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Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell.

Karki, Khadga Jung LU ; Widom, Julia R; Seibt, Joachim LU ; Moody, Ian; Lonergan, Mark C; Pullerits, Tönu LU and Marcus, Andrew H (2014) In Nature Communications 5.
Abstract
Recently there has been growing interest in the role of coherence in electronic dynamics. Coherent multidimensional spectroscopy has been used to reveal coherent phenomena in numerous material systems. Here we utilize a recent implementation of coherent multidimensional spectroscopy-two-dimensional photocurrent spectroscopy-in which we detect the photocurrent from a PbS quantum dot photocell resulting from its interactions with a sequence of four ultrafast laser pulses. We observe sub-picosecond evolution of two-dimensional spectra consistent with multiple exciton generation. Moreover, a comparison with two-dimensional fluorescence spectra of the quantum dots demonstrates the potential of two-dimensional photocurrent spectroscopy to... (More)
Recently there has been growing interest in the role of coherence in electronic dynamics. Coherent multidimensional spectroscopy has been used to reveal coherent phenomena in numerous material systems. Here we utilize a recent implementation of coherent multidimensional spectroscopy-two-dimensional photocurrent spectroscopy-in which we detect the photocurrent from a PbS quantum dot photocell resulting from its interactions with a sequence of four ultrafast laser pulses. We observe sub-picosecond evolution of two-dimensional spectra consistent with multiple exciton generation. Moreover, a comparison with two-dimensional fluorescence spectra of the quantum dots demonstrates the potential of two-dimensional photocurrent spectroscopy to elucidate detailed origins of photocurrent generating electronic state coherence pathways. Since the measurement is based on detecting the photocell current in situ, the method is well suited to study the fundamental ultrafast processes that affect the function of the device. This opens new avenues to investigate and implement coherent optimization strategies directly within devices. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
5
publisher
Nature Publishing Group
external identifiers
  • pmid:25519819
  • wos:000347176200002
ISSN
2041-1723
DOI
10.1038/ncomms6869
language
English
LU publication?
yes
id
64101560-58f8-4552-bb96-2f55f1572da8 (old id 4907992)
date added to LUP
2015-01-13 17:06:32
date last changed
2016-09-20 04:32:34
@article{64101560-58f8-4552-bb96-2f55f1572da8,
  abstract     = {Recently there has been growing interest in the role of coherence in electronic dynamics. Coherent multidimensional spectroscopy has been used to reveal coherent phenomena in numerous material systems. Here we utilize a recent implementation of coherent multidimensional spectroscopy-two-dimensional photocurrent spectroscopy-in which we detect the photocurrent from a PbS quantum dot photocell resulting from its interactions with a sequence of four ultrafast laser pulses. We observe sub-picosecond evolution of two-dimensional spectra consistent with multiple exciton generation. Moreover, a comparison with two-dimensional fluorescence spectra of the quantum dots demonstrates the potential of two-dimensional photocurrent spectroscopy to elucidate detailed origins of photocurrent generating electronic state coherence pathways. Since the measurement is based on detecting the photocell current in situ, the method is well suited to study the fundamental ultrafast processes that affect the function of the device. This opens new avenues to investigate and implement coherent optimization strategies directly within devices.},
  articleno    = {5869},
  author       = {Karki, Khadga Jung and Widom, Julia R and Seibt, Joachim and Moody, Ian and Lonergan, Mark C and Pullerits, Tönu and Marcus, Andrew H},
  issn         = {2041-1723},
  language     = {eng},
  publisher    = {Nature Publishing Group},
  series       = {Nature Communications},
  title        = {Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell.},
  url          = {http://dx.doi.org/10.1038/ncomms6869},
  volume       = {5},
  year         = {2014},
}