubic structure, including hexagonal close-packed (hcp) Au30 and body-centered cubic (bcc) Au38 NCs protected by the same type of capping ligand. The bcc Au38 NC had an exceptionally long carrier lifetime (4.7 microseconds) comparable to that of bulk silicon, whereas the hcp Au30 NC had a very short lifetime (1 nanosecond). Although the presence of ligands may, in general, affect carrier lifetimes, experimental and theoretical results showed that the drastically different recombination lifetimes originate in the different overlaps of wave functions between the tetrahedral Au4 building blocks in the hierarchical structures of these NCs.

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