Evidence map›Paper›PMID 31336046›Full record

ArticleJournal of the American Chemical Society2019

Engineering Molecular Ligand Shells on Quantum Dots for Quantitative Harvesting of Triplet Excitons Generated by Singlet Fission.

Jesse R Allardice, Arya Thampi, Simon Dowland, James Xiao, Victor Gray, Zhilong Zhang, Peter Budden, Anthony J Petty, Nathaniel J L K Davis, Neil C Greenham and 2 more

Erratum issuedOpen access · hybridAbstract read
In one paragraph

Article in Journal of the American Chemical Society, 2019. The graph could read no effect estimate from its abstract, so it casts no vote on the map. An erratum has been issued. Cited by 20 papers.

0numbers the graph read from it
0cells of the map it votes in
20citing papers in PubMed
3.6field-weighted citation impact, top 6% of its field
1 · What the graph read from it

What it found

Each row is one number read from the abstract, on the scale the paper reported it, with its interval. Left of the dashed line favours the treatment, right favours the comparator. Under each row is the sentence it came from. New to these charts? A ten-minute tutorial.

The abstract states no effect estimate the extractor could read, or names no intervention and outcome on the map, so this paper lights no cell and moves no belief. It is still indexed, cited and linked below.

2 · The registry

The trial behind it

Trials whose registry record cites this paper, or whose number appears in the abstract. A trial that started after this paper was published is citing it as background, not reporting it.

Neither the registry nor the abstract names a trial number. If this is a trial report, that itself is worth knowing.

3 · Its place in the literature

Who cites it

20 citing papers in PubMed, 62 citations in OpenAlex.

  1. Article
  2. Article
  3. Article
  4. Article
  5. Article
  6. Computational Discovery of Intermolecular Singlet Fission Materials Using Many-Body Perturbation Theory.The journal of physical chemistry. C, Nanomaterials and interfaces · 2024
    Review
  7. Article
  8. Article
  9. Article
  10. Aza-Cibalackrot: Turning on Singlet Fission Through Crystal Engineering.Journal of the American Chemical Society · 2023
    Article
  11. Article
  12. Article
  13. Review
  14. Dye-Sensitized Multiple Exciton Generation in Lead Sulfide Quantum Dots.Journal of the American Chemical Society · 2022
    Article
  15. Article
  16. Article
  17. Review
  18. Article
  19. Article
  20. Article
4 · The record

Corrections and comments

5 · Who and what money

Authors and funding

12 authors at 3 institutions in 4 countries.

Jesse R AllardiceCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.ORCID 0000-0002-1969-7536
Arya ThampiCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.ORCID 0000-0001-6003-5991
Simon DowlandCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.
James XiaoCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.
Victor GrayCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.ORCID 0000-0001-6583-8654
Zhilong ZhangCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.ORCID 0000-0001-9903-4945
Peter BuddenCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.
Anthony J PettyCenter for Applied Energy Research , University of Kentucky , Research Park Drive , Lexington , Kentucky 40511 , United States.
Nathaniel J L K DavisCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.
Neil C GreenhamCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.ORCID 0000-0002-2155-2432
John E AnthonyCenter for Applied Energy Research , University of Kentucky , Research Park Drive , Lexington , Kentucky 40511 , United States.ORCID 0000-0002-8972-1888
Akshay RaoCavendish Laboratory , University of Cambridge , J. J. Thomson Avenue , Cambridge CB3 0HE , United Kingdom.ORCID 0000-0003-4261-0766
University of Cambridge · GBUniversity of Kentucky · USUppsala University · SE

Funding

No grant is acknowledged in the PubMed record.

6 · The paper itself

Abstract

Singlet fission is an exciton multiplication process in organic molecules in which a photogenerated spin-singlet exciton is rapidly and efficiently converted to two spin-triplet excitons. This process offers a mechanism to break the Shockley-Queisser limit by overcoming the thermalization losses inherent to all single-junction photovoltaics. One of the most promising methods to harness the singlet fission process is via the efficient extraction of the dark triplet excitons into quantum dots (QDs) where they can recombine radiatively, thereby converting high-energy photons to pairs of low-energy photons, which can then be captured in traditional inorganic PVs such as Si. Such a singlet fission photon multiplication (SF-PM) process could increase the efficiency of the best Si cells from 26.7% to 32.5%, breaking the Shockley-Queisser limit. However, there has been no demonstration of such a singlet fission photon multiplication (SF-PM) process in a bulk system to date. Here, we demonstrate a solution-based bulk SF-PM system based on the singlet fission material TIPS-Tc combined with PbS QDs. Using a range of steady-state and time-resolved measurements combined with analytical modeling we study the dynamics and mechanism of the triplet harvesting process. We show that the system absorbs >95% of incident photons within the singlet fission material to form singlet excitons, which then undergo efficient singlet fission in the solution phase (135 ± 5%) before quantitative harvesting of the triplet excitons (95 ± 5%) via a low concentration of QD acceptors, followed by the emission of IR photons. We find that in order to achieve efficient triplet harvesting it is critical to engineer the surface of the QD with a triplet transfer ligand and that bimolecular decay of triplets is potentially a major loss pathway which can be controlled via tuning the concentration of QD acceptors. We demonstrate that the photon multiplication efficiency is maintained up to solar fluence. Our results establish the solution-based SF-PM system as a simple and highly tunable platform to understand the dynamics of a triplet energy transfer process between organic semiconductors and QDs, one that can provide clear design rules for new materials.

Identifiers

PMID31336046
PMCPMC7007228
OpenAlexW2963955575

What OpenQuestion holds

Textmetadata
Read underepoch 390

Registered trials

None linked

Read under generation 80e0d062 · epoch 390. Bibliography from PubMed, PubMed Central and OpenAlex; grants from NIH RePORTER; trial links from ClinicalTrials.gov; estimates, votes and beliefs from the OpenQuestion graph.