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Unravelling the ultrafast charge dynamics in PbS quantum dots through resonant Auger mapping of the sulfur K-edge
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0002-6469-3374
KTH, School of Engineering Sciences (SCI), Applied Physics. Sorbonne Univ, CNRS, Inst NanoSci Paris, INSP, F-75005 Paris, France..ORCID iD: 0000-0002-6471-1093
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0002-7390-3062
Uppsala Univ, Dept Phys & Astron, Div Xray Photon Sci, Box 516, S-75120 Uppsala, Sweden..
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2022 (English)In: RSC Advances, E-ISSN 2046-2069, Vol. 12, no 49, p. 31671-31679Article in journal (Refereed) Published
Abstract [en]

There is a great fundamental interest in charge dynamics of PbS quantum dots, as they are promising for application in photovoltaics and other optoelectronic devices. The ultrafast charge transport is intriguing, offering insight into the mechanism of electron tunneling processes within the material. In this study, we investigated the charge transfer times of PbS quantum dots of different sizes and non-quantized PbS reference materials by comparing the propensity of localized or delocalized decays of sulfur 1s core hole states excited by X-rays. We show that charge transfer times in PbS quantum dots decrease with excitation energy and are similar at high excitation energy for quantum dots and non-quantized PbS. However, at low excitation energies a distinct difference in charge transfer time is observed with the fastest charge transfer in non-quantized PbS and the slowest in the smallest quantum dots. Our observations can be explained by iodide ligands on the quantum dots creating a barrier for charge transfer, which reduces the probability of interparticle transfer at low excitation energies. The probability of intraparticle charge transfer is limited by the density of available states which we describe according to a wave function in a quantum well model. The stronger quantum confinement effect in smaller PbS quantum dots is manifested as longer charge transfer times relative to the larger quantum dots at low excitation energies.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC) , 2022. Vol. 12, no 49, p. 31671-31679
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Condensed Matter Physics
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URN: urn:nbn:se:kth:diva-321909DOI: 10.1039/d2ra06091dISI: 000880040700001PubMedID: 36380927Scopus ID: 2-s2.0-85142018038OAI: oai:DiVA.org:kth-321909DiVA, id: diva2:1716658
Note

QC 20221206

Available from: 2022-12-06 Created: 2022-12-06 Last updated: 2023-12-04Bibliographically approved

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Sloboda, TamaraJohansson, FredrikKammlander, BirgitGarcia Fernandez, AlbertoCappel, Ute B.

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