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Title: Heat-driven acoustic phonons in lamellar nanoplatelet assemblies

Journal Article · · Nanoscale
DOI:https://doi.org/10.1039/d0nr00695e· OSTI ID:1632310
ORCiD logo [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [4]
  1. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
  2. Univ. of Chicago, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; Univ. of Chicago, IL (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States)

Colloidal CdSe nanoplatelets, with the electronic structure of quantum wells, self-assemble into lamellar stacks due to large co-facial van der Waals attractions. These lamellar stacks are shown to display coherent acoustic phonons that are detected from oscillatory changes in the absorption spectrum observed in infrared pump, electronic probe measurements. Rather than direct electronic excitation of the nanocrystals using a femtosecond laser, impulsive transfer of heat from the organic ligand shell, excited at C–H stretching vibrational resonances, to the inorganic core of individual nanoplatelets occurs on a time-scale of <100 ps. This heat transfer drives in-phase longitudinal acoustic phonons of the nanoplatelet lamellae, which are accompanied by subtle deformations along the nanoplatelet short axes. The frequencies of the oscillations vary from 0.7 to 2 GHz (3–8 μeV and 0.5–1 ns oscillation period) depending on the thickness of the nanoplatelets—but not their lateral areas—and the temperature of the sample. Temperaturedependence of the acoustic phonon frequency conveys a substantial stiffening of the organic ligand bonds between nanoplatelets with reduced temperature. Overall, these results demonstrate a potential for acoustic modulation of the excitonic structure of nanocrystal assemblies in self-assembled anisotropic semiconductor systems at temperatures at or above 300 K.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357; DMR-142070; DMR-1629383; DMR-1629601
OSTI ID:
1632310
Alternate ID(s):
OSTI ID: 1615690
Journal Information:
Nanoscale, Vol. 12, Issue 17; ISSN 2040-3364
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

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