Nano- and single-crystals of lead halide perovskites: from bright light emission to hard radiation detection

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Event details

Date 01.12.2016
Hour 16:3017:30
Speaker Prof. Dr. Maksym Kovalenko
ETH Zurich
Department of Chemistry and Applied Biosciences
Location
Category Conferences - Seminars
 Chemically synthesized inorganic nanocrystals (NCs) are considered to be promising building blocks for a broad spectrum of applications including electronic, thermoelectric, and photovoltaic devices. We have synthesized monodisperse colloidal nanocubes (4-15 nm edge lengths) of fully inorganic cesium lead halide perovskites (CsPbX3, X=Cl, Br, and I or mixed halide systems Cl/Br and Br/I) using inexpensive commercial precursors [1]. Their bandgap energies and emission spectra are readily tunable over the entire visible spectral region of 410-700 nm. The photoluminescence of CsPbX3 NCs is characterized by narrow emission line-widths of 12-42 nm, wide color gamut covering up to 140% of the NTSC color standard, high quantum yields of up to 90% and radiative lifetimes in the range of 4-29 ns. Post-synthestic chemical transformations of colloidal NCs, such as ion-exchange reactions, provide an avenue to compositional fine tuning or to otherwise inaccessible materials and morphologies [2]. Identical synthesis methodology is perfectly suited also for hybrid perovskite nanocrystals of CH3NH3PbX3 [3] and CH(NH2)2PbX3 [4].
 
We also present low-threshold amplified spontaneous emission and lasing from CsPbX3 NCs [5]. We find that room-temperature optical amplification can be obtained in the entire visible spectral range (440-700 nm) with low pump thresholds down to 5±1 µJ cm-2 and high values of modal net gain of at least 450±30 cm-1.
 
Here we also demonstrate that 0.5-1 centimeter large, solution-grown single crystals of APbI3  (where A is methylammonium  or  formamidinium mixed with Cs+) can serve as inexpensive, operating at ambient temperatures solid-state gamma detectors (e.g. for direct sensing of photons with energies as high as mega-electron-volts, MeV) [6].  Such possibility arises from extremely high room-temperature mobility(µ)-lifetime(t) product of 1.8 × 10-2 cm2 V-1, low dark carrier density 109 - 1011 cm-3 and low density of charge traps (~1010 cm–3), and high absorptivity of hard radiation by lead and iodine atoms. 
 
  1. L. Protesescu et al. Nano Letters 2015, 15, 3692–3696
  2. G. Nedelcu et al. Nano Letters 2015, 15, 5635–5640
  3. O. Vybornyi et al. Nanoscale 2016, 8, 6278-6283
  4. L. Protesescu et al. J. Am. Chem. Soc. 2016, DOI: 10.1021/jacs.6b08900
  5. S. Yakunin et al. Nature Communications 2015, 9, 8056.
  6. S. Yakunin et al. Nature Photonics 2016, 10, 585–589