Ultrafast Exciton Fine Structure Relaxation Dynamics in Lead Chalcogenide Nanocrystals

Johnson, Justin C.; Gerth, Kathrine A.; Song, Qing; Murphy, James E.; Nozik, Arthur J.; Scholes, Gregory D.

doi:10.1021/nl080126a

Ultrafast Exciton Fine Structure Relaxation Dynamics in Lead Chalcogenide Nanocrystals

Journal Article · Tue Jan 01 04:00:00 EST 2008 · Nano Letters

DOI:https://doi.org/10.1021/nl080126a· OSTI ID:950129

; Gerth, Kathrine A.; Song, Qing; Murphy, James E.; ; Scholes, Gregory D.

The rates of fine structure relaxation in PbS, PbSe, and PbTe nanocrystals were measured on a femtosecond time scale as a function of temperature with no applied magnetic field by cross-polarized transient grating spectroscopy (CPTG) and circularly polarized pump-probe spectroscopy. The relaxation rates among exciton fine structure states follow trends with nanocrystal composition and size that are consistent with the expected influence of material dependent spin-orbit coupling, confinement enhanced electron-hole exchange interaction, and splitting between L valleys that are degenerate in the bulk. The size dependence of the fine structure relaxation rate is considerably different from what is observed for small CdSe nanocrystals, which appears to result from the unique material properties of the highly confined lead chalcogenide quantum dots. Modeling and qualitative considerations lead to conclusions about the fine structure of the lowest exciton absorption band, which has a potentially significant bearing on photophysical processes that make these materials attractive for practical purposes.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science, Office of Basic Energy Sciences

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 950129

Report Number(s):: NREL/JA-270-42994; MainId:47462; UUID:0e4fc126-d8d4-e411-b769-d89d67132a6d; MainAdminId:29554

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 5 Vol. 8

Country of Publication:: United States

Language:: English

References (28)

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
Spintronics: Fundamentals and applications Žutić, Igor; Fabian, Jaroslav; Das Sarma, S. Reviews of Modern Physics, Vol. 76, Issue 2 https://doi.org/10.1103/RevModPhys.76.323	journal	April 2004
The grating decomposition method: A new approach for understanding polarization‐selective transient grating experiments. I. Theory Fourkas, John T.; Trebino, Rick; Fayer, M. D. The Journal of Chemical Physics, Vol. 97, Issue 1 https://doi.org/10.1063/1.463565	journal	July 1992
Direct Pseudopotential Calculation of Exciton Coulomb and Exchange Energies in Semiconductor Quantum Dots Franceschetti, Alberto; Zunger, Alex Physical Review Letters, Vol. 78, Issue 5 https://doi.org/10.1103/PhysRevLett.78.915	journal	February 1997
Colloidal PbS Nanocrystals with Size-Tunable Near-Infrared Emission: Observation of Post-Synthesis Self-Narrowing of the Particle Size Distribution Hines, M. A.; Scholes, G. D. Advanced Materials, Vol. 15, Issue 21, p. 1844-1849 https://doi.org/10.1002/adma.200305395	journal	November 2003
Chromophore-Solvent Dynamics Fleming, Graham R.; Cho, Minhaeng Annual Review of Physical Chemistry, Vol. 47, Issue 1 https://doi.org/10.1146/annurev.physchem.47.1.109	journal	October 1996
Short-range versus long-range electron-hole exchange interactions in semiconductor quantum dots Franceschetti, A.; Wang, L. W.; Fu, H. Physical Review B, Vol. 58, Issue 20 https://doi.org/10.1103/PhysRevB.58.R13367	journal	November 1998
The Excitonic Exchange Splitting and Radiative Lifetime in PbSe Quantum Dots An, J. M.; Franceschetti, A.; Zunger, A. Nano Letters, Vol. 7, Issue 7 https://doi.org/10.1021/nl071219f	journal	July 2007
Semiconductor Spintronics and Quantum Computation Awschalom, D. D.; Loss, D.; Samarth, N. NanoScience and Technology https://doi.org/10.1007/978-3-662-05003-3	book	January 2002
The Peculiar Electronic Structure of PbSe Quantum Dots An, J. M.; Franceschetti, A.; Dudiy, S. V. Nano Letters, Vol. 6, Issue 12 https://doi.org/10.1021/nl061684x	journal	December 2006
Electronic and structural anomalies in lead chalcogenides Wei, Su-Huai; Zunger, Alex Physical Review B, Vol. 55, Issue 20 https://doi.org/10.1103/PhysRevB.55.13605	journal	May 1997
Dynamics within the Exciton Fine Structure of Colloidal CdSe Quantum Dots Huxter, Vanessa M.; Kovalevskij, Vitalij; Scholes, Gregory D. The Journal of Physical Chemistry B, Vol. 109, Issue 43 https://doi.org/10.1021/jp0546406	journal	October 2005
Excitons in CdSe quantum dots Laheld, U. E. H.; Einevoll, G. T. Physical Review B, Vol. 55, Issue 8 https://doi.org/10.1103/PhysRevB.55.5184	journal	February 1997
Ultrafast Solvation Dynamics Explored by Femtosecond Photon echo Spectroscopies de Boeij, Wim P.; Pshenichnikov, Maxim S.; Wiersma, Douwe A. Annual Review of Physical Chemistry, Vol. 49, Issue 1 https://doi.org/10.1146/annurev.physchem.49.1.99	journal	October 1998
Selection rules for probing biexcitons and electron spin transitions in isotropic quantum dot ensembles Scholes, Gregory D. The Journal of Chemical Physics, Vol. 121, Issue 20 https://doi.org/10.1063/1.1808414	journal	November 2004
Band-edge exciton in quantum dots of semiconductors with a degenerate valence band: Dark and bright exciton states Efros, Al. L.; Rosen, M.; Kuno, M. Physical Review B, Vol. 54, Issue 7 https://doi.org/10.1103/PhysRevB.54.4843	journal	August 1996
Effect of band anisotropy on electronic structure of PbS, PbSe, and PbTe quantum dots Tudury, G. E.; Marquezini, M. V.; Ferreira, L. G. Physical Review B, Vol. 62, Issue 11 https://doi.org/10.1103/PhysRevB.62.7357	journal	September 2000
Nanocrystal Shape and the Mechanism of Exciton Spin Relaxation Scholes, Gregory D.; Kim, Jeongho; Wong, Cathy Y. Nano Letters, Vol. 6, Issue 8 https://doi.org/10.1021/nl061414e	journal	July 2006
Confinement effects in PbSe quantum wells and nanocrystals Allan, G.; Delerue, C. Physical Review B, Vol. 70, Issue 24 https://doi.org/10.1103/PhysRevB.70.245321	journal	December 2004
Magnetoexcitons in anisotropic semiconductors Zhang, Yong; Mascarenhas, A.; Jones, E. D. Journal of Applied Physics, Vol. 83, Issue 1 https://doi.org/10.1063/1.366659	journal	January 1998
Lead Salt Quantum Dots: the Limit of Strong Quantum Confinement Wise, Frank W. Accounts of Chemical Research, Vol. 33, Issue 11 https://doi.org/10.1021/ar970220q	journal	November 2000
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
Energy Bands of PbTe, PbSe, and PbS Lin, Pay June; Kleinman, Leonard Physical Review, Vol. 142, Issue 2 https://doi.org/10.1103/PhysRev.142.478	journal	February 1966
Exciton spin relaxation in quantum dots measured using ultrafast transient polarization grating spectroscopy Scholes, Gregory D.; Kim, Jeongho; Wong, Cathy Y. Physical Review B, Vol. 73, Issue 19 https://doi.org/10.1103/PhysRevB.73.195325	journal	May 2006
Mechanism and Origin of Exciton Spin Relaxation in CdSe Nanorods Kim, Jeongho; Wong, Cathy Y.; Nair, P. Sreekumari The Journal of Physical Chemistry B, Vol. 110, Issue 50 https://doi.org/10.1021/jp0644816	journal	October 2006
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
Electronic structure and optical properties of PbS and PbSe quantum dots Kang, Inuk; Wise, Frank W. Journal of the Optical Society of America B, Vol. 14, Issue 7 https://doi.org/10.1364/JOSAB.14.001632	journal	January 1997
Highly Efficient Multiple Exciton Generation in Colloidal PbSe and PbS Quantum Dots Ellingson, Randy J.; Beard, Matthew C.; Johnson, Justin C. Nano Letters, Vol. 5, Issue 5, p. 865-871 https://doi.org/10.1021/nl0502672	journal	May 2005

Similar Records

Shape Dependence of Band-Edge Exciton Fine Structure in CdSe Nanocrystals

Journal Article · Sun Dec 31 23:00:00 EST 2006 · Nano Letters · OSTI ID:982936

Revealing the Exciton Fine Structure of PbSe Nanocrystal Quantum Dots Using Optical Spectroscopy in High Magnetic Fields

Journal Article · Wed Aug 04 00:00:00 EDT 2010 · Phys. Rev. Lett. · OSTI ID:1065041

Surface relaxation in CdSe nanocrystals

Journal Article · Tue Jun 01 00:00:00 EDT 1999 · Journal of Chemical Physics · OSTI ID:341365

Related Subjects

ABSORPTION
BEARINGS
CHALCOGENIDES
CONFINEMENT
EXCHANGE INTERACTIONS
EXCITONS
FINE STRUCTURE
MAGNETIC FIELDS
NANOSCIENCE AND NANOTECHNOLOGY
QUANTUM DOTS
RELAXATION
SIMULATION
SPECTROSCOPY
TRANSIENTS
absorption
bearings
chalcogenides
confinement
exchange interactions
excitons
fine structure
magnetic fields
quantum dots
relaxation
simulation
spectroscopy
transients

Ultrafast Exciton Fine Structure Relaxation Dynamics in Lead Chalcogenide Nanocrystals

Citation Formats

References (28)

Similar Records

Related Subjects