Colloidal Two-Dimensional PbS Nanosheets and Ultrathin PbS Nanoplatelets – High Mobility vs. Photoluminescence Properties
Jannika Lauth a, Michele Failla b, Francisco Manteiga Vázquez b, Qianli Yu b, Eugen Klein c, Ryan Crisp b, Christian Klinke c, Sachin Kinge d, Arjan Houtepen b, Laurens Siebbeles b
a Carl von Ossietzky University Oldenburg, Carl von Ossietzky Starß2 9-11, Oldenburg, 26129, Germany
b Delft University of Technology, The Netherlands, Julianalaan, 136, Delft, Netherlands
c University of Hamburg, Institute of Physical Chemistry, Hamburg, Germany
d Materials Research & Development, Toyota Motor Europe, Zaventem, Belgium
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2018 (NFM18)
S6 Solution-based Two-dimensional Nanomaterials Sol2D
Torremolinos, Spain, 2018 October 22nd - 26th
Organizers: Christophe Delerue, Sandrine Ithurria and Christian Klinke
Oral, Jannika Lauth, presentation 111
DOI: https://doi.org/10.29363/nanoge.nfm.2018.111
Publication date: 6th July 2018

Solution-processed two-dimensional (2D) semiconductors with tunable band gaps represent highly promising materials for next generation ultrathin electronics. Their dimensionality-dependent optoelectronic properties differ significantly from their zero-, one- and three-dimensional counterparts and can be tuned by colloidal chemistry methods for controlling the structures’ thickness.

We use optical pump-terahertz probe (OPTHzP) spectroscopy as a non-contact method to determine the thickness-dependent transient charge carrier mobility in 2D PbS nanosheets of different thickness (4 – 16 nm) and find high values ranging from 231 cm2/Vs in the thinnest, 4 nm thick sheets, up to 472 cm2/Vs and 427 cm2/Vs in 6 nm and 16 nm thick PbS nanosheets, respectively. Furthermore, we model the frequency dependent charge carrier mobility of 2D PbS nanosheets with a Drude-Smith behavior and reveal a growing contribution of photoexcited excitons in thinner PbS nanosheets due to their increased exciton binding energy.[1] 

We find that by carefully controlling the reaction kinetics, the thickness of colloidal 2D PbS layers can be reduced to < 2 nm to the formation of ultrathin PbS nanoplatelets. Ultrathin 2D PbS layers are particularly interesting due to their increasing carrier multiplication (CM) efficiency with decreasing nanosheet/nanoplatelet thickness.[2,3] We show that in thicker PbS nanosheets, free and mobile charges are generated under photoexcitation, whereas in ultrathin PbS nanoplatelets bound excitons are formed. A photoluminescence quantum yield of up to 20 % is obtained by surface passivation of the significantly blue-shifted PbS nanoplatelets (Abs: 683 nm, 1.8 eV, PL: 705 nm, 1.75 eV) and underpins their potential for NIR light-emitting applications.[4] Our work emphasizes the excellent usability of colloidal chemistry and spectroscopy methods for producing 2D tailor-made band gap materials for high mobility AND light emitting optoelectronics.

[1] Lauth, J., Failla, M, Klein, E., Klinke, C., Kinge, S., Siebbeles, L. D. A., submitted 2018.

[2] Bielewicz, T.; Dogan, S.; Klinke, C., Small 2015,11, 826-833.

[3] Aerts, M.; Bielewicz, T.; Klinke, C.; Grozema, F. C.; Houtepen, A. J.; Schins, J. M.; Siebbeles, L. D. A., Nat. Commun. 2014,5, 3789.

[4] Manteiga Vazquéz, F., Yu, Q., Crisp, R., Kinge, S., Houtepen, A. J., Siebbeles, L. D. A., Lauth, J., in preparation.

 

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