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 · 28 July 2017 · Nano Letters

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

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

^[2]; Zhang, Xiaoyi ^[2]; Wagner, Michael J. ^[1]; Hayes, Dugan ^[2]; Chang, Angela Y. ^[1]; Rowland, Clare E. ^[1]; Lethiec, Clotilde M. ^[1];

^[1]; Chen, Lin X. ^[3];

^[3]

Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Lemont, IL (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 relate heating and peak amplitude reduction confers lattice disordering. 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. Here, 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.

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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, Vol. 17, Issue 9; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 22 works

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Related Subjects

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