Light Emission Mechanisms in CuInS2 Quantum
Dots Evaluated by Spectral Electrochemistry
Version 2 2017-12-17, 14:29
Version 1 2017-09-25, 12:05
Posted on 2017-12-17 - 14:29
Luminescent
CuInS2 (CIS) quantum dots (QDs) exhibit
highly efficient intragap emission and long, hundreds-of-nanoseconds
radiative lifetimes. These spectral properties, distinct from structurally
similar II–VI QDs, can be explained by the involvement of intragap
defect states containing a localized hole capable of coupling with
a conduction band electron for a radiative transition. However, the
absolute energies of the intragap and band-edge states, the structure
of the emissive defect(s), and the role and origin of nonemissive
decay channels still remain poorly understood. Here, we address these
questions by applying methods of spectral electrochemistry. Cyclic
voltammetry measurements reveal a well-defined intragap state whose
redox potential is close to that of the Cux defect state (where x = 1+ or 2+). The energy offset
of this state from the valence band accounts well for the apparent
photoluminescence Stokes shift observed in optical spectra. These
results provide direct evidence that Cu-related defects serve as emission
centers responsible for strong intragap emission from CIS QDs. We
then use in situ spectroelectrochemistry to reveal
two distinct emission pathways based on the differing oxidation states
of Cu defects, which can be controlled by altering QD stoichiometry
(1+ for stoichiometric QDs and 2+ for Cu-deficient QDs).
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Fuhr, Addis
S.; Yun, Hyeong Jin; Makarov, Nikolay S.; Li, Hongbo; McDaniel, Hunter; Klimov, Victor I. (2017). Light Emission Mechanisms in CuInS2 Quantum
Dots Evaluated by Spectral Electrochemistry. ACS Publications. Collection. https://doi.org/10.1021/acsphotonics.7b00560
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AUTHORS (6)
AF
Addis
S. Fuhr
HY
Hyeong Jin Yun
NM
Nikolay S. Makarov
HL
Hongbo Li
HM
Hunter McDaniel
VK
Victor I. Klimov
KEYWORDS
nonemissive decay channelsCuInS 2 Quantum Dots Evaluatedhundreds-of-nanoseconds radiative lifetimesintragap defect statesCyclic voltammetry measurementsintragap emissionconduction band electronlight Emission Mechanismsphotoluminescence Stokes shiftvalence band accountsCISSpectral Electrochemistry Luminescent CuInS 2Cu x defect stateIIQD