CsPbX3 (X = Cl, Br, I) Perovskite Nanocrystals: Beyond CdSe Quantum Dots
Angshuman Nag a, Pankaj Mandal a, Yettapu Gurivi Reddy a, Ganesh B. Markad a, Vikash Kumar Ravi a, Abhishek Swarnkar a, Ramya Chulliyil b, Arindam Chowdhury b
a Indian Institute of Science Education and Research (IISER), Pune, IN, Pune, Maharastra 411008, India, Pune, India
b Department of Chemistry, Indian Institute of Technology Bombay, Mumbai 400076, India
Materials for Sustainable Development Conference (MATSUS)
Proceedings of September Meeting 2016 (NFM16)
Berlin, Germany, 2016 September 5th - 13th
Organizers: Marin Alexe, Enrique Cánovas, Celso de Mello Donega, Ivan Infante, Thomas Kirchartz, Maksym Kovalenko, Federico Rosei, Lukas Schmidt-Mende, Laurens Siebbeles, Peter Strasser, Teodor K Todorov, Roel van de Krol and Ulrike Woggon
Oral, Angshuman Nag, presentation 136
Publication date: 14th June 2016

Colloidal quantum dots (cQDs), such as those based on CdSe are widely known for their interesting electronic, optical andoptoelectronic properties. In the beginning of 2015, Protesescu et al1 reported CsPbX3 perovskite nanocrystals with ~90% photoluminescence efficiency, suggesting that these perovskite nanocrystals have the possibility to perform better as an optoelectronic material compared to traditional cQDs like CdSe based ones. In this presentation, I will discuss our recent results showing (i) unique advantages in both ensemble and single-nanocrystal photluminescence of colloidal CsPbBr3 nanocrystals compared to traditional CdSe cQDs,2 (ii) the influence of halide composition on valence and conduction band edges, (iii) ultrafast terahertz (THz) spectroscopy results signifying surface defects do not trap charge carriers.

Colloidal CsPbBr3 nanocrystals (11 nm) exhibit ~90% PL quantum yield with narrow (FWHM = 86 meV) spectral width. FWHM of a single-nanocrystal and ensemble are almost identical, ruling out the problem of size-distribution in photoluminescence broadening, along with batch-to-batch reproducibility of nanocrystals exhibiting photoluminescence peak within ±1 nm. Tuning of luminescence color across the visible region can be achieved by controlling halide composition, and our cyclic voltammetry results show that change in valence band maximum with halide composition is mainly responsible for the change in optical gap. However, conduction band minimum (CBM) also shift (though to a smaller extent) systematically with halide composition, suggesting contribution of X np orbital to the CBM is not negligible. Finally, CsPbBr3 nanocrystals exhibit very high (~ 5000 cm2V-1S-1) THz carrier mobility within a nanocrystal suggesting minimal influence of the surface defects as mid-gap deep trap states.

Reference:

1. Protesescu, L.; Yakunin, S.; Bodnarchuk, M. I.; Krieg, F.; Caputo, R.; Hendon, C. H.; Yang, R. X.; Walsh, A.; Kovalenko, M. V. Nano Lett. 2015, 15, 3692.

2. Swarnkar, A; Chulliyil, R.; Ravi, V. K.; Irfanullah, M.; Chowdhury, A.; Nag A. Angew. Chem. Int. Ed. 2015, 53, 15424.



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