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Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy

Journal Article · · ACS Nano
 [1];  [2];  [1];  [3];  [1];  [2];  [4];  [1];  [2];  [4];  [5];  [1]
  1. Univ. of Illinois, Chicago, IL (United States). Department of Chemistry
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  3. Northwestern Univ., Evanston, IL (United States). Department of Chemistry
  4. Univ. of Illinois, Chicago, IL (United States). Department of Physics
  5. Northwestern Univ., Evanston, IL (United States). Department of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Center of Nanoscale Materials
+ Show Author Affiliations

Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report the results of time-resolved X-ray absorption studies on copper-doped cadmium sulfide nanoparticles that provide an explicit description of the electronic dynamics of the dopants. The interaction of a dopant ion and an excess charge carrier is unambiguously observed via monitoring the oxidation state. The experimental data combined with DFT calculations demonstrate that dopant bonding to the host matrix is modulated by its interaction with charge carriers. Additionally, the transient photoluminescence and the kinetics of dopant oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1417192
Journal Information:
ACS Nano, Journal Name: ACS Nano Journal Issue: 10 Vol. 11; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
cadmium sulfide
doping
nanoparticle
quantum dot
semiconductor
x-ray absorption