Auger Heating and Thermal Dissipation in Zero-Dimensional CdSe Nanocrystals Examined Using Femtosecond Stimulated Raman Spectroscopy

Harvey, Samantha M.; Phelan, Brian T.; Hannah, Daniel C.; Brown, Kristen E.; Young, Ryan M.; Kirschner, Matthew S.; Wasielewski, Michael R.; Schaller, Richard D.

doi:10.1021/acs.jpclett.8b01504

Title: Auger Heating and Thermal Dissipation in Zero-Dimensional CdSe Nanocrystals Examined Using Femtosecond Stimulated Raman Spectroscopy

Journal Article · Mon Jul 16 00:00:00 EDT 2018 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.8b01504· OSTI ID:1491813

Harvey, Samantha M. ^[1]; Phelan, Brian T. ^[1]; Hannah, Daniel C. ^[1]; Brown, Kristen E. ^[1];

^[1]; Kirschner, Matthew S. ^[1];

^[1];

^[2]

Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

In this paper, we report femtosecond stimulated Raman spectroscopy (FSRS) measurements on dispersions of CdSe semiconductor nanocrystals (NCs) as a function of particle size and pump fluence. Upon photoexcitation we observe depletion of stimulated Raman gain corresponding to generation of longitudinal optical (LO) phonons followed by recovery on picosecond timescales. At higher fluences, production of multiple excitons slows recovery of FSRS signals, which we attribute to sustained increases of LO phonon populations due to multiexcitonic Auger heating. Additionally, owing to discretized electronic structure of these NCs, such heating cannot be readily monitored via electronic spectroscopic analysis of high energy band tails as has been performed for higher-dimensionality materials. Notably, recovery timescales exceed those of the biexcitonic Auger recombination process and as such reveal overall thermalization timescales likely owing to an acoustic phonon thermalization bottleneck that dictates the cooling timescale.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357; FG02-99ER14999

OSTI ID:: 1491813

Journal Information:: Journal of Physical Chemistry Letters, Vol. 9, Issue 16; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 13 works

Citation information provided by
Web of Science

References (49)

Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer Colvin, V. L.; Schlamp, M. C.; Alivisatos, A. P. Nature, Vol. 370, Issue 6488 https://doi.org/10.1038/370354a0	journal	August 1994
Full Color Emission from II-VI Semiconductor Quantum Dot-Polymer Composites Lee, J.; Sundar, V. C.; Heine, J. R. Advanced Materials, Vol. 12, Issue 15, p. 1102-1105 https://doi.org/10.1002/1521-4095(200008)12:15<1102::AID-ADMA1102>3.0.CO;2-J	journal	July 2000
Quantum Dots as Cellular Probes Alivisatos, A. Paul; Gu, Weiwei; Larabell, Carolyn Annual Review of Biomedical Engineering, Vol. 7, Issue 1 https://doi.org/10.1146/annurev.bioeng.7.060804.100432	journal	August 2005
Bioanalytics and biolabeling with semiconductor nanoparticles (quantum dots) Lin, Cheng-An J.; Liedl, Tim; Sperling, Ralph A. J. Mater. Chem., Vol. 17, Issue 14 https://doi.org/10.1039/B618902D	journal	January 2007
Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots Klimov, V. I.; Mikhailovsky, A. A.; Xu, Su Science, Vol. 290, Issue 5490, p. 314-317 https://doi.org/10.1126/science.290.5490.314	journal	October 2000
Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces Park, Young-Shin; Bae, Wan Ki; Baker, Thomas Nano Letters, Vol. 15, Issue 11 https://doi.org/10.1021/acs.nanolett.5b02595	journal	October 2015
Colloidal Quantum Dot Solar Cells Carey, Graham H.; Abdelhady, Ahmed L.; Ning, Zhijun Chemical Reviews, Vol. 115, Issue 23 https://doi.org/10.1021/acs.chemrev.5b00063	journal	June 2015
Hybrid Photovoltaics Based on Semiconductor Nanocrystals and Amorphous Silicon Sun, Baoquan; Findikoglu, Alp T.; Sykora, Milan Nano Letters, Vol. 9, Issue 3 https://doi.org/10.1021/nl9001469	journal	March 2009
Semiconductor Clusters, Nanocrystals, and Quantum Dots Alivisatos, A. P. Science, Vol. 271, Issue 5251, p. 933-937 https://doi.org/10.1126/science.271.5251.933	journal	February 1996
Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy Ulbricht, Ronald; Hendry, Euan; Shan, Jie Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.543	journal	June 2011
Performance Degradation of High-Brightness Light Emitting Diodes Under DC and Pulsed Bias Buso, S.; Spiazzi, G.; Meneghini, M. IEEE Transactions on Device and Materials Reliability, Vol. 8, Issue 2 https://doi.org/10.1109/TDMR.2008.916549	journal	June 2008
Cooling of photovoltaic cells under concentrated illumination: a critical review Royne, A.; Dey, C.; Mills, D. Solar Energy Materials and Solar Cells, Vol. 86, Issue 4 https://doi.org/10.1016/j.solmat.2004.09.003	journal	April 2005
Exciton Fate in Semiconductor Nanocrystals at Elevated Temperatures: Hole Trapping Outcompetes Exciton Deactivation Rowland, Clare E.; Schaller, Richard D. The Journal of Physical Chemistry C, Vol. 117, Issue 33 https://doi.org/10.1021/jp405616u	journal	August 2013
Size- and temperature-dependence of exciton lifetimes in CdSe quantum dots de Mello Donegá, C.; Bode, M.; Meijerink, A. Physical Review B, Vol. 74, Issue 8 https://doi.org/10.1103/PhysRevB.74.085320	journal	August 2006
The effect of Auger heating on intraband carrier relaxation in semiconductor quantum rods Achermann, Marc; Bartko, Andrew P.; Hollingsworth, Jennifer A. Nature Physics, Vol. 2, Issue 8 https://doi.org/10.1038/nphys363	journal	July 2006
Carrier Cooling in Colloidal Quantum Wells Pelton, Matthew; Ithurria, Sandrine; Schaller, Richard D. Nano Letters, Vol. 12, Issue 12 https://doi.org/10.1021/nl302986y	journal	February 2012
Observation of Size-Dependent Thermalization in CdSe Nanocrystals Using Time-Resolved Photoluminescence Spectroscopy Hannah, Daniel C.; Dunn, Nicholas J.; Ithurria, Sandrine Physical Review Letters, Vol. 107, Issue 17 https://doi.org/10.1103/PhysRevLett.107.177403	journal	October 2011
Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation Kirschner, Matthew S.; Hannah, Daniel C.; Diroll, Benjamin T. Nano Letters, Vol. 17, Issue 9 https://doi.org/10.1021/acs.nanolett.7b01705	journal	August 2017
Surface chemistry mediates thermal transport in three-dimensional nanocrystal arrays Ong, Wee-Liat; Rupich, Sara M.; Talapin, Dmitri V. Nature Materials, Vol. 12, Issue 5 https://doi.org/10.1038/nmat3596	journal	March 2013
Electron and hole relaxation pathways in semiconductor quantum dots Klimov, V. I.; McBranch, D. W.; Leatherdale, C. A. Physical Review B, Vol. 60, Issue 19 https://doi.org/10.1103/PhysRevB.60.13740	journal	November 1999
Intraband relaxation in CdSe quantum dots Guyot-Sionnest, Philippe; Shim, Moonsub; Matranga, Chris Physical Review B, Vol. 60, Issue 4 https://doi.org/10.1103/PhysRevB.60.R2181	journal	July 1999
Unraveling the Structure and Dynamics of Excitons in Semiconductor Quantum Dots Kambhampati, Patanjali Accounts of Chemical Research, Vol. 44, Issue 1 https://doi.org/10.1021/ar1000428	journal	January 2011
Femtosecond $1 P$ -to- $1 S$ Electron Relaxation in Strongly Confined Semiconductor Nanocrystals Klimov, Victor I.; McBranch, Duncan W. Physical Review Letters, Vol. 80, Issue 18 https://doi.org/10.1103/PhysRevLett.80.4028	journal	May 1998
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
Multiexcitons confined within a subexcitonic volume: Spectroscopic and dynamical signatures of neutral and charged biexcitons in ultrasmall semiconductor nanocrystals Achermann, M.; Hollingsworth, J. A.; Klimov, V. I. Physical Review B, Vol. 68, Issue 24 https://doi.org/10.1103/PhysRevB.68.245302	journal	December 2003
Scaling of multiexciton lifetimes in semiconductor nanocrystals Klimov, V. I.; McGuire, J. A.; Schaller, R. D. Physical Review B, Vol. 77, Issue 19 https://doi.org/10.1103/PhysRevB.77.195324	journal	May 2008
Multicarrier recombination in colloidal quantum dots Pandey, Anshu; Guyot-Sionnest, Philippe The Journal of Chemical Physics, Vol. 127, Issue 11 https://doi.org/10.1063/1.2786068	journal	September 2007
Multiexciton fluorescence from semiconductor nanocrystals Fisher, Brent; Caruge, Jean-Michel; Chan, Yin-Thai Chemical Physics, Vol. 318, Issue 1-2, p. 71-81 https://doi.org/10.1016/j.chemphys.2005.05.036	journal	November 2005
Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: Intrinsic limits to the dark-exciton lifetime Crooker, S. A.; Barrick, T.; Hollingsworth, J. A. Applied Physics Letters, Vol. 82, Issue 17 https://doi.org/10.1063/1.1570923	journal	April 2003
Theory of Thermal Relaxation of Electrons in Semiconductors Sadasivam, Sridhar; Chan, Maria K. Y.; Darancet, Pierre Physical Review Letters, Vol. 119, Issue 13 https://doi.org/10.1103/PhysRevLett.119.136602	journal	September 2017
Reverse Non-Equilibrium Molecular Dynamics Demonstrate That Surface Passivation Controls Thermal Transport at Semiconductor–Solvent Interfaces Hannah, Daniel C.; Gezelter, J. Daniel; Schaller, Richard D. ACS Nano, Vol. 9, Issue 6 https://doi.org/10.1021/acsnano.5b01724	journal	May 2015
Identification of parameters through which surface chemistry determines the lifetimes of hot electrons in small Au nanoparticles Aruda, Kenneth O.; Tagliazucchi, Mario; Sweeney, Christina M. Proceedings of the National Academy of Sciences, Vol. 110, Issue 11 https://doi.org/10.1073/pnas.1222327110	journal	February 2013
Study of Heat Transfer Dynamics from Gold Nanorods to the Environment via Time-Resolved Infrared Spectroscopy Nguyen, Son C.; Zhang, Qiao; Manthiram, Karthish ACS Nano, Vol. 10, Issue 2 https://doi.org/10.1021/acsnano.5b06623	journal	January 2016
Energy Flow from Solute to Solvent Probed by Femtosecond IR Spectroscopy: Malachite Green and Heme Protein Solutions Lian, Tianquan; Locke, Bruce; Kholodenko, Yuriy The Journal of Physical Chemistry, Vol. 98, Issue 45 https://doi.org/10.1021/j100096a005	journal	November 1994
Phonon Spectra of Small Colloidal II-VI Semiconductor Nanocrystals Dzhagan, Volodymyr; Valakh, Mykhailo; Mel'nik, Nikolai International Journal of Spectroscopy, Vol. 2012 https://doi.org/10.1155/2012/532385	journal	September 2012
Size-Dependent Photoconductivity in CdSe Nanoparticles as Measured by Time-Resolved Terahertz Spectroscopy Beard, Matthew C.; Turner, Gordon M.; Schmuttenmaer, Charles A. Nano Letters, Vol. 2, Issue 9 https://doi.org/10.1021/nl0256210	journal	September 2002
Direct Measurement of Lattice Dynamics and Optical Phonon Excitation in Semiconductor Nanocrystals Using Femtosecond Stimulated Raman Spectroscopy Hannah, Daniel C.; Brown, Kristen E.; Young, Ryan M. Physical Review Letters, Vol. 111, Issue 10 https://doi.org/10.1103/PhysRevLett.111.107401	journal	September 2013
Femtosecond stimulated Raman spectroscopy Frontiera, R. R.; Mathies, R. A. Laser & Photonics Reviews, Vol. 5, Issue 1 https://doi.org/10.1002/lpor.200900048	journal	December 2010
Femtosecond Stimulated Raman Spectroscopy Kukura, Philipp; McCamant, David W.; Mathies, Richard A. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.032806.104456	journal	May 2007
Vibrational Dynamics of a Perylene–Perylenediimide Donor–Acceptor Dyad Probed with Femtosecond Stimulated Raman Spectroscopy Brown, Kristen E.; Veldkamp, Brad S.; Co, Dick T. The Journal of Physical Chemistry Letters, Vol. 3, Issue 17 https://doi.org/10.1021/jz301107c	journal	August 2012
Excited-state Raman spectroscopy with and without actinic excitation: S ₁ Raman spectra of trans-azobenzene Dobryakov, A. L.; Quick, M.; Ioffe, I. N. The Journal of Chemical Physics, Vol. 140, Issue 18 https://doi.org/10.1063/1.4874854	journal	May 2014
Resonance Femtosecond-Stimulated Raman Spectroscopy without Actinic Excitation Showing Low-Frequency Vibrational Activity in the S ₂ State of All-Trans β-Carotene Quick, Martin; Dobryakov, Alexander L.; Kovalenko, Sergey A. The Journal of Physical Chemistry Letters, Vol. 6, Issue 7 https://doi.org/10.1021/acs.jpclett.5b00243	journal	March 2015
Theory of femtosecond stimulated Raman spectroscopy Lee, Soo-Y.; Zhang, Donghui; McCamant, David W. The Journal of Chemical Physics, Vol. 121, Issue 8 https://doi.org/10.1063/1.1777214	journal	August 2004
Quantum theory of (femtosecond) time-resolved stimulated Raman scattering Sun, Zhigang; Lu, J.; Zhang, Dong H. The Journal of Chemical Physics, Vol. 128, Issue 14 https://doi.org/10.1063/1.2888551	journal	April 2008
Resonance Raman depolarization in CdSe nanocrystals Shiang, J. J.; Craig, I. M.; Alivisatos, A. P. Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 26, Issue 1-4 https://doi.org/10.1007/BF01429194	journal	March 1993
The “Surface Optical” Phonon in CdSe Nanocrystals Lin, Chen; Kelley, David F.; Rico, Mikaela ACS Nano, Vol. 8, Issue 4 https://doi.org/10.1021/nn5008513	journal	March 2014
Optical Studies of Dynamics in Noble Metal Nanostructures Hartland, Gregory V. Chemical Reviews, Vol. 111, Issue 6 https://doi.org/10.1021/cr1002547	journal	June 2011
Auger Processes in Nanosize Semiconductor Crystals Efros, Alexander Semiconductor Nanocrystals https://doi.org/10.1007/978-1-4757-3677-9_2	book	January 2003
Screening of hot-carrier relaxation in highly photoexcited semiconductors Yoffa, Ellen J. Physical Review B, Vol. 23, Issue 4 https://doi.org/10.1103/PhysRevB.23.1909	journal	February 1981

Cited By (1)

Reducing the Chromaticity Shifts of Light‐Emitting Diodes Using Gradient‐Alloyed Cd _x Zn ₁₋ _x Se _y S ₁₋ _y @ZnS Core Shell Quantum Dots with Enhanced High‐Temperature Photoluminescence Tang, Jialun; Li, Fei; Yang, Gaoling Advanced Optical Materials, Vol. 7, Issue 10 https://doi.org/10.1002/adom.201801687	journal	February 2019

Figures / Tables (4)

Similar Records

Size-Dependent Asymmetric Auger Interactions in Plasma-Produced n- and p-Type-Doped Silicon Nanocrystals

Journal Article · Wed Feb 13 00:00:00 EST 2019 · Journal of Physical Chemistry. C · OSTI ID:1491813

Limpens, Rens; Pach, Gregory F.; Mulder, David W.; +1 more

Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids

Journal Article · Mon Mar 16 00:00:00 EDT 2015 · Nature Materials · OSTI ID:1491813

Rowland, Clare E.; Fedin, Igor; Zhang, Hui; +4 more

Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates

Journal Article · Wed Nov 29 00:00:00 EST 2017 · Nanoscale · OSTI ID:1491813

Guo, Tianle; Sampat, Siddharth; Rupich, Sara M.; +6 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE