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

Khadga J. Karki, Julia R. Widom, Joachim Seibt, Ian Moody, Mark C. Lonergan (), Tõnu Pullerits () and Andrew H. Marcus ()
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Khadga J. Karki: Lund University
Julia R. Widom: University of Oregon
Joachim Seibt: Lund University
Ian Moody: University of Oregon
Mark C. Lonergan: University of Oregon
Tõnu Pullerits: Lund University
Andrew H. Marcus: University of Oregon

Nature Communications, 2014, vol. 5, issue 1, 1-7

Abstract: 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.

Date: 2014
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms6869

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DOI: 10.1038/ncomms6869

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