Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.

doi:10.1038/ncomms9185

Title: Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

Journal Article · Tue Sep 08 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms9185· OSTI ID:1224438

Gao, Jianbo ^[1]; Fidler, Andrew F. ^[2]; Klimov, Victor I. ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, Berkeley, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects of electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1224438

Report Number(s):: LA-UR-15-25555; ncomms9185

Journal Information:: Nature Communications, Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 49 works

Citation information provided by
Web of Science

References (55)

Novel optimization principles and efficiency limits for semiconductor solar cells Werner, Jürgen H.; Kolodinski, Sabine; Queisser, Hans J. Physical Review Letters, Vol. 72, Issue 24 https://doi.org/10.1103/PhysRevLett.72.3851	journal	June 1994
Quantum dot solar cells Nozik, A. J. Physica E: Low-dimensional Systems and Nanostructures, Vol. 14, Issue 1-2, p. 115-120 https://doi.org/10.1016/S1386-9477(02)00374-0	journal	April 2002
The quantum efficiency of the photo-electric effect in germanium for the 0.3–2 μ wavelength region Koc, Stanislav Czechoslovak Journal of Physics, Vol. 7, Issue 1 https://doi.org/10.1007/BF01688719	journal	January 1957
High Efficiency Carrier Multiplication in PbSe Nanocrystals: Implications for Solar Energy Conversion Schaller, R. D.; Klimov, V. I. Physical Review Letters, Vol. 92, Issue 18 https://doi.org/10.1103/PhysRevLett.92.186601	journal	May 2004
Enhanced carrier multiplication in engineered quasi-type-II quantum dots Cirloganu, Claudiu M.; Padilha, Lazaro A.; Lin, Qianglu Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5148	journal	June 2014
Evidence for Barrierless Auger Recombination in PbSe Nanocrystals: A Pressure-Dependent Study of Transient Optical Absorption Pietryga, Jeffrey M.; Zhuravlev, Kirill K.; Whitehead, Michael Physical Review Letters, Vol. 101, Issue 21 https://doi.org/10.1103/PhysRevLett.101.217401	journal	November 2008
Multiexciton Generation by a Single Photon in Nanocrystals Shabaev, A.; Efros, Al. L.; Nozik, A. J. Nano Letters, Vol. 6, Issue 12 https://doi.org/10.1021/nl062059v	journal	December 2006
Carrier multiplication in semiconductor nanocrystals via intraband optical transitions involving virtual biexciton states Rupasov, Valery I.; Klimov, Victor I. Physical Review B, Vol. 76, Issue 12 https://doi.org/10.1103/PhysRevB.76.125321	journal	September 2007
PbTe Colloidal Nanocrystals: Synthesis, Characterization, and Multiple Exciton Generation Murphy, James E.; Beard, Matthew C.; Norman, Andrew G. Journal of the American Chemical Society, Vol. 128, Issue 10 https://doi.org/10.1021/ja0574973	journal	March 2006
Carrier Multiplication in InAs Nanocrystal Quantum Dots with an Onset Defined by the Energy Conservation Limit Schaller, Richard D.; Pietryga, Jeffrey M.; Klimov, Victor I. Nano Letters, Vol. 7, Issue 11 https://doi.org/10.1021/nl072046x	journal	November 2007
Multiple Exciton Generation in Colloidal Silicon Nanocrystals Beard, Matthew C.; Knutsen, Kelly P.; Yu, Pingrong Nano Letters, Vol. 7, Issue 8 https://doi.org/10.1021/nl071486l	journal	August 2007
Carrier Multiplication in CdTe Quantum Dots by Single-photon Timing Spectroscopy Kobayashi, Yoichi; Udagawa, Takeshi; Tamai, Naoto Chemistry Letters, Vol. 38, Issue 8 https://doi.org/10.1246/cl.2009.830	journal	August 2009
Efficient carrier multiplication in InP nanoparticles Stubbs, Stuart K.; Hardman, Samantha J. O.; Graham, Darren M. Physical Review B, Vol. 81, Issue 8 https://doi.org/10.1103/PhysRevB.81.081303	journal	February 2010
Direct generation of multiple excitons in adjacent silicon nanocrystals revealed by induced absorption Trinh, M. Tuan; Limpens, Rens; de Boer, Wieteke D. A. M. Nature Photonics, Vol. 6, Issue 5 https://doi.org/10.1038/nphoton.2012.36	journal	March 2012
Aspect Ratio Dependence of Auger Recombination and Carrier Multiplication in PbSe Nanorods Padilha, Lazaro A.; Stewart, John T.; Sandberg, Richard L. Nano Letters, Vol. 13, Issue 3 https://doi.org/10.1021/nl304426y	journal	February 2013
An Upper Bound to Carrier Multiplication Efficiency in Type II Colloidal Quantum Dots Gachet, David; Avidan, Assaf; Pinkas, Iddo Nano Letters, Vol. 10, Issue 1 https://doi.org/10.1021/nl903172f	journal	January 2010
Multiple Exciton Generation in Single-Walled Carbon Nanotubes Wang, Shujing; Khafizov, Marat; Tu, Xiaomin Nano Letters, Vol. 10, Issue 7 https://doi.org/10.1021/nl100343j	journal	July 2010
Experimental Verification of Carrier Multiplication in Graphene Plötzing, T.; Winzer, T.; Malic, E. Nano Letters, Vol. 14, Issue 9 https://doi.org/10.1021/nl502114w	journal	August 2014
Colloidal Quantum-Dot Photodetectors Exploiting Multiexciton Generation Sukhovatkin, V.; Hinds, S.; Brzozowski, L. Science, Vol. 324, Issue 5934 https://doi.org/10.1126/science.1173812	journal	June 2009
Multiple Exciton Collection in a Sensitized Photovoltaic System Sambur, J. B.; Novet, T.; Parkinson, B. A. Science, Vol. 330, Issue 6000 https://doi.org/10.1126/science.1191462	journal	September 2010
Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell Semonin, O. E.; Luther, J. M.; Choi, S. Science, Vol. 334, Issue 6062 https://doi.org/10.1126/science.1209845	journal	December 2011
High-Energy Excitations in Silicon Nanoparticles Gali, Adam; Vörös, Márton; Rocca, Dario Nano Letters, Vol. 9, Issue 11 https://doi.org/10.1021/nl901970u	journal	November 2009
Exciton Multiplication from First Principles Jaeger, Heather M.; Hyeon-Deuk, Kim; Prezhdo, Oleg V. Accounts of Chemical Research, Vol. 46, Issue 6 https://doi.org/10.1021/ar3002365	journal	March 2013
Theory of multiexciton generation in semiconductor nanocrystals Rabani, Eran; Baer, Roi Chemical Physics Letters, Vol. 496, Issue 4-6 https://doi.org/10.1016/j.cplett.2010.07.059	journal	August 2010
Direct carrier multiplication due to inverse Auger scattering in CdSe quantum dots Califano, Marco; Zunger, Alex; Franceschetti, Alberto Applied Physics Letters, Vol. 84, Issue 13 https://doi.org/10.1063/1.1690104	journal	March 2004
Multicarrier Interactions in Semiconductor Nanocrystals in Relation to the Phenomena of Auger Recombination and Carrier Multiplication Klimov, Victor I. Annual Review of Condensed Matter Physics, Vol. 5, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031113-133900	journal	March 2014
Generating Free Charges by Carrier Multiplication in Quantum Dots for Highly Efficient Photovoltaics ten Cate, Sybren; Sandeep, C. S. Suchand; Liu, Yao Accounts of Chemical Research, Vol. 48, Issue 2 https://doi.org/10.1021/ar500248g	journal	January 2015
Third Generation Photovoltaics based on Multiple Exciton Generation in Quantum Confined Semiconductors Beard, Matthew C.; Luther, Joseph M.; Semonin, Octavi E. Accounts of Chemical Research, Vol. 46, Issue 6 https://doi.org/10.1021/ar3001958	journal	October 2012
Quantum Dot Solar Cells. Semiconductor Nanocrystals as Light Harvesters Kamat, Prashant V. The Journal of Physical Chemistry C, Vol. 112, Issue 48 https://doi.org/10.1021/jp806791s	journal	October 2008
Electroluminescence from single monolayers of nanocrystals in molecular organic devices Coe, Seth; Woo, Wing-Keung; Bawendi, Moungi Nature, Vol. 420, Issue 6917 https://doi.org/10.1038/nature01217	journal	December 2002
Schottky Solar Cells Based on Colloidal Nanocrystal Films Luther, Joseph M.; Law, Matt; Beard, Matthew C. Nano Letters, Vol. 8, Issue 10 https://doi.org/10.1021/nl802476m	journal	October 2008
Ultrasensitive solution-cast quantum dot photodetectors Konstantatos, Gerasimos; Howard, Ian; Fischer, Armin Nature, Vol. 442, Issue 7099 https://doi.org/10.1038/nature04855	journal	July 2006
High charge-carrier mobility enables exploitation of carrier multiplication in quantum-dot films Sandeep, C. S. Suchand; Cate, Sybren ten; Schins, Juleon M. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3360	journal	August 2013
Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots Klimov, V. I. Science, Vol. 287, Issue 5455 https://doi.org/10.1126/science.287.5455.1011	journal	February 2000
Mechanism of Carrier Photogeneration and Carrier Transport in Molecular Crystal Tetracene Moses, Daniel; Soci, Cesare; Chi, Xialiou Physical Review Letters, Vol. 97, Issue 6 https://doi.org/10.1103/PhysRevLett.97.067401	journal	August 2006
Temperature-Independent Photoconductivity in Thin Films of Semiconducting Polymers: Photocarrier Sweep-Out Prior to Deep Trapping Moses, D.; Wang, J.; Yu, G. Physical Review Letters, Vol. 80, Issue 12 https://doi.org/10.1103/PhysRevLett.80.2685	journal	March 1998
Impulse response of photoconductors in transmission lines Auston, D. IEEE Journal of Quantum Electronics, Vol. 19, Issue 4 https://doi.org/10.1109/JQE.1983.1071904	journal	April 1983
Dependence of Carrier Mobility on Nanocrystal Size and Ligand Length in PbSe Nanocrystal Solids Liu, Yao; Gibbs, Markelle; Puthussery, James Nano Letters, Vol. 10, Issue 5 https://doi.org/10.1021/nl101284k	journal	May 2010
Bandlike Transport in Strongly Coupled and Doped Quantum Dot Solids: A Route to High-Performance Thin-Film Electronics Choi, Ji-Hyuk; Fafarman, Aaron T.; Oh, Soong Ju Nano Letters, Vol. 12, Issue 5 https://doi.org/10.1021/nl301104z	journal	April 2012
Band-like transport, high electron mobility and high photoconductivity in all-inorganic nanocrystal arrays Lee, Jong-Soo; Kovalenko, Maksym V.; Huang, Jing Nature Nanotechnology, Vol. 6, Issue 6 https://doi.org/10.1038/nnano.2011.46	journal	April 2011
PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors Talapin, D. V. Science, Vol. 310, Issue 5745, p. 86-89 https://doi.org/10.1126/science.1116703	journal	October 2005
Optical Nonlinearities and Ultrafast Carrier Dynamics in Semiconductor Nanocrystals Klimov, Victor I. The Journal of Physical Chemistry B, Vol. 104, Issue 26 https://doi.org/10.1021/jp9944132	journal	July 2000
Composition and Size-Dependent Extinction Coefficient of Colloidal PbSe Quantum Dots Moreels, Iwan; Lambert, Karel; De Muynck, David Chemistry of Materials, Vol. 19, Issue 25 https://doi.org/10.1021/cm071410q	journal	December 2007
New Aspects of Carrier Multiplication in Semiconductor Nanocrystals McGuire, John A.; Joo, Jin; Pietryga, Jeffrey M. Accounts of Chemical Research, Vol. 41, Issue 12 https://doi.org/10.1021/ar800112v	journal	December 2008
Impact ionization in silicon: A review and update Maes, W.; De Meyer, K.; Van Overstraeten, R. Solid-State Electronics, Vol. 33, Issue 6 https://doi.org/10.1016/0038-1101(90)90183-F	journal	June 1990
Engineering colloidal quantum dot solids within and beyond the mobility-invariant regime Zhitomirsky, David; Voznyy, Oleksandr; Levina, Larissa Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4803	journal	May 2014
Highly Effective Surface Passivation of PbSe Quantum Dots through Reaction with Molecular Chlorine Bae, Wan Ki; Joo, Jin; Padilha, Lazaro A. Journal of the American Chemical Society, Vol. 134, Issue 49 https://doi.org/10.1021/ja309783v	journal	November 2012
Quantum Dot Size Dependent J − V Characteristics in Heterojunction ZnO/PbS Quantum Dot Solar Cells Gao, Jianbo; Luther, Joseph M.; Semonin, Octavi E. Nano Letters, Vol. 11, Issue 3 https://doi.org/10.1021/nl103814g	journal	March 2011
Quantum dot solar cells Raffaelle, Ryne P.; Castro, Stephanie L.; Hepp, Aloysius F. Progress in Photovoltaics: Research and Applications, Vol. 10, Issue 6 https://doi.org/10.1002/pip.452	journal	January 2002
Impact ionization in silicon: a review and update Maes, W.; De Meyer, K.; Van Overstraeten, R. Microelectronics Reliability, Vol. 32, Issue 1-2, p. 301 https://doi.org/10.1016/0026-2714(92)90255-j	journal	January 1992
Quantum dot solar cells Aroutiounian, V.; Petrosyan, S.; Khachatryan, A. Journal of Applied Physics, Vol. 89, Issue 4 https://doi.org/10.1063/1.1339210	journal	February 2001
Quantum simulation of multiple-exciton generation in a nanocrystal by a single photon Witzel, Wayne M.; Shabaev, Andrew; Hellberg, C. Stephen arXiv https://doi.org/10.48550/arxiv.1005.4069	text	January 2010
Theory of multiexciton generation in semiconductor nanocrystals Rabani, Eran; Baer, Roi arXiv https://doi.org/10.48550/arxiv.1007.1090	text	January 2010
Role of impact ionization in multiple exciton generation in PbSe nanocrystals Allan, G.; Delerue, C. Physical Review B, Vol. 73, Issue 20 https://doi.org/10.1103/physrevb.73.205423	journal	May 2006
Non-Poissonian Exciton Populations in Semiconductor Nanocrystals via Carrier Multiplication Schaller, Richard D.; Klimov, Victor I. Physical Review Letters, Vol. 96, Issue 9 https://doi.org/10.1103/physrevlett.96.097402	journal	March 2006

Cited By (10)

Tuning Areal Density and Surface Passivation of ZnO Nanowire Array Enable Efficient PbS QDs Solar Cells with Enhanced Current Density Tavakoli Dastjerdi, Hadi; Prochowicz, Daniel; Yadav, Pankaj Advanced Materials Interfaces, Vol. 7, Issue 1 https://doi.org/10.1002/admi.201901551	journal	November 2019
Biexciton Auger recombination in mono-dispersed, quantum-confined CsPbBr3 perovskite nanocrystals obeys universal volume-scaling Li, Yulu; Ding, Tao; Luo, Xiao Nano Research, Vol. 12, Issue 3 https://doi.org/10.1007/s12274-018-2266-7	journal	December 2018
Solution-processed semiconductors for next-generation photodetectors García de Arquer, F. Pelayo; Armin, Ardalan; Meredith, Paul Nature Reviews Materials, Vol. 2, Issue 3 https://doi.org/10.1038/natrevmats.2016.100	journal	January 2017
Auger electron emission initiated by the creation of valence-band holes in graphene by positron annihilation Chirayath, V. A.; Callewaert, V.; Fairchild, A. J. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms16116	journal	July 2017
Synergistic ligand exchange and UV curing of PbS quantum dots for effective surface passivation Tavakoli Dastjerdi, Hadi; Prochowicz, Daniel; Yadav, Pankaj Nanoscale, Vol. 11, Issue 47 https://doi.org/10.1039/c9nr07854a	journal	January 2019
Low-cost uncooled MWIR PbSe quantum dots photodiodes Qiu, Jijun; Weng, Binbin; McDowell, Lance L. RSC Advances, Vol. 9, Issue 72 https://doi.org/10.1039/c9ra07664f	journal	January 2019
Strategy to overcome recombination limited photocurrent generation in CsPbX ₃ nanocrystal arrays Mir, Wasim J.; Livache, Clément; Goubet, Nicolas Applied Physics Letters, Vol. 112, Issue 11 https://doi.org/10.1063/1.5009432	journal	March 2018
Sub-50 picosecond to microsecond carrier transport dynamics in pentacene thin films Adhikari, Pan; Kobbekaduwa, Kanishka; Shi, Ying Applied Physics Letters, Vol. 113, Issue 18 https://doi.org/10.1063/1.5048108	journal	October 2018
Shape-modulated multiple exciton generation and optoelectronic properties in PbSe nanostructures He, Yan; Ouyang, Tianyi; Ouyang, Gang Journal of Applied Physics, Vol. 124, Issue 18 https://doi.org/10.1063/1.5048382	journal	November 2018
Multiple Exciton Generation in Nanostructures for Advanced Photovoltaic Cells Siemons, Nicholas; Serafini, Alessio Journal of Nanotechnology, Vol. 2018 https://doi.org/10.1155/2018/7285483	journal	January 2018

Similar Records

Engineering of Lead Selenide Quantum Dot Based Devices and Core/Shell Heterostructures

Thesis/Dissertation · Fri May 01 00:00:00 EDT 2020 · OSTI ID:1224438

Nakotte, Tom

Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots

Journal Article · Tue Feb 16 00:00:00 EST 2016 · Nano Letters · OSTI ID:1224438

Makarov, Nikolay Sergeevich; Guo, Shaojun; Isaienko, Oleksandr; +3 more

Two‐Color Amplified Spontaneous Emission from Auger‐Suppressed Quantum Dots in Liquids

Journal Article · Fri Dec 08 00:00:00 EST 2023 · Advanced Materials · OSTI ID:1224438

Li, Xueyang; Du, Jun; Zhao, Guohui; +10 more

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
physical sciences
nanotechnology
optical physics
materials science

Title: Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

Citation Formats

References (55)

Cited By (10)

Similar Records

Related Subjects