Resonance plasmonic coupling: selective enhancement of band edge emission over trap state emission of CdSe quantum dots

Paul, Livin; Thomas, Elizabeth Mariam; Chemmangat, Akshaya; Gray, Stephen K.; Thomas, K. George

doi:10.1039/d4sc04960h

Resonance plasmonic coupling: selective enhancement of band edge emission over trap state emission of CdSe quantum dots

Journal Article · Mon Nov 11 00:00:00 EST 2024 · Chemical Science

DOI:https://doi.org/10.1039/d4sc04960h· OSTI ID:2478038

Paul, Livin ^[1]; Thomas, Elizabeth Mariam ^[1]; Chemmangat, Akshaya ^[1]; Gray, Stephen K. ^[2]; ^[1]

Indian Institute of Science Education and Research Thiruvananthapuram (IISER TVM) (India)
Argonne National Laboratory (ANL), Argonne, IL (United States)

The photoluminescence properties of quantum dots (QDs) are often enhanced by eliminating surface trap states through chemical methods. Alternatively, a physical approach is presented here for improving photoluminescence purity in QDs by employing frequency-specific plasmon resonance coupling. Emitter-bound plasmonic hybrids are designed by electrostatically binding negatively charged QDs in water to positively charged gold nanoparticles having a thin polymer coating. Herein, two types of QDs are used: (i) bare CdSe, which exhibits both band edge and trap state emission, and (ii) CdSe overcoated with a ZnS shell (CdSe/ZnS) devoid of trap state emission. Tuning the extinction spectrum of the plasmonic system to match the band edge emission of CdSe enables the selective enhancement of band edge emission over trap state emission. Excellent match in the extinction spectrum of the gold nanoparticle with both, experimentally calculated photoluminescence enhancement factor and theoretically calculated radiative rate enhancement signifies the role of frequency-specific plasmon resonance coupling. Plasmon-coupled photoluminescence of CdSe/ZnS is further investigated by varying the number density of emitter on the surface of plasmonic nanoparticle. An enhancement in the photoluminescence is observed at a lower emitter density of CdSe/ZnS and the photoluminescence enhancement factor closely follows the plasmon resonance. However, photoluminescence quenching occurs with an increase in CdSe/ZnS due to plasmon-assisted nonradiative energy transfer between nearby QDs, as indicated by a red shift in the PL maximum. These studies establish that resonance plasmonic coupling is a convenient physical strategy for tuning the intrinsic photoluminescence properties of QDs for various optoelectronic applications.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2478038

Alternate ID(s):: OSTI ID: 2588033

Journal Information:: Chemical Science, Journal Name: Chemical Science Journal Issue: 48 Vol. 15; ISSN 2041-6539; ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United States

Language:: English

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