Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity

Bronstein, Noah D.; Martinez, Marissa S.; Kroupa, Daniel M.; Vörös, Márton; Lu, Haipeng; Brawand, Nicholas P.; Nozik, Arthur J.; Sellinger, Alan; Galli, Giulia; Beard, Matthew C.

doi:10.1021/acsnano.9b00191

Title: Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity

Abstract

We present a combined experimental and theoretical study of ligand ligand cooperativity during X-type carboxylate-to-carboxylate ligand exchange reactions on PbS quantum dot surfaces. We find that the ligand dipole moment (varied through changing the substituents on the benzene ring of cinnamic acid derivatives) impacts the ligand-exchange isotherms; in particular, ligands with large electron withdrawing character result in a sharper transition from an oleate-dominated ligand shell to a cinnamate-dominated ligand shell. We developed a two-dimensional lattice model to simulate the ligand-exchange isotherms that accounts for the difference in ligand binding energy as well as ligand ligand cooperativity. Our model shows that ligands with larger ligand ligand coupling energy exhibit sharper isotherms indicating an order disorder phase transition. Lastly, we developed an anisotropic Janus ligand shell by taking advantage of the ligand ligand cooperative ligand exchanges. We monitored the Janus ligand shell using ¹⁹F nuclear magnetic resonance, showing that when the ligand ligand coupling energy falls within the order region of the phase diagram, Janus ligand shells can be constructed.

Authors:

^[1]; Martinez, Marissa S. ^[2]; Kroupa, Daniel M. ^[2];

^[3];

^[1];

^[4];

^[2];

^[5]; Galli, Giulia ^[3];

^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, IL (United States)
Univ. of Chicago, IL (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)

Publication Date:: Mon Mar 11 00:00:00 EDT 2019

Research Org.:: National Renewable Energy Lab. (NREL), Golden, CO (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

OSTI Identifier:: 1544532

Alternate Identifier(s):: OSTI ID: 1524451

Report Number(s):: NREL/JA-5900-72996
Journal ID: ISSN 1936-0851

Grant/Contract Number:: AC36-08GO28308; AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: ACS Nano

Additional Journal Information:: Journal Volume: 13; Journal Issue: 4; Journal ID: ISSN 1936-0851

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; ligand coupling; ligand-QD interactions; PbS quantum dots; QD optical properties; QD surface science; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ligand−QD interactions

Citation Formats


                    Bronstein, Noah D., Martinez, Marissa S., Kroupa, Daniel M., Vörös, Márton, Lu, Haipeng, Brawand, Nicholas P., Nozik, Arthur J., Sellinger, Alan, Galli, Giulia, and Beard, Matthew C. Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity.  United States: N. p., 2019. 
Web.  doi:10.1021/acsnano.9b00191.

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                    Bronstein, Noah D., Martinez, Marissa S., Kroupa, Daniel M., Vörös, Márton, Lu, Haipeng, Brawand, Nicholas P., Nozik, Arthur J., Sellinger, Alan, Galli, Giulia, & Beard, Matthew C. Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity.  United States.  https://doi.org/10.1021/acsnano.9b00191

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                    Bronstein, Noah D., Martinez, Marissa S., Kroupa, Daniel M., Vörös, Márton, Lu, Haipeng, Brawand, Nicholas P., Nozik, Arthur J., Sellinger, Alan, Galli, Giulia, and Beard, Matthew C. Mon .  
"Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity".  United States.  https://doi.org/10.1021/acsnano.9b00191.  https://www.osti.gov/servlets/purl/1544532.

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@article{osti_1544532,

  title        = {Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity},

  author       = {Bronstein, Noah D. and Martinez, Marissa S. and Kroupa, Daniel M. and Vörös, Márton and Lu, Haipeng and Brawand, Nicholas P. and Nozik, Arthur J. and Sellinger, Alan and Galli, Giulia and Beard, Matthew C.},

  abstractNote = {We present a combined experimental and theoretical study of ligand ligand cooperativity during X-type carboxylate-to-carboxylate ligand exchange reactions on PbS quantum dot surfaces. We find that the ligand dipole moment (varied through changing the substituents on the benzene ring of cinnamic acid derivatives) impacts the ligand-exchange isotherms; in particular, ligands with large electron withdrawing character result in a sharper transition from an oleate-dominated ligand shell to a cinnamate-dominated ligand shell. We developed a two-dimensional lattice model to simulate the ligand-exchange isotherms that accounts for the difference in ligand binding energy as well as ligand ligand cooperativity. Our model shows that ligands with larger ligand ligand coupling energy exhibit sharper isotherms indicating an order disorder phase transition. Lastly, we developed an anisotropic Janus ligand shell by taking advantage of the ligand ligand cooperative ligand exchanges. We monitored the Janus ligand shell using 19F nuclear magnetic resonance, showing that when the ligand ligand coupling energy falls within the order region of the phase diagram, Janus ligand shells can be constructed.},

  doi          = {10.1021/acsnano.9b00191},

  journal      = {ACS Nano},

  number       = 4,

  volume       = 13,

  place        = {United States},

  year         = {Mon Mar 11 00:00:00 EDT 2019},

  month        = {Mon Mar 11 00:00:00 EDT 2019}

}

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Works referencing / citing this record:

Enhanced photoredox activity of CsPbBr ₃ nanocrystals by quantitative colloidal ligand exchange
journal, November 2019

Lu, Haipeng; Zhu, Xiaolin; Miller, Collin
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Title: Designing Janus Ligand Shells on PbS Quantum Dots using Ligand–Ligand Cooperativity

Abstract

Citation Formats

Semiconductor Clusters, Nanocrystals, and Quantum Dots journal, February 1996

Infrared Quantum Dots: Progress, Challenges, and Opportunities journal, January 2019

Prospects of Nanoscience with Nanocrystals journal, January 2015

Reaction Chemistry and Ligand Exchange at Cadmium−Selenide Nanocrystal Surfaces journal, September 2008

Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach journal, October 2007

Metal Halide Solid-State Surface Treatment for High Efficiency PbS and PbSe QD Solar Cells journal, April 2015

Structural, Optical, and Electrical Properties of Self-Assembled Films of PbSe Nanocrystals Treated with 1,2-Ethanedithiol journal, January 2008

PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors journal, October 2005

Ligand Exchange and the Stoichiometry of Metal Chalcogenide Nanocrystals: Spectroscopic Observation of Facile Metal-Carboxylate Displacement and Binding journal, November 2013

A new approach to the formal classification of covalent compounds of the elements journal, September 1995

The coordination chemistry of nanocrystal surfaces journal, February 2015

Ligand-Mediated Interactions between Nanoscale Surfaces Depend Sensitively and Nonlinearly on Temperature, Facet Dimensions, and Ligand Coverage journal, January 2016

Ligand-induced twisting of nanoplatelets and their self-assembly into chiral ribbons journal, September 2017

Ligand Adsorption/Desorption on Sterically Stabilized InP Colloidal Nanocrystals: Observation and Thermodynamic Analysis journal, May 2006

“Darker-than-Black” PbS Quantum Dots: Enhancing Optical Absorption of Colloidal Semiconductor Nanocrystals via Short Conjugated Ligands journal, January 2015

Optical Absorbance Enhancement in PbS QD/Cinnamate Ligand Complexes journal, June 2018

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Anisotropic particles with patchy, multicompartment and Janus architectures: preparation and application journal, January 2011

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Role of Interligand Coupling in Determining the Interfacial Electronic Structure of Colloidal CdS Quantum Dots journal, December 2015

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A survey of Hammett substituent constants and resonance and field parameters journal, March 1991

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The Cooperative Molecular Field Effect journal, October 2005

Calculation of the dielectric constant of monolayer films on a material surface journal, September 1996

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Rethinking the term “pi-stacking” journal, January 2012

Determination of monolayer-protected gold nanoparticle ligand–shell morphology using NMR journal, January 2012

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Semiconductor Clusters, Nanocrystals, and Quantum Dots
journal, February 1996

Infrared Quantum Dots: Progress, Challenges, and Opportunities
journal, January 2019

Prospects of Nanoscience with Nanocrystals
journal, January 2015

Reaction Chemistry and Ligand Exchange at Cadmium−Selenide Nanocrystal Surfaces
journal, September 2008

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journal, October 2007

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journal, April 2015

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journal, January 2008

PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors
journal, October 2005

Ligand Exchange and the Stoichiometry of Metal Chalcogenide Nanocrystals: Spectroscopic Observation of Facile Metal-Carboxylate Displacement and Binding
journal, November 2013

A new approach to the formal classification of covalent compounds of the elements
journal, September 1995

The coordination chemistry of nanocrystal surfaces
journal, February 2015

Ligand-Mediated Interactions between Nanoscale Surfaces Depend Sensitively and Nonlinearly on Temperature, Facet Dimensions, and Ligand Coverage
journal, January 2016

Ligand-induced twisting of nanoplatelets and their self-assembly into chiral ribbons
journal, September 2017

Ligand Adsorption/Desorption on Sterically Stabilized InP Colloidal Nanocrystals: Observation and Thermodynamic Analysis
journal, May 2006

“Darker-than-Black” PbS Quantum Dots: Enhancing Optical Absorption of Colloidal Semiconductor Nanocrystals via Short Conjugated Ligands
journal, January 2015

Optical Absorbance Enhancement in PbS QD/Cinnamate Ligand Complexes
journal, June 2018

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification
journal, May 2017

Relaxation of Exciton Confinement in CdSe Quantum Dots by Modification with a Conjugated Dithiocarbamate Ligand
journal, May 2010

Electronic Processes within Quantum Dot-Molecule Complexes
journal, August 2016

Dependence of the Band Gap of CdSe Quantum Dots on the Surface Coverage and Binding Mode of an Exciton-Delocalizing Ligand, Methylthiophenolate
journal, August 2015

Anisotropic particles with patchy, multicompartment and Janus architectures: preparation and application
journal, January 2011

Subnanometre ligand-shell asymmetry leads to Janus-like nanoparticle membranes
journal, June 2015

Characterization of Ligand Shell for Mixed-Ligand Coated Gold Nanoparticles
journal, July 2017

Role of Interligand Coupling in Determining the Interfacial Electronic Structure of Colloidal CdS Quantum Dots
journal, December 2015

A tunable library of substituted thiourea precursors to metal sulfide nanocrystals
journal, June 2015

A survey of Hammett substituent constants and resonance and field parameters
journal, March 1991

Effect of Degree, Type, and Position of Unsaturation on the pKa of Long-Chain Fatty Acids
journal, December 2002

The Cooperative Molecular Field Effect
journal, October 2005

Calculation of the dielectric constant of monolayer films on a material surface
journal, September 1996

Electrostatic charge-charge and dipole-dipole interactions near the surface of a medium with screening non-locality (Review Article)
journal, August 2016

Rethinking the term “pi-stacking”
journal, January 2012

Determination of monolayer-protected gold nanoparticle ligand–shell morphology using NMR
journal, January 2012

In Situ Observation of Rapid Ligand Exchange in Colloidal Nanocrystal Suspensions Using Transfer NOE Nuclear Magnetic Resonance Spectroscopy
journal, March 2009

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journal, November 2019