Probing ligand removal and ordering at quantum dot surfaces using vibrational sum frequency generation spectroscopy

Watson, Brianna R.; Ma, Ying -Zhong; Cahill, John F.; Doughty, Benjamin L.; Calhoun, Tessa R.

doi:10.1016/j.jcis.2018.11.011

Title: Probing ligand removal and ordering at quantum dot surfaces using vibrational sum frequency generation spectroscopy

Journal Article · Wed Nov 07 00:00:00 EST 2018 · Journal of Colloid and Interface Science

DOI:https://doi.org/10.1016/j.jcis.2018.11.011· OSTI ID:1484145

Watson, Brianna R. ^[1];

^[2];

^[2]; Calhoun, Tessa R. ^[1]

Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Controlling nanomaterial interfaces for emerging technologies has driven the need to understand the molecular species located there; however, challenges arise using traditional analytical techniques to directly characterize the molecular structure and local environments of these interfacial species due to their low relative populations. We hypothesized that vibrational sum frequency generation (vSFG) spectroscopy would be uniquely sensitive to the chemical modification of nanoparticle surfaces that is obscured using traditional bulk sensitive methods. Octadecylamine ligands were removed from model CdSe quantum dot surfaces using a common precipitation-resuspension procedure with polar protic and aprotic nonsolvents. Vibrational spectra of the ligands at the surface were collected with vSFG to directly probe the ligand ordering and coverage. Photoluminescence (PL), optical absorption, NMR, and mass spectrometry measurements were conducted for comparison. vSFG was found to be sensitive to subtle changes in ligand disorder over multiple precipitation-resuspension washes, and a limit to the number of ligand molecules removed from the surface and subsequent amount of disorder introduced to their packing was clearly observed. As a result, we also find that nonsolvents do not remain associated with the surface after washing.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1484145

Alternate ID(s):: OSTI ID: 1635949

Journal Information:: Journal of Colloid and Interface Science, Vol. 537, Issue C; ISSN 0021-9797

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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Title: Probing ligand removal and ordering at quantum dot surfaces using vibrational sum frequency generation spectroscopy

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