DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Rapid In Situ Ligand‐Exchange Process Used to Prepare 3D PbSe Nanocrystal Superlattice Infrared Photodetectors

Abstract

Abstract Colloidal semiconductor nanocrystals are important building blocks for low‐cost, solution‐processed electronic devices with tunable functionalities. Considerable progress is made in improving charge transport through nanocrystal films by exchanging long insulating ligands with shorter passivating ligands. To take full advantage of this strategy, it is equally important to fabricate close‐packed structures that reduce the average interparticle spacing. Yet it remains a challenge to retain long‐range, close‐packed order after ligand exchange. Here, a novel one‐step in situ ligand‐exchange method is demonstrated that enables rapid (5 min) ligand exchange of nanocrystal films, which are more than 50 layers thick. Using this simple and efficient method, it is shown that the face‐centered cubic ordering of 500 nm thick PbSe nanocrystal films is retained after ligand exchange from oleic acid to benzoic acid. Moreover, it is demonstrated that PbSe nanocrystal photodetectors with a well‐ordered structure have superior optoelectronic properties compared to disordered films; ordered films have a 16× higher responsivity of ≈0.25 A W −1 at 1 V and a 2× faster response time. As far as it is known, this is the first report to realize a rapid one‐step ligand exchange through a thick superlattice film with retention of long‐range order.

Authors:
 [1]; ORCiD logo [1];  [2]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Lawrence Livermore National Laboratory 7000 East Avenue Livermore CA 94550 USA
  2. Voxtel Opto An Allegro Microsystems Company 1443 E. 13th Avenue Eugene OR 97403 USA
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1784350
Alternate Identifier(s):
OSTI ID: 1784355; OSTI ID: 1787205
Report Number(s):
LLNL-JRNL-818923
Journal ID: ISSN 1613-6810; 2101166
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Published Article
Journal Name:
Small
Additional Journal Information:
Journal Name: Small Journal Volume: 17 Journal Issue: 25; Journal ID: ISSN 1613-6810
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nanoparticles; superlattice; nanomaterials; assembly; ligand-exchange; lead selenide; infrared detecton

Citation Formats

Xu, Xiaojie, Kweon, Kyoung E., Keuleyan, Sean, Sawvel, April, Cho, En Ju, and Orme, Christine. Rapid In Situ Ligand‐Exchange Process Used to Prepare 3D PbSe Nanocrystal Superlattice Infrared Photodetectors. Germany: N. p., 2021. Web. doi:10.1002/smll.202101166.
Xu, Xiaojie, Kweon, Kyoung E., Keuleyan, Sean, Sawvel, April, Cho, En Ju, & Orme, Christine. Rapid In Situ Ligand‐Exchange Process Used to Prepare 3D PbSe Nanocrystal Superlattice Infrared Photodetectors. Germany. https://doi.org/10.1002/smll.202101166
Xu, Xiaojie, Kweon, Kyoung E., Keuleyan, Sean, Sawvel, April, Cho, En Ju, and Orme, Christine. Fri . "Rapid In Situ Ligand‐Exchange Process Used to Prepare 3D PbSe Nanocrystal Superlattice Infrared Photodetectors". Germany. https://doi.org/10.1002/smll.202101166.
@article{osti_1784350,
title = {Rapid In Situ Ligand‐Exchange Process Used to Prepare 3D PbSe Nanocrystal Superlattice Infrared Photodetectors},
author = {Xu, Xiaojie and Kweon, Kyoung E. and Keuleyan, Sean and Sawvel, April and Cho, En Ju and Orme, Christine},
abstractNote = {Abstract Colloidal semiconductor nanocrystals are important building blocks for low‐cost, solution‐processed electronic devices with tunable functionalities. Considerable progress is made in improving charge transport through nanocrystal films by exchanging long insulating ligands with shorter passivating ligands. To take full advantage of this strategy, it is equally important to fabricate close‐packed structures that reduce the average interparticle spacing. Yet it remains a challenge to retain long‐range, close‐packed order after ligand exchange. Here, a novel one‐step in situ ligand‐exchange method is demonstrated that enables rapid (5 min) ligand exchange of nanocrystal films, which are more than 50 layers thick. Using this simple and efficient method, it is shown that the face‐centered cubic ordering of 500 nm thick PbSe nanocrystal films is retained after ligand exchange from oleic acid to benzoic acid. Moreover, it is demonstrated that PbSe nanocrystal photodetectors with a well‐ordered structure have superior optoelectronic properties compared to disordered films; ordered films have a 16× higher responsivity of ≈0.25 A W −1 at 1 V and a 2× faster response time. As far as it is known, this is the first report to realize a rapid one‐step ligand exchange through a thick superlattice film with retention of long‐range order.},
doi = {10.1002/smll.202101166},
journal = {Small},
number = 25,
volume = 17,
place = {Germany},
year = {Fri May 21 00:00:00 EDT 2021},
month = {Fri May 21 00:00:00 EDT 2021}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/smll.202101166

Save / Share:

Works referenced in this record:

Fast Voltammetric and Electrochromic Response of Semiconductor Nanocrystal Thin Films
journal, July 2003

  • Guyot-Sionnest, Philippe; Wang, Congjun
  • The Journal of Physical Chemistry B, Vol. 107, Issue 30
  • DOI: 10.1021/jp0275084

Solar cells from colloidal nanocrystals: Fundamentals, materials, devices, and economics
journal, August 2009

  • Hillhouse, Hugh W.; Beard, Matthew C.
  • Current Opinion in Colloid & Interface Science, Vol. 14, Issue 4
  • DOI: 10.1016/j.cocis.2009.05.002

Ultrasensitive solution-cast quantum dot photodetectors
journal, July 2006

  • Konstantatos, Gerasimos; Howard, Ian; Fischer, Armin
  • Nature, Vol. 442, Issue 7099
  • DOI: 10.1038/nature04855

Building devices from colloidal quantum dots
journal, August 2016


Projector augmented-wave method
journal, December 1994


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
  • DOI: 10.1021/nl101284k

Prospects of Nanoscience with Nanocrystals
journal, January 2015

  • Kovalenko, Maksym V.; Manna, Liberato; Cabot, Andreu
  • ACS Nano, Vol. 9, Issue 2
  • DOI: 10.1021/nn506223h

Packing State Management to Realize Dense and Semiconducting Lead Sulfide Nanocrystals Film via a Single-Step Deposition
journal, September 2020


Accurate characterization of next-generation thin-film photodetectors
journal, December 2018


2D matrix engineering for homogeneous quantum dot coupling in photovoltaic solids
journal, April 2018


Self-Assembly and Thermal Stability of Binary Superlattices of Gold and Silicon Nanocrystals
journal, October 2013

  • Yu, Yixuan; Bosoy, Christian A.; Smilgies, Detlef-M.
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 21
  • DOI: 10.1021/jz401964s

1/f noise in semiconductor and metal nanocrystal solids
journal, April 2014

  • Liu, Heng; Lhuillier, Emmanuel; Guyot-Sionnest, Philippe
  • Journal of Applied Physics, Vol. 115, Issue 15
  • DOI: 10.1063/1.4871682

New concept ultraviolet photodetectors
journal, November 2015


The role of ligands in electron transport in nanocrystal solids
journal, January 2020

  • Khabibullin, Artem R.; Efros, Alexander L.; Erwin, Steven C.
  • Nanoscale, Vol. 12, Issue 45
  • DOI: 10.1039/D0NR06892F

Colloidal quantum dots for infrared detection beyond silicon
journal, August 2019

  • Guyot-Sionnest, Philippe; Ackerman, Matthew M.; Tang, Xin
  • The Journal of Chemical Physics, Vol. 151, Issue 6
  • DOI: 10.1063/1.5115501

Mechanistic Insight into the Formation of Cationic Naked Nanocrystals Generated under Equilibrium Control
journal, October 2014

  • Doris, Sean E.; Lynch, Jared J.; Li, Changyi
  • Journal of the American Chemical Society, Vol. 136, Issue 44
  • DOI: 10.1021/ja508675t

PbE (E = S, Se) Colloidal Quantum Dot-Layered 2D Material Hybrid Photodetectors
journal, January 2020

  • Nakotte, Tom; Luo, Hongmei; Pietryga, Jeff
  • Nanomaterials, Vol. 10, Issue 1
  • DOI: 10.3390/nano10010172

A Generalized Ligand-Exchange Strategy Enabling Sequential Surface Functionalization of Colloidal Nanocrystals
journal, February 2011

  • Dong, Angang; Ye, Xingchen; Chen, Jun
  • Journal of the American Chemical Society, Vol. 133, Issue 4, p. 998-1006
  • DOI: 10.1021/ja108948z

Organic and Inorganic Blocking Layers for Solution-Processed Colloidal PbSe Nanocrystal Infrared Photodetectors
journal, November 2010

  • Sarasqueta, Galileo; Choudhury, Kaushik Roy; Subbiah, Jegadesan
  • Advanced Functional Materials, Vol. 21, Issue 1
  • DOI: 10.1002/adfm.201001328

Toward printable solar cells based on PbX colloidal quantum dot inks
journal, January 2021

  • Liu, Yang; Shi, Guozheng; Liu, Zeke
  • Nanoscale Horizons, Vol. 6, Issue 1
  • DOI: 10.1039/D0NH00488J

Recent Research Progress in Surface Ligand Exchange of PbS Quantum Dots for Solar Cell Application
journal, February 2020

  • You, Hyung Ryul; Park, Jin Young; Lee, Duck Hoon
  • Applied Sciences, Vol. 10, Issue 3
  • DOI: 10.3390/app10030975

Interparticle Spacing and Structural Ordering in Superlattice PbS Nanocrystal Solids Undergoing Ligand Exchange
journal, December 2014

  • Weidman, Mark C.; Yager, Kevin G.; Tisdale, William A.
  • Chemistry of Materials, Vol. 27, Issue 2
  • DOI: 10.1021/cm503626s

Reversible, Tunable, Electric-Field Driven Assembly of Silver Nanocrystal Superlattices
journal, May 2017


Irena : tool suite for modeling and analysis of small-angle scattering
journal, February 2009


Trap engineering in solution processed PbSe quantum dots for high-speed MID-infrared photodetectors
journal, January 2019

  • Dolatyari, Mahboubeh; Rostami, Ali; Mathur, Sanjay
  • Journal of Materials Chemistry C, Vol. 7, Issue 19
  • DOI: 10.1039/C8TC06093B

Hydrogenated Nanocrystalline Silicon Near Infrared Photodiode Detector
journal, November 2014


A review on fundamentals and applications of electrophoretic deposition (EPD)
journal, January 2007


Effect of Solvent Treatment on Solution-Processed Colloidal PbSe Nanocrystal Infrared Photodetectors
journal, May 2010

  • Sarasqueta, Galileo; Choudhury, Kaushik Roy; So, Franky
  • Chemistry of Materials, Vol. 22, Issue 11
  • DOI: 10.1021/cm1006229

Preparation and Characterization of Monodisperse PbSe Semiconductor Nanocrystals in a Noncoordinating Solvent
journal, August 2004

  • Yu, William W.; Falkner, Joshua C.; Shih, Bertram S.
  • Chemistry of Materials, Vol. 16, Issue 17
  • DOI: 10.1021/cm049476y

What should the density of amorphous solids be?
journal, November 2019

  • Cui, Xiang-Yuan; Ringer, Simon P.; Wang, Gang
  • The Journal of Chemical Physics, Vol. 151, Issue 19
  • DOI: 10.1063/1.5113733

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


Single-Crystalline InGaAs Nanowires for Room-Temperature High-Performance Near-Infrared Photodetectors
journal, September 2015


Effects of Post-Synthesis Processing on CdSe Nanocrystals and Their Solids: Correlation between Surface Chemistry and Optoelectronic Properties
journal, November 2014

  • Goodwin, E. D.; Diroll, Benjamin T.; Oh, Soong Ju
  • The Journal of Physical Chemistry C, Vol. 118, Issue 46
  • DOI: 10.1021/jp5076912

Hydroxylation of the surface of PbS nanocrystals passivated with oleic acid
journal, May 2014


Electrodeposition of patterned CdSe nanocrystal films using thermally charged nanocrystals
journal, May 2002

  • Islam, Mohammad A.; Herman, Irving P.
  • Applied Physics Letters, Vol. 80, Issue 20
  • DOI: 10.1063/1.1480878

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films
journal, July 2017


Collective topo-epitaxy in the self-assembly of a 3D quantum dot superlattice
journal, October 2019


Decoding the Superlattice and Interface Structure of Truncate PbS Nanocrystal-Assembled Supercrystal and Associated Interaction Forces
journal, August 2014

  • Li, Ruipeng; Bian, Kaifu; Hanrath, Tobias
  • Journal of the American Chemical Society, Vol. 136, Issue 34
  • DOI: 10.1021/ja5057032

Photoconductivity studies of treated CdSe quantum dot films exhibiting increased exciton ionization efficiency
journal, November 2004


Micron Thick Colloidal Quantum Dot Solids
journal, June 2020


Space- and time-resolved small angle X-ray scattering to probe assembly of silver nanocrystal superlattices
journal, October 2018


Properties and potential optoelectronic applications of lead halide perovskite nanocrystals
journal, November 2017

  • Kovalenko, Maksym V.; Protesescu, Loredana; Bodnarchuk, Maryna I.
  • Science, Vol. 358, Issue 6364
  • DOI: 10.1126/science.aam7093

Exceptionally Mild Reactive Stripping of Native Ligands from Nanocrystal Surfaces by Using Meerwein’s Salt
journal, December 2011

  • Rosen, Evelyn L.; Buonsanti, Raffaella; Llordes, Anna
  • Angewandte Chemie International Edition, Vol. 51, Issue 3, p. 684-689
  • DOI: 10.1002/anie.201105996

CdS/PbSe heterojunction for high temperature mid-infrared photovoltaic detector applications
journal, March 2014

  • Weng, Binbin; Qiu, Jijun; Zhao, Lihua
  • Applied Physics Letters, Vol. 104, Issue 12
  • DOI: 10.1063/1.4869752

Properties of PbS, PbSe, and PbTe
journal, March 1980


Nanocrystal photovoltaics: a review of recent progress
journal, May 2013

  • Stolle, C. Jackson; Harvey, Taylor B.; Korgel, Brian A.
  • Current Opinion in Chemical Engineering, Vol. 2, Issue 2, p. 160-167
  • DOI: 10.1016/j.coche.2013.03.001

Mid-infrared HgTe colloidal quantum dot photodetectors
journal, July 2011


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
  • DOI: 10.1021/ja800040c

Van der Waals Density Functional for General Geometries
journal, June 2004


Adsorption of 3-Thiophene Carboxylic Acid on Silver Nanocolloids: FTIR, Raman, and SERS Study Aided by Density Functional Theory
journal, July 2011

  • Chandra, Subhendu; Chowdhury, Joydeep; Ghosh, Manash
  • The Journal of Physical Chemistry C, Vol. 115, Issue 29
  • DOI: 10.1021/jp204297y

Colloidal nanocrystals for quality lighting and displays: milestones and recent developments
journal, June 2016


Colloidal quantum dot photodetectors
journal, May 2011


Synthesis, characterization and electrochemical characterization of lead selenide sub-micron particles capped with a benzoate ligand and prepared at different temperatures
journal, September 2014

  • Rodríguez-Rodríguez, Weyshla A.; Colón, Jadiel; Guzmán, Roger
  • Materials Research Express, Vol. 1, Issue 3
  • DOI: 10.1088/2053-1591/1/3/035906

Pushing the Band Gap Envelope:  Mid-Infrared Emitting Colloidal PbSe Quantum Dots
journal, September 2004

  • Pietryga, Jeffrey M.; Schaller, Richard D.; Werder, Donald
  • Journal of the American Chemical Society, Vol. 126, Issue 38
  • DOI: 10.1021/ja047659f

Charge transport in strongly coupled quantum dot solids
journal, November 2015

  • Kagan, Cherie R.; Murray, Christopher B.
  • Nature Nanotechnology, Vol. 10, Issue 12
  • DOI: 10.1038/nnano.2015.247

Colloidal quantum dot ligand engineering for high performance solar cells
journal, January 2016

  • Wang, Ruili; Shang, Yuequn; Kanjanaboos, Pongsakorn
  • Energy & Environmental Science, Vol. 9, Issue 4
  • DOI: 10.1039/C5EE03887A

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
  • DOI: 10.1021/cr900137k

Ligand-Induced Shape Transformation of PbSe Nanocrystals
journal, April 2017


The Electrophoretic Deposition of Inorganic Nanoscaled Materials —A Review—
journal, January 2006

  • Boccaccini, Aldo R.; Roether, Judith A.; Thomas, Boris J. C.
  • Journal of the Ceramic Society of Japan, Vol. 114, Issue 1325
  • DOI: 10.2109/jcersj.114.1

Self-Assembly of Colloidal Nanocrystals: From Intricate Structures to Functional Materials
journal, August 2016


Bandlike Transport in Strongly Coupled and Doped Quantum Dot Solids: A Route to High-Performance Thin-Film Electronics
journal, April 2012

  • Choi, Ji-Hyuk; Fafarman, Aaron T.; Oh, Soong Ju
  • Nano Letters, Vol. 12, Issue 5
  • DOI: 10.1021/nl301104z

A Photoconductor Intrinsically Has No Gain
journal, September 2018