Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange
Abstract
Controlling the interparticle spacing in quantum dot (QD) thin films is the most readily accessible way to control transport rates between neighboring QDs and a critical component of device optimization. Here, we use X-ray scattering measurements to accurately measure the interparticle spacing in films of highly monodisperse lead sulfide (PbS) QDs that have undergone a variety of device-relevant ligand exchanges. We tabulate these values for use in simulations and data analysis. We find that monothiol and dithiol ligand species typically result in interparticle spacing values that are equal to the length of a single monothiol or dithiol ligand. Additionally, we find that spin-coating a thick film of QDs followed by a long-duration ligand exchange results in a more complete ligand exchange than spin-coating many thin layers with short-duration ligand exchanges in between. The former method also preserves a remarkable degree of the long-range ordering that was present in the film prior to ligand exchange. These results shed light on ways to produce highly-ordered QD solids with compact and functional ligands, which could lead to enhanced interdot coupling and transport phenomena.
- Authors:
-
- MIT (Massachusetts Inst. of Technology), Cambridge, MA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1183851
- Report Number(s):
- BNL-107970-2015-JA
Journal ID: ISSN 0897-4756; R&D Project: 16077; KC0403020
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 27; Journal Issue: 2; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; functional nanomaterials
Citation Formats
Weidman, Mark C., Yager, Kevin G., and Tisdale, William A. Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange. United States: N. p., 2014.
Web. doi:10.1021/cm503626s.
Weidman, Mark C., Yager, Kevin G., & Tisdale, William A. Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange. United States. https://doi.org/10.1021/cm503626s
Weidman, Mark C., Yager, Kevin G., and Tisdale, William A. Fri .
"Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange". United States. https://doi.org/10.1021/cm503626s. https://www.osti.gov/servlets/purl/1183851.
@article{osti_1183851,
title = {Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange},
author = {Weidman, Mark C. and Yager, Kevin G. and Tisdale, William A.},
abstractNote = {Controlling the interparticle spacing in quantum dot (QD) thin films is the most readily accessible way to control transport rates between neighboring QDs and a critical component of device optimization. Here, we use X-ray scattering measurements to accurately measure the interparticle spacing in films of highly monodisperse lead sulfide (PbS) QDs that have undergone a variety of device-relevant ligand exchanges. We tabulate these values for use in simulations and data analysis. We find that monothiol and dithiol ligand species typically result in interparticle spacing values that are equal to the length of a single monothiol or dithiol ligand. Additionally, we find that spin-coating a thick film of QDs followed by a long-duration ligand exchange results in a more complete ligand exchange than spin-coating many thin layers with short-duration ligand exchanges in between. The former method also preserves a remarkable degree of the long-range ordering that was present in the film prior to ligand exchange. These results shed light on ways to produce highly-ordered QD solids with compact and functional ligands, which could lead to enhanced interdot coupling and transport phenomena.},
doi = {10.1021/cm503626s},
journal = {Chemistry of Materials},
number = 2,
volume = 27,
place = {United States},
year = {Fri Dec 12 00:00:00 EST 2014},
month = {Fri Dec 12 00:00:00 EST 2014}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 94 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors
journal, October 2005
- Talapin, D. V.
- Science, Vol. 310, Issue 5745, p. 86-89
Hybrid passivated colloidal quantum dot solids
journal, July 2012
- Ip, Alexander H.; Thon, Susanna M.; Hoogland, Sjoerd
- Nature Nanotechnology, Vol. 7, Issue 9
Quantum Dots for LED Downconversion in Display Applications
journal, November 2012
- Coe-Sullivan, Seth; Liu, Wenhao; Allen, Peter
- ECS Journal of Solid State Science and Technology, Vol. 2, Issue 2
Energy Level Modification in Lead Sulfide Quantum Dot Thin Films through Ligand Exchange
journal, May 2014
- Brown, Patrick R.; Kim, Donghun; Lunt, Richard R.
- ACS Nano, Vol. 8, Issue 6
Photogenerated Exciton Dissociation in Highly Coupled Lead Salt Nanocrystal Assemblies
journal, May 2010
- Choi, Joshua J.; Luria, Justin; Hyun, Byung-Ryool
- Nano Letters, Vol. 10, Issue 5
Full Color Emission from II-VI Semiconductor Quantum Dot-Polymer Composites
journal, July 2000
- Lee, J.; Sundar, V. C.; Heine, J. R.
- Advanced Materials, Vol. 12, Issue 15, p. 1102-1105
Dependence of Carrier Mobility on Nanocrystal Size and Ligand Length in PbSe Nanocrystal Solids
journal, May 2010
- Liu, Yao; Gibbs, Markelle; Puthussery, James
- Nano Letters, Vol. 10, Issue 5
Structural, Optical, and Electrical Properties of Self-Assembled Films of PbSe Nanocrystals Treated with 1,2-Ethanedithiol
journal, January 2008
- Luther, Joseph M.; Law, Matt; Song, Qing
- ACS Nano, Vol. 2, Issue 2
Self-Organization of CdSe Nanocrystallites into Three-Dimensional Quantum Dot Superlattices
journal, November 1995
- Murray, C. B.; Kagan, C. R.; Bawendi, M. G.
- Science, Vol. 270, Issue 5240
Self-Assembly of PbTe Quantum Dots into Nanocrystal Superlattices and Glassy Films
journal, March 2006
- Urban, Jeffrey J.; Talapin, Dmitri V.; Shevchenko, Elena V.
- Journal of the American Chemical Society, Vol. 128, Issue 10
Colloidal PbS Quantum Dot Solar Cells with High Fill Factor
journal, June 2010
- Zhao, Ni; Osedach, Tim P.; Chang, Liang-Yi
- ACS Nano, Vol. 4, Issue 7
QLEDs for displays and solid-state lighting
journal, September 2013
- Supran, Geoffrey J.; Shirasaki, Yasuhiro; Song, Katherine W.
- MRS Bulletin, Vol. 38, Issue 9
High-performance crosslinked colloidal quantum-dot light-emitting diodes
journal, May 2009
- Cho, Kyung-Sang; Lee, Eun Kyung; Joo, Won-Jae
- Nature Photonics, Vol. 3, Issue 6
Monodisperse, Air-Stable PbS Nanocrystals via Precursor Stoichiometry Control
journal, May 2014
- Weidman, Mark C.; Beck, Megan E.; Hoffman, Rachel S.
- ACS Nano, Vol. 8, Issue 6
Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage
journal, March 2011
- Choi, Joshua J.; Bealing, Clive R.; Bian, Kaifu
- Journal of the American Chemical Society, Vol. 133, Issue 9
PbS Nanoparticles Capped with Tetrathiafulvalenetetracarboxylate: Utilizing Energy Level Alignment for Efficient Carrier Transport
journal, February 2014
- Scheele, Marcus; Hanifi, David; Zherebetskyy, Danylo
- ACS Nano, Vol. 8, Issue 3
Enhanced Mobility-Lifetime Products in PbS Colloidal Quantum Dot Photovoltaics
journal, December 2011
- Jeong, Kwang S.; Tang, Jiang; Liu, Huan
- ACS Nano, Vol. 6, Issue 1
Engineering colloidal quantum dot solids within and beyond the mobility-invariant regime
journal, May 2014
- Zhitomirsky, David; Voznyy, Oleksandr; Levina, Larissa
- Nature Communications, Vol. 5, Issue 1
Grazing-incidence transmission X-ray scattering: surface scattering in the Born approximation
journal, January 2013
- Lu, Xinhui; Yager, Kevin G.; Johnston, Danvers
- Journal of Applied Crystallography, Vol. 46, Issue 1
Infrared colloidal lead chalcogenide nanocrystals: Synthesis, properties, and photovoltaic applications
journal, January 2012
- Fu, Huiying; Tsang, Sai-Wing
- Nanoscale, Vol. 4, Issue 7
Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control
journal, May 2012
- Sun, Liangfeng; Choi, Joshua J.; Stachnik, David
- Nature Nanotechnology, Vol. 7, Issue 6
Structural, Optical, and Electrical Properties of PbSe Nanocrystal Solids Treated Thermally or with Simple Amines
journal, May 2008
- Law, Matt; Luther, Joseph M.; Song, Qing
- Journal of the American Chemical Society, Vol. 130, Issue 18
p-Type PbSe and PbS Quantum Dot Solids Prepared with Short-Chain Acids and Diacids
journal, March 2010
- Zarghami, Mohammad H.; Liu, Yao; Gibbs, Markelle
- ACS Nano, Vol. 4, Issue 4
Ligand Coupling Symmetry Correlates with Thermopower Enhancement in Small-Molecule/Nanocrystal Hybrid Materials
journal, September 2014
- Lynch, Jared; Kotiuga, Michele; Doan-Nguyen, Vicky V. T.
- ACS Nano, Vol. 8, Issue 10, p. 10528-10536
Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications
journal, January 2010
- Talapin, Dmitri V.; Lee, Jong-Soo; Kovalenko, Maksym V.
- Chemical Reviews, Vol. 110, Issue 1
Practical Roadmap and Limits to Nanostructured Photovoltaics
journal, November 2011
- Lunt, Richard R.; Osedach, Timothy P.; Brown, Patrick R.
- Advanced Materials, Vol. 23, Issue 48
Structure/Processing Relationships of Highly Ordered Lead Salt Nanocrystal Superlattices
journal, September 2009
- Hanrath, Tobias; Choi, Joshua J.; Smilgies, Detlef-M.
- ACS Nano, Vol. 3, Issue 10
Electrical Transport in Colloidal Quantum Dot Films
journal, April 2012
- Guyot-Sionnest, Philippe
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 9
Improved Current Extraction from ZnO/PbS Quantum Dot Heterojunction Photovoltaics Using a MoO 3 Interfacial Layer
journal, July 2011
- Brown, Patrick R.; Lunt, Richard R.; Zhao, Ni
- Nano Letters, Vol. 11, Issue 7
Emergence of colloidal quantum-dot light-emitting technologies
journal, December 2012
- Shirasaki, Yasuhiro; Supran, Geoffrey J.; Bawendi, Moungi G.
- Nature Photonics, Vol. 7, Issue 1
Works referencing / citing this record:
Colloidal Crystals of NaYF 4 Upconversion Nanocrystals Studied by Small-Angle X-Ray Scattering (SAXS)
journal, December 2018
- Homann, Christian; Bolze, Joerg; Haase, Markus
- Particle & Particle Systems Characterization, Vol. 36, Issue 2
Engineering interactions in QDs–PCBM blends: a surface chemistry approach
journal, January 2018
- Righetto, Marcello; Privitera, Alberto; Carraro, Francesco
- Nanoscale, Vol. 10, Issue 25
Bridging functional nanocomposites to robust macroscale devices
journal, June 2019
- Begley, Matthew R.; Gianola, Daniel S.; Ray, Tyler R.
- Science, Vol. 364, Issue 6447
Kinetics of the self-assembly of nanocrystal superlattices measured by real-time in situ X-ray scattering
journal, March 2016
- Weidman, Mark C.; Smilgies, Detlef-M.; Tisdale, William A.
- Nature Materials, Vol. 15, Issue 7
Angular X-ray Cross-Correlation Analysis (AXCCA): Basic Concepts and Recent Applications to Soft Matter and Nanomaterials
journal, October 2019
- Zaluzhnyy, Ivan; Kurta, Ruslan; Scheele, Marcus
- Materials, Vol. 12, Issue 21
Nanocrystal superlattices as phonon-engineered solids and acoustic metamaterials
journal, September 2019
- Yazdani, Nuri; Jansen, Maximilian; Bozyigit, Deniz
- Nature Communications, Vol. 10, Issue 1
Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification
journal, May 2017
- Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.
- Nature Communications, Vol. 8, Issue 1
Ligand coverage dependence of structural stability and interparticle spacing of gold supracrystals
journal, January 2018
- Liu, Xuepeng; Lu, Pin; Zhai, Hua
- Journal of Applied Physics, Vol. 123, Issue 4
Molecular dynamics simulation of interparticle spacing and many-body effect in gold supracrystals
journal, February 2016
- Liu, X. P.; Ni, Y.; He, L. H.
- Nanotechnology, Vol. 27, Issue 13
Electron Mobility of 24 cm 2 V −1 s −1 in PbSe Colloidal-Quantum-Dot Superlattices
journal, August 2018
- Balazs, Daniel M.; Matysiak, Bartosz M.; Momand, Jamo
- Advanced Materials, Vol. 30, Issue 38
Rapid ordering of block copolymer thin films
journal, August 2016
- Majewski, Pawel W.; Yager, Kevin G.
- Journal of Physics: Condensed Matter, Vol. 28, Issue 40
Enhancing the photocatalytic properties of PbS QD solids: the ligand exchange approach
journal, January 2019
- Abargues, Rafael; Navarro, Juan; Rodríguez-Cantó, Pedro J.
- Nanoscale, Vol. 11, Issue 4
Angular X-ray Cross-Correlation Analysis (AXCCA): Basic Concepts and Recent Applications to Soft Matter and Nanomaterials
text, January 2019
- Zaluzhnyy, Ivan; Kurta, Ruslan; Scheele, Marcus
- Deutsches Elektronen-Synchrotron, DESY, Hamburg
Charge transport and localization in atomically coherent quantum dot solids
journal, February 2016
- Whitham, Kevin; Yang, Jun; Savitzky, Benjamin H.
- Nature Materials, Vol. 15, Issue 5
Phonon-engineered solids constructed from nanocrystals
journal, August 2019
- Jansen, Maximilian; Yazdani, Nuri; Wood, Vanessa
- APL Materials, Vol. 7, Issue 8
Characterization of colloidal nanocrystal surface structure using small angle neutron scattering and efficient Bayesian parameter estimation
journal, June 2019
- Winslow, Samuel W.; Shcherbakov-Wu, Wenbi; Liu, Yun
- The Journal of Chemical Physics, Vol. 150, Issue 24
Phonon-engineered solids constructed from nanocrystals
text, January 2019
- Jansen, Maximilian; Yazdani, Nuri; Wood, Vanessa
- ETH Zurich
Nanocrystal superlattices as phonon-engineered solids and acoustic metamaterials
text, January 2019
- Yazdani, Nuri; Jansen, Maximilian; Bozyigit, Deniz
- ETH Zurich
Comparing Halide Ligands in PbS Colloidal Quantum Dots for Field-Effect Transistors and Solar Cells
journal, November 2018
- Bederak, Dmytro; Balazs, Daniel M.; Sukharevska, Nataliia V.
- ACS Applied Nano Materials, Vol. 1, Issue 12
Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films
journal, July 2017
- Sainato, Michela; Shevitski, Brian; Sahu, Ayaskanta
- ACS Omega, Vol. 2, Issue 7
Correction to “Three-Dimensional Superlattice of PbS Quantum Dots in Flakes”
journal, March 2018
- Ermakov, Viktor A.; da Silva Filho, José Maria Clemente; Bonato, Luiz Gustavo
- ACS Omega, Vol. 3, Issue 3
Nanocrystal superlattices as phonon-engineered solids and acoustic metamaterials
journal, September 2019
- Yazdani, Nuri; Jansen, Maximilian; Bozyigit, Deniz
- Nature Communications, Vol. 10, Issue 1