Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation

Kirschner, Matthew S.; Hannah, Daniel C.; Diroll, Benjamin T.; Zhang, Xiaoyi; Wagner, Michael J.; Hayes, Dugan; Chang, Angela Y.; Rowland, Clare E.; Lethiec, Clotilde M.; Schatz, George C.; Chen, Lin X.; Schaller, Richard D.

doi:10.1021/acs.nanolett.7b01705

Title: Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation

Journal Article · Fri Jul 28 00:00:00 EDT 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.7b01705· OSTI ID:1374084

Kirschner, Matthew S. ^[1]; Hannah, Daniel C. ^[1];

; Zhang, Xiaoyi; Wagner, Michael J. ^[1]; Hayes, Dugan; Chang, Angela Y. ^[1]; Rowland, Clare E. ^[1]; Lethiec, Clotilde M. ^[1];

^[1]; Chen, Lin X. ^[1];

^[1]

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States

Ultrafast optical pump, X-ray diffraction probe experiments were performed on CdSe nanocrystal (NC) colloidal dispersions as functions of particle size, polytype, and pump fluence. Bragg peak shifts related to heating and peak amplitude reduction associated with lattice disordering are observed. For smaller NCs, melting initiates upon absorption of as few as ~15 electron–hole pair excitations per NC on average (0.89 excitations/nm3 for a 1.5 nm radius) with roughly the same excitation density inducing melting for all examined NCs. Diffraction intensity recovery kinetics, attributable to recrystallization, occur over hundreds of picoseconds with slower recoveries for larger particles. Zincblende and wurtzite NCs revert to initial structures following intense photoexcitation suggesting melting occurs primarily at the surface, as supported by simulations. Electronic structure calculations relate significant band gap narrowing with decreased crystallinity. These findings reflect the need to consider the physical stability of nanomaterials and related electronic impacts in high intensity excitation applications such as lasing and solid-state lighting.

View Journal Article

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1374084

Alternate ID(s):: OSTI ID: 1405316; OSTI ID: 1414909

Journal Information:: Nano Letters, Journal Name: Nano Letters; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 22 works

Citation information provided by
Web of Science

References (44)

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
Ultrafast heating of silicon on sapphire by femtosecond optical pulses Downer, M. C.; Shank, C. V. Physical Review Letters, Vol. 56, Issue 7 https://doi.org/10.1103/PhysRevLett.56.761	journal	February 1986
Synthesis of CdSe and CdTe Nanocrystals without Precursor Injection Yang, Yongan Andrew; Wu, Huimeng; Williams, Kathryn R. Angewandte Chemie, Vol. 117, Issue 41 https://doi.org/10.1002/ange.200502279	journal	October 2005
Nucleation of tetrahedral solids: A molecular dynamics study of supercooled liquid silicon Li, Tianshu; Donadio, Davide; Galli, Giulia The Journal of Chemical Physics, Vol. 131, Issue 22 https://doi.org/10.1063/1.3268346	journal	December 2009
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
Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals Robel, István; Gresback, Ryan; Kortshagen, Uwe Physical Review Letters, Vol. 102, Issue 17, Article No. 177404 https://doi.org/10.1103/PhysRevLett.102.177404	journal	May 2009
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
Canonical sampling through velocity rescaling Bussi, Giovanni; Donadio, Davide; Parrinello, Michele The Journal of Chemical Physics, Vol. 126, Issue 1 https://doi.org/10.1063/1.2408420	journal	January 2007
Real-Time Visualization of Nanocrystal Solid–Solid Transformation Pathways Wittenberg, Joshua S.; Miller, Timothy A.; Szilagyi, Erzsi Nano Letters, Vol. 14, Issue 4 https://doi.org/10.1021/nl500043c	journal	March 2014
Controlling the Surface of Semiconductor Nanocrystals for Efficient Light Emission from Single Excitons to Multiexcitons Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M. The Journal of Physical Chemistry C, Vol. 119, Issue 28 https://doi.org/10.1021/acs.jpcc.5b03853	journal	June 2015
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
Visualization of nanocrystal breathing modes at extreme strains Szilagyi, Erzsi; Wittenberg, Joshua S.; Miller, Timothy A. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7577	journal	March 2015
An interatomic pair potential for cadmium selenide Rabani, Eran The Journal of Chemical Physics, Vol. 116, Issue 1 https://doi.org/10.1063/1.1424321	journal	January 2002
Size dependent, state-resolved studies of exciton-phonon couplings in strongly confined semiconductor quantum dots Sagar, D. M.; Cooney, Ryan R.; Sewall, Samuel L. Physical Review B, Vol. 77, Issue 23 https://doi.org/10.1103/PhysRevB.77.235321	journal	June 2008
Melting in Semiconductor Nanocrystals Goldstein, A. N.; Echer, C. M.; Alivisatos, A. P. Science, Vol. 256, Issue 5062, p. 1425-1427 https://doi.org/10.1126/science.256.5062.1425	journal	June 1992
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Suppressed Auger Recombination in “Giant” Nanocrystals Boosts Optical Gain Performance García-Santamaría, Florencio; Chen, Yongfen; Vela, Javier Nano Letters, Vol. 9, Issue 10 https://doi.org/10.1021/nl901681d	journal	October 2009
Perspectives on the Physical Chemistry of Semiconductor Nanocrystals Alivisatos, A. P. The Journal of Physical Chemistry, Vol. 100, Issue 31 https://doi.org/10.1021/jp9535506	journal	January 1996
S PECTROSCOPY AND H OT E LECTRON R ELAXATION D YNAMICS IN S EMICONDUCTOR Q UANTUM W ELLS AND Q UANTUM D OTS Nozik, Arthur J. Annual Review of Physical Chemistry, Vol. 52, Issue 1 https://doi.org/10.1146/annurev.physchem.52.1.193	journal	October 2001
Nonhomogeneous surface premelting of Au nanoparticles Wang, Ningyu; Rokhlin, S. I.; Farson, D. F. Nanotechnology, Vol. 19, Issue 41 https://doi.org/10.1088/0957-4484/19/41/415701	journal	September 2008
Imaging transient melting of a nanocrystal using an X-ray laser Clark, Jesse N.; Beitra, Loren; Xiong, Gang Proceedings of the National Academy of Sciences, Vol. 112, Issue 24 https://doi.org/10.1073/pnas.1417678112	journal	June 2015
Microsecond-sustained lasing from colloidal quantum dot solids Adachi, Michael M.; Fan, Fengjia; Sellan, Daniel P. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9694	journal	October 2015
Colloidal quantum-dot light-emitting diodes with metal-oxide charge transport layers Caruge, J. M.; Halpert, J. E.; Wood, V. Nature Photonics, Vol. 2, Issue 4 https://doi.org/10.1038/nphoton.2008.34	journal	March 2008
Mechanisms for Photogeneration and Recombination of Multiexcitons in Semiconductor Nanocrystals: Implications for Lasing and Solar Energy Conversion Klimov, Victor I. The Journal of Physical Chemistry B, Vol. 110, Issue 34 https://doi.org/10.1021/jp0615959	journal	August 2006
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
Structural, bonding, dynamical, and electronic properties of liquid silicon: An ab initio molecular-dynamics study Štich, I.; Car, R.; Parrinello, M. Physical Review B, Vol. 44, Issue 9 https://doi.org/10.1103/PhysRevB.44.4262	journal	September 1991
Synthesis of High Quality Zinc Blende CdSe Nanocrystals Mohamed, Mona B.; Tonti, Dino; Al-Salman, Awos The Journal of Physical Chemistry B, Vol. 109, Issue 21 https://doi.org/10.1021/jp051123e	journal	June 2005
Stable and Low-Threshold Optical Gain in CdSe/CdS Quantum Dots: An All-Colloidal Frequency Up-Converted Laser Guzelturk, Burak; Kelestemur, Yusuf; Gungor, Kivanc Advanced Materials, Vol. 27, Issue 17 https://doi.org/10.1002/adma.201500418	journal	March 2015
Interband and Intraband Optical Studies of PbSe Colloidal Quantum Dots Wehrenberg, Brian L.; Wang, Congjun; Guyot-Sionnest, Philippe The Journal of Physical Chemistry B, Vol. 106, Issue 41 https://doi.org/10.1021/jp021187e	journal	October 2002
Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach Carbone, Luigi; Nobile, Concetta; De Giorgi, Milena Nano Letters, Vol. 7, Issue 10 https://doi.org/10.1021/nl0717661	journal	October 2007
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
Electronic wave functions in semiconductor clusters: experiment and theory Brus, Louis The Journal of Physical Chemistry, Vol. 90, Issue 12, p. 2555-2560 https://doi.org/10.1021/j100403a003	journal	June 1986
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
Particle-Level Engineering of Thermal Conductivity in Matrix-Embedded Semiconductor Nanocrystals Hannah, Daniel C.; Ithurria, Sandrine; Krylova, Galyna Nano Letters, Vol. 12, Issue 11 https://doi.org/10.1021/nl303109r	journal	October 2012
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
‘Giant’ CdSe/CdS Core/Shell Nanocrystal Quantum Dots As Efficient Electroluminescent Materials: Strong Influence of Shell Thickness on Light-Emitting Diode Performance Pal, Bhola N.; Ghosh, Yagnaseni; Brovelli, Sergio Nano Letters, Vol. 12, Issue 1 https://doi.org/10.1021/nl203620f	journal	December 2011
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
Interplay between Optical Gain and Photoinduced Absorption in CdSe Nanocrystals Malko, A. V.; Mikhailovsky, A. A.; Petruska, M. A. The Journal of Physical Chemistry B, Vol. 108, Issue 17 https://doi.org/10.1021/jp037699q	journal	April 2004
Trion Decay in Colloidal Quantum Dots Jha, Praket P.; Guyot-Sionnest, Philippe ACS Nano, Vol. 3, Issue 4 https://doi.org/10.1021/nn9001177	journal	March 2009
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
Ultrafast lattice dynamics in lead selenide quantum dot induced by laser excitation Wang, Xuan; Rahmani, Hamidreza; Zhou, Jun Applied Physics Letters, Vol. 109, Issue 15 https://doi.org/10.1063/1.4964269	journal	October 2016
The CdS-MnS and CdSe-MnSe Phase Diagrams Cook, William R. Journal of the American Ceramic Society, Vol. 51, Issue 9 https://doi.org/10.1111/j.1151-2916.1968.tb15678.x	journal	September 1968
Melting and critical superheating Belonoshko, A. B.; Skorodumova, N. V.; Rosengren, A. Physical Review B, Vol. 73, Issue 1 https://doi.org/10.1103/PhysRevB.73.012201	journal	January 2006

Figures / Tables (4)

Similar Records

Optical Signatures of Transiently Disordered Semiconductor Nanocrystals

Journal Article · Thu Sep 13 00:00:00 EDT 2018 · ACS Nano · OSTI ID:1374084

Kirschner, Matthew S.; Diroll, Benjamin T.; Brumberg, Alexandra; +4 more

Advanced Branching Control and Characterization of Inorganic Semiconducting Nanocrystals

Thesis/Dissertation · Mon Jan 01 00:00:00 EST 2007 · OSTI ID:1374084

Hughes, Steven Michael

Anisotropic Transient Disordering of Colloidal, Two-Dimensional CdSe Nanoplatelets upon Optical Excitation

Journal Article · Tue Jan 19 00:00:00 EST 2021 · Nano Letters · OSTI ID:1374084

Brumberg, Alexandra; Kirschner, Matthew S.; Diroll, Benjamin T.; +18 more

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
melting
molecular dynamics
multiexciton
Nanocrystals
phonon
transient diffraction

Title: Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation

Citation Formats

References (44)

Figures / Tables (4)

Similar Records

Related Subjects