Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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

Abstract

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.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1491813
Grant/Contract Number:  
AC02-06CH11357; FG02-99ER14999
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 16; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Harvey, Samantha M., Phelan, Brian T., Hannah, Daniel C., Brown, Kristen E., Young, Ryan M., Kirschner, Matthew S., Wasielewski, Michael R., and Schaller, Richard D. Auger Heating and Thermal Dissipation in Zero-Dimensional CdSe Nanocrystals Examined Using Femtosecond Stimulated Raman Spectroscopy. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b01504.
Copy to clipboard
Harvey, Samantha M., Phelan, Brian T., Hannah, Daniel C., Brown, Kristen E., Young, Ryan M., Kirschner, Matthew S., Wasielewski, Michael R., & Schaller, Richard D. Auger Heating and Thermal Dissipation in Zero-Dimensional CdSe Nanocrystals Examined Using Femtosecond Stimulated Raman Spectroscopy. United States. https://doi.org/10.1021/acs.jpclett.8b01504
Copy to clipboard
Harvey, Samantha M., Phelan, Brian T., Hannah, Daniel C., Brown, Kristen E., Young, Ryan M., Kirschner, Matthew S., Wasielewski, Michael R., and Schaller, Richard D. Mon . "Auger Heating and Thermal Dissipation in Zero-Dimensional CdSe Nanocrystals Examined Using Femtosecond Stimulated Raman Spectroscopy". United States. https://doi.org/10.1021/acs.jpclett.8b01504. https://www.osti.gov/servlets/purl/1491813.
Copy to clipboard
@article{osti_1491813,
title = {Auger Heating and Thermal Dissipation in Zero-Dimensional CdSe Nanocrystals Examined Using Femtosecond Stimulated Raman Spectroscopy},
author = {Harvey, Samantha M. and Phelan, Brian T. and Hannah, Daniel C. and Brown, Kristen E. and Young, Ryan M. and Kirschner, Matthew S. and Wasielewski, Michael R. and Schaller, Richard D.},
abstractNote = {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.},
doi = {10.1021/acs.jpclett.8b01504},
journal = {Journal of Physical Chemistry Letters},
number = 16,
volume = 9,
place = {United States},
year = {Mon Jul 16 00:00:00 EDT 2018},
month = {Mon Jul 16 00:00:00 EDT 2018}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpclett.8b01504
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: (a) Schematic of a time-resolved FSRS experiment where the sample is first excited by a femtosecond actinic pump of controlled fluence followed by a pair of pulses at set time delays (Raman pump on the order of picoseconds and a femtosecond chirped broad-band probe) that produce stimulated Ramanmore » signal. (b) Absorption spectra of the three samples of CdSe NCs. The Raman pump wavelength is given as a (*) for each sample. (c) Example of a static FSRS spectrum for R = 1.3 nm CdSe. The LO phonon Raman features evident at approximately ±210 cm−1 sit atop a broad background along with the Rayleigh scattering (black line). This background is subtracted before data analysis (red line). (d) Schematic showing the optical excitation of a NC resulting in the creation of two excitons followed by subsequent relaxation and recombination. During intraband relaxation, cooling of hot carriers can generate LO phonons, causing the NC lattice to become heated. The combination of a Raman pump and probe allows stimulated Raman monitoring of these phonons.« less
All figures and tables (4 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer
journal, August 1994

  • Colvin, V. L.; Schlamp, M. C.; Alivisatos, A. P.
  • Nature, Vol. 370, Issue 6488
  • DOI: 10.1038/370354a0

Full Color Emission from II-VI Semiconductor Quantum Dot-Polymer Composites
journal, July 2000

Quantum Dots as Cellular Probes
journal, August 2005

Bioanalytics and biolabeling with semiconductor nanoparticles (quantum dots)
journal, January 2007

  • Lin, Cheng-An J.; Liedl, Tim; Sperling, Ralph A.
  • J. Mater. Chem., Vol. 17, Issue 14
  • DOI: 10.1039/B618902D

Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots
journal, October 2000

Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces
journal, October 2015

Colloidal Quantum Dot Solar Cells
journal, June 2015

Hybrid Photovoltaics Based on Semiconductor Nanocrystals and Amorphous Silicon
journal, March 2009

  • Sun, Baoquan; Findikoglu, Alp T.; Sykora, Milan
  • Nano Letters, Vol. 9, Issue 3
  • DOI: 10.1021/nl9001469

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

Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy
journal, June 2011

Performance Degradation of High-Brightness Light Emitting Diodes Under DC and Pulsed Bias
journal, June 2008

  • Buso, S.; Spiazzi, G.; Meneghini, M.
  • IEEE Transactions on Device and Materials Reliability, Vol. 8, Issue 2
  • DOI: 10.1109/TDMR.2008.916549

Cooling of photovoltaic cells under concentrated illumination: a critical review
journal, April 2005

Exciton Fate in Semiconductor Nanocrystals at Elevated Temperatures: Hole Trapping Outcompetes Exciton Deactivation
journal, August 2013

  • Rowland, Clare E.; Schaller, Richard D.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 33
  • DOI: 10.1021/jp405616u

Size- and temperature-dependence of exciton lifetimes in CdSe quantum dots
journal, August 2006

The effect of Auger heating on intraband carrier relaxation in semiconductor quantum rods
journal, July 2006

  • Achermann, Marc; Bartko, Andrew P.; Hollingsworth, Jennifer A.
  • Nature Physics, Vol. 2, Issue 8
  • DOI: 10.1038/nphys363

Carrier Cooling in Colloidal Quantum Wells
journal, February 2012

  • Pelton, Matthew; Ithurria, Sandrine; Schaller, Richard D.
  • Nano Letters, Vol. 12, Issue 12
  • DOI: 10.1021/nl302986y

Observation of Size-Dependent Thermalization in CdSe Nanocrystals Using Time-Resolved Photoluminescence Spectroscopy
journal, October 2011

Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation
journal, August 2017

Surface chemistry mediates thermal transport in three-dimensional nanocrystal arrays
journal, March 2013

  • Ong, Wee-Liat; Rupich, Sara M.; Talapin, Dmitri V.
  • Nature Materials, Vol. 12, Issue 5
  • DOI: 10.1038/nmat3596

Electron and hole relaxation pathways in semiconductor quantum dots
journal, November 1999

Intraband relaxation in CdSe quantum dots
journal, July 1999

  • Guyot-Sionnest, Philippe; Shim, Moonsub; Matranga, Chris
  • Physical Review B, Vol. 60, Issue 4
  • DOI: 10.1103/PhysRevB.60.R2181

Unraveling the Structure and Dynamics of Excitons in Semiconductor Quantum Dots
journal, January 2011

  • Kambhampati, Patanjali
  • Accounts of Chemical Research, Vol. 44, Issue 1
  • DOI: 10.1021/ar1000428

Femtosecond 1 P -to- 1 S Electron Relaxation in Strongly Confined Semiconductor Nanocrystals
journal, May 1998

Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots
journal, February 2000

Scaling of multiexciton lifetimes in semiconductor nanocrystals
journal, May 2008

Multicarrier recombination in colloidal quantum dots
journal, September 2007

  • Pandey, Anshu; Guyot-Sionnest, Philippe
  • The Journal of Chemical Physics, Vol. 127, Issue 11
  • DOI: 10.1063/1.2786068

Multiexciton fluorescence from semiconductor nanocrystals
journal, November 2005

Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: Intrinsic limits to the dark-exciton lifetime
journal, April 2003

  • Crooker, S. A.; Barrick, T.; Hollingsworth, J. A.
  • Applied Physics Letters, Vol. 82, Issue 17
  • DOI: 10.1063/1.1570923

Theory of Thermal Relaxation of Electrons in Semiconductors
journal, September 2017

Reverse Non-Equilibrium Molecular Dynamics Demonstrate That Surface Passivation Controls Thermal Transport at Semiconductor–Solvent Interfaces
journal, May 2015

  • Hannah, Daniel C.; Gezelter, J. Daniel; Schaller, Richard D.
  • ACS Nano, Vol. 9, Issue 6
  • DOI: 10.1021/acsnano.5b01724

Identification of parameters through which surface chemistry determines the lifetimes of hot electrons in small Au nanoparticles
journal, February 2013

  • Aruda, Kenneth O.; Tagliazucchi, Mario; Sweeney, Christina M.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 11
  • DOI: 10.1073/pnas.1222327110

Study of Heat Transfer Dynamics from Gold Nanorods to the Environment via Time-Resolved Infrared Spectroscopy
journal, January 2016

Energy Flow from Solute to Solvent Probed by Femtosecond IR Spectroscopy: Malachite Green and Heme Protein Solutions
journal, November 1994

  • Lian, Tianquan; Locke, Bruce; Kholodenko, Yuriy
  • The Journal of Physical Chemistry, Vol. 98, Issue 45
  • DOI: 10.1021/j100096a005

Phonon Spectra of Small Colloidal II-VI Semiconductor Nanocrystals
journal, September 2012

  • Dzhagan, Volodymyr; Valakh, Mykhailo; Mel'nik, Nikolai
  • International Journal of Spectroscopy, Vol. 2012
  • DOI: 10.1155/2012/532385

Size-Dependent Photoconductivity in CdSe Nanoparticles as Measured by Time-Resolved Terahertz Spectroscopy
journal, September 2002

  • Beard, Matthew C.; Turner, Gordon M.; Schmuttenmaer, Charles A.
  • Nano Letters, Vol. 2, Issue 9
  • DOI: 10.1021/nl0256210

Direct Measurement of Lattice Dynamics and Optical Phonon Excitation in Semiconductor Nanocrystals Using Femtosecond Stimulated Raman Spectroscopy
journal, September 2013

Femtosecond stimulated Raman spectroscopy
journal, December 2010

Femtosecond Stimulated Raman Spectroscopy
journal, May 2007

Vibrational Dynamics of a Perylene–Perylenediimide Donor–Acceptor Dyad Probed with Femtosecond Stimulated Raman Spectroscopy
journal, August 2012

  • Brown, Kristen E.; Veldkamp, Brad S.; Co, Dick T.
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 17
  • DOI: 10.1021/jz301107c

Excited-state Raman spectroscopy with and without actinic excitation: S 1 Raman spectra of trans-azobenzene
journal, May 2014

  • Dobryakov, A. L.; Quick, M.; Ioffe, I. N.
  • The Journal of Chemical Physics, Vol. 140, Issue 18
  • DOI: 10.1063/1.4874854

Resonance Femtosecond-Stimulated Raman Spectroscopy without Actinic Excitation Showing Low-Frequency Vibrational Activity in the S 2 State of All-Trans β-Carotene
journal, March 2015

  • Quick, Martin; Dobryakov, Alexander L.; Kovalenko, Sergey A.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 7
  • DOI: 10.1021/acs.jpclett.5b00243

Theory of femtosecond stimulated Raman spectroscopy
journal, August 2004

  • Lee, Soo-Y.; Zhang, Donghui; McCamant, David W.
  • The Journal of Chemical Physics, Vol. 121, Issue 8
  • DOI: 10.1063/1.1777214

Quantum theory of (femtosecond) time-resolved stimulated Raman scattering
journal, April 2008

  • Sun, Zhigang; Lu, J.; Zhang, Dong H.
  • The Journal of Chemical Physics, Vol. 128, Issue 14
  • DOI: 10.1063/1.2888551

Resonance Raman depolarization in CdSe nanocrystals
journal, March 1993

  • Shiang, J. J.; Craig, I. M.; Alivisatos, A. P.
  • Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 26, Issue 1-4
  • DOI: 10.1007/BF01429194

The “Surface Optical” Phonon in CdSe Nanocrystals
journal, March 2014

  • Lin, Chen; Kelley, David F.; Rico, Mikaela
  • ACS Nano, Vol. 8, Issue 4
  • DOI: 10.1021/nn5008513

Optical Studies of Dynamics in Noble Metal Nanostructures
journal, June 2011

Auger Processes in Nanosize Semiconductor Crystals
book, January 2003

Screening of hot-carrier relaxation in highly photoexcited semiconductors
journal, February 1981

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Figure 1 (p. 2)figure
      Figure 2 (p. 3)figure
      Figure 3 (p. 4)figure
      Figure 4 (p. 5)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: