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Probing and Controlling Surface Passivation of PbS Quantum Dot Solid for Improved Performance of Infrared Absorbing Solar Cells
Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0002-9432-3112
Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China..
Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China..
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2019 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 31, no 11, p. 4081-4091Article in journal (Refereed) Published
Abstract [en]

Surface properties of colloidal quantum dots (CQDs) are critical for the transportation and recombination of the photoinduced charge carrier in CQD solar cells, therefore dominating the photovoltaic performance. Herein, PbS CQD passivated using liquid-state ligand exchange (LSLX) and solid-state ligand exchange (SSLX) strategies are in detail investigated using photoelectron spectroscopy (PES), and solar cell devices are prepared to understand the link between the CQD surface properties and the solar cell function. PES using different energies in the soft and hard Xray regime is applied to study the surface and bulk properties of the CQDs, and the results show more effective surface passivation of the CQDs prepared with the LSLX strategy and less formation of lead-oxide. The CQD solar cells prepared with LSLX strategy show higher performance, and the photoelectric measurements suggest that the recombination of photoinduced charges is reduced for the solar cell prepared with the LSLX approach. Meanwhile, the fabricated solar cells exhibit good stability. This work provides important insights into how to fine-tune the CQD surface properties by improving the CQD passivation, and how this is linked to further improvements of the device photovoltaic performance.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019. Vol. 31, no 11, p. 4081-4091
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-254499DOI: 10.1021/acs.chemmater.9b00742ISI: 000471728200026Scopus ID: 2-s2.0-85067114703OAI: oai:DiVA.org:kth-254499DiVA, id: diva2:1337742
Note

QC 20190715

Available from: 2019-07-16 Created: 2019-07-16 Last updated: 2024-03-15Bibliographically approved
In thesis
1. Spectroscopy on the Dot: Photoelectron Spectroscopy and Time-Resolved Studies of Lead Sulfide Quantum Dots for Solar Cells
Open this publication in new window or tab >>Spectroscopy on the Dot: Photoelectron Spectroscopy and Time-Resolved Studies of Lead Sulfide Quantum Dots for Solar Cells
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Renewable energy is an important topic as global energy consumption continues to rise. Because the sun emits an enormous amount of energy, solar energy is a promising source. However, most of the commercial solar cell technology is manufactured in an energy demanding process and there is a need for new, easily processed materials. This thesis concerns quantum dots, which are nanoparticles that can absorb light of different energies depending on their size. They can be synthesised by solution-based chemistry and turned into solid thin films to harvest sunlight. The fundamental properties of quantum dots need to be better understood before production on large scales may commence. The aim of this thesis was to investigate the fundamental properties of lead sulfide quantum dots. 

The methods used in this thesis are based on photoelectron spectroscopy. They allowed investigation of materials as-is, but also changes upon excitation by laser or X-rays. Using a laser, dynamics on pico- to microsecond timescales were studied by time-resolved photoelectron spectroscopy. Using a range of X-rays, the probability of charge transfer in the attosecond range was investigated.  

Steady-state investigation showed that different surface treatment of the quantum dots caused different resistance towards surface oxidation and X-ray damage. 

Different layers in the structure of solar cells can influence the photovoltage, an important parameter in achieving high power conversion efficiencies. Time-resolved photoelectron spectroscopy was developed and used to investigate the contributions of the layers to photovoltage generation. We observed photovoltage dynamics on a timescale covering six orders of magnitude. 

The mechanism of charge transfer in quantum dots of different sizes was studied by core-hole clock spectroscopy in the attosecond regime. Our results show that quantum confinement affects the charge transfer only at low excitation energies. 

Abstract [sv]

Förnybar energi är viktig då den globala energikonsumtionen fortsätter öka. Solenergi är en lovande energikälla eftersom solen strålar ut otroligt mycket energi. Då kommersiell solcellsteknologi använder mycket energikrävande tillverkningsprocesser finns det behov av nya material som är enkla att tillverka. Denna avhandling handlar om kvantpunkter som är nanopartiklar vilka kan absorbera ljus av olika energi, beroende på partiklarnas storlek. 

Lösningsbaserad syntes är en teknik för att tillverka tunna filmer av kvantpunkter. Grundläggande egenskaper hos kvantpunkter behöver kartläggas ytterligare innan storskalig produktion av sådana kan påbörjas. Målet med denna avhandling var att undersöka grundläggande egenskaper hos kvantpunkter bestående av blysulfid.   

Analysmetoderna i denna avhandling baseras på fotoelektron-spektroskopi. Dessa möjliggör studier av material utan ytterligare bearbetning samt hur de förändras när de påverkas av laserljus eller röntgenstrålning. Med laserpåverkan har dynamik på pico- till mikrosekundsskala kunnat studeras med tidsupplöst fotoelektron-spektroskopi och genom att använda röntgenstrålning med olika energi har sannolikheten för laddningsöverföring studerats på attosekundtidsskalan.

Tidsoberoende studier visade att olika ytbehandlingar på kvantpunkterna gav upphov till olika motstånd mot oxidation och strålskador. 

Olika lager i solcellers struktur kan påverka fotospänningen, vilken är en viktig parameter för att uppnå hög energiomvandlingseffektivitet. Tidsupplöst fotoelektronspektroskopi utvecklades och användes för att undersöka olika lagers bidrag till fotospänningen. Vi observerade tidsberoendet hos fotospänningen på en tidskala som spände över sex storleksordningar.

Laddningsöverföringsmekanismen hos kvantpunkter med olika storlek studerades på attosekundstidsskalan med kärnhålsklocks-spektroskopi. Våra resultat visar att kvanteffekter orsakade av instängning påverkar laddningsöverföringen enbart vid låga excitationsenergier. 

Place, publisher, year, edition, pages
Stockholm, Sweden: KTH Royal Institute of Technology, 2022. p. 107
Series
TRITA-CBH-FOU ; 2022:52
National Category
Physical Chemistry
Research subject
Chemistry
Identifiers
urn:nbn:se:kth:diva-319933 (URN)978-91-8040-370-2 (ISBN)
Public defence
2022-11-04, Kollegiesalen, Brinnelvägen 8, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20221011

Available from: 2022-10-11 Created: 2022-10-11 Last updated: 2025-10-30Bibliographically approved

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Cappel, Ute B.Sloboda, TamaraGardner, James M.

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