Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene

Journal Article · · Scientific Reports
DOI:https://doi.org/10.1038/srep02004· OSTI ID:1382294

Colloidal nanocrystals (NCs) of lead chalcogenides are a promising class of tunable infrared materials for applications in devices such as photodetectors and solar cells. Such devices typically employ electronic materials in which charge carrier concentrations are manipulated through “doping;” however, persistent electronic doping of these NCs remains a challenge. Here, we demonstrate that heavily doped n-type PbSe and PbS NCs can be realized utilizing ground-state electron transfer from cobaltocene. This allows injecting up to eight electrons per NC into the band-edge state and maintaining the doping level for at least a month at room temperature. Doping is confirmed by inter- and intra-band optical absorption, as well as by carrier dynamics. Finally, FET measurements of doped NC films and the demonstration of a p-n diode provide additional evidence that the developed doping procedure allows for persistent incorporation of electrons into the quantum-confined NC states.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)
Sponsoring Organization:
USDOE SC Office of Basic Energy Sciences (SC-22)
DOE Contract Number:
AC52-06NA25396
OSTI ID:
1382294
Journal Information:
Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 3; ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

References (34)

Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications journal January 2010
A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids journal August 2012
Scaling of multiexciton lifetimes in semiconductor nanocrystals journal May 2008
Thiocyanate-Capped PbS Nanocubes: Ambipolar Transport Enables Quantum Dot Based Circuits on a Flexible Substrate journal November 2011
Chemical Redox Agents for Organometallic Chemistry journal January 1996
Size-Dependent Valence and Conduction Band-Edge Energies of Semiconductor Nanocrystals journal June 2011
A Reduction Pathway in the Synthesis of PbSe Nanocrystal Quantum Dots journal August 2009
Composition and Size-Dependent Extinction Coefficient of Colloidal PbSe Quantum Dots journal December 2007
PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors journal October 2005
Electron Injection from Colloidal PbS Quantum Dots into Titanium Dioxide Nanoparticles journal October 2008
Electron and Hole Injection in PbSe Quantum Dot Films journal July 2003
Spectroscopic Signatures of Photocharging due to Hot-Carrier Transfer in Solutions of Semiconductor Nanocrystals under Low-Intensity Ultraviolet Excitation journal October 2010
New Aspects of Carrier Multiplication in Semiconductor Nanocrystals journal December 2008
Comparison of Carrier Multiplication Yields in PbS and PbSe Nanocrystals: The Role of Competing Energy-Loss Processes journal January 2012
Role of mid-gap states in charge transport and photoconductivity in semiconductor nanocrystal films journal September 2011
Control of the Carrier Type in InAs Nanocrystal Films by Predeposition Incorporation of Cd journal December 2010
PbSe Quantum Dot Field-Effect Transistors with Air-Stable Electron Mobilities above 7 cm 2 V –1 s –1 journal March 2013
Utilizing the Lability of Lead Selenide to Produce Heterostructured Nanocrystals with Bright, Stable Infrared Emission journal April 2008
Impact of dithiol treatment and air annealing on the conductivity, mobility, and hole density in PbS colloidal quantum dot solids journal May 2008
Stoichiometry Control in Quantum Dots: A Viable Analog to Impurity Doping of Bulk Materials journal March 2013
Spectral and Dynamical Properties of Multiexcitons in Semiconductor Nanocrystals journal May 2007
n-type colloidal semiconductor nanocrystals journal October 2000
Effect of Air Exposure on Surface Properties, Electronic Structure, and Carrier Relaxation in PbSe Nanocrystals journal March 2010
Stoichiometric Control of Lead Chalcogenide Nanocrystal Solids to Enhance Their Electronic and Optoelectronic Device Performance journal February 2013
Size-Dependent Optical Properties of Colloidal PbS Quantum Dots journal September 2009
Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell journal December 2011
Controlled Chemical Doping of Semiconductor Nanocrystals Using Redox Buffers journal August 2012
Interband and Intraband Optical Studies of PbSe Colloidal Quantum Dots journal October 2002
PbSe Nanocrystal Network Formation during Pyridine Ligand Displacement journal January 2009
Colloidal PbS Nanocrystals with Size-Tunable Near-Infrared Emission: Observation of Post-Synthesis Self-Narrowing of the Particle Size Distribution journal November 2003
Selection rules for optical transitions in PbSe nanocrystal quantum dots: Drastic effect of structure inversion asymmetry journal June 2009
Heavily Doped Semiconductor Nanocrystal Quantum Dots journal March 2011
Electronic structure and optical properties of PbS and PbSe quantum dots journal January 1997
Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control journal May 2012

Cited By (16)

The Role of Dopant Ions on Charge Injection and Transport in Electrochemically Doped Quantum Dot Films journal May 2018
Electrically control amplified spontaneous emission in colloidal quantum dots journal October 2019
Level Anticrossing of Impurity States in Semiconductor Nanocrystals journal November 2014
PbE (E = S, Se) Colloidal Quantum Dot-Layered 2D Material Hybrid Photodetectors journal January 2020
Mid- and Long-Wave Infrared Optoelectronics via Intraband Transitions in PbS Colloidal Quantum Dots journal December 2019
25th Anniversary Article: Colloidal Quantum Dot Materials and Devices: A Quarter-Century of Advances journal September 2013
25th Anniversary Article: Colloidal Quantum Dot Materials and Devices: A Quarter-Century of Advances journal July 2015
Influence of L-Tryptophan on Growth and Optical Properties of PbS Nanocrystalline Thin Films journal July 2018
Tuning Carrier Mobilities and Polarity of Charge Transport in Films of CuInSexS2-x Quantum Dots journal January 2015
Air-stable n-type colloidal quantum dot solids journal June 2014
Charge-extraction strategies for colloidal quantum dot photovoltaics journal February 2014
Towards zero-threshold optical gain using charged semiconductor quantum dots journal October 2017
Colloidal quantum dot solids for solution-processed solar cells journal February 2016
Tin(IV) Methylselenolate as a Low Temperature SnSe Precursor and Conductive “Glue” Between Colloidal Nanocrystals journal January 2020
Enabling Ambipolar to Heavy n-Type Transport in PbS Quantum Dot Solids through Doping with Organic Molecules journal May 2017
Room-Temperature Electron Transport in Self-Assembled Sheets of PbSe Nanocrystals with a Honeycomb Nanogeometry journal May 2019