Nonthermal Plasma-Synthesized Phosphorus–Boron co-Doped Si Nanocrystals: A New Approach to Nontoxic NIR-Emitters

Limpens, Rens; Pach, Gregory F.; Neale, Nathan R.

doi:10.1021/acs.chemmater.9b00810

Title: Nonthermal Plasma-Synthesized Phosphorus–Boron co-Doped Si Nanocrystals: A New Approach to Nontoxic NIR-Emitters

Journal Article · Thu May 09 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b00810· OSTI ID:1524321

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National Renewable Energy Lab. (NREL), Golden, CO (United States)

We report on the successful creation of nonthermal plasma-synthesized phorphorus and boron co-doped Si nanocrystals (PB:Si NCs) with diameters (D_NC) ranging from 2.9 to 7.3 nm. Peak photoluminescence (PL) emission energies for all PB:Si NC diameters are ca. 400-500 meV lower than the excitonic emission values in intrinsic Si NCs, which can be attributed to prevalent donor-acceptor (D-A) transitions within the co-doped system. This D-A transition model is further evidenced by PL lifetimes within the range of 40-80 us, faster than what is observed for intrinsic Si NCs. By reducing the level of confinement within PB:Si NCs (i.e., D_NC > 4 nm), we are able to red-shift the near-infrared (NIR)-emitting D-A transitions to below the band gap of bulk Si (1.12 eV). We quantify the PL quantum yield (PLQY) for a range of DNC and show that the plasma method can achieve reasonably high PLQY values (12% for D_NC = 2.9 nm), even without any optimization of the synthesis or surface chemistry. We posit that perfect charge compensation cannot explain these results and propose a model in which dominant n-type doping accounts for the observations. Furthermore, these results demonstrate that nonthermal plasma synthesis is a viable pathway for preparing PB:Si NCs featuring NIR sub-band gap D-A transitions with relatively high quantum yields. More generally, this study provides insight into how doping affects energy and charge transfer within quantum-confined systems.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Solar Photochemistry Program; USDOE National Renewable Energy Laboratory (NREL), Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1524321

Report Number(s):: NREL/JA-5900-73281

Journal Information:: Chemistry of Materials, Vol. 31, Issue 12; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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