Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals

Mingjie Li, Saikat Bhaumik, Teck Wee Goh, Muduli Subas Kumar, Natalia Yantara, Michael Grätzel, Subodh Mhaisalkar, Nripan Mathews () and Tze Chien Sum ()
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Mingjie Li: School of Physical and Mathematical Sciences, Nanyang Technological University
Saikat Bhaumik: Energy Research Institute @ NTU (ERI@N)
Teck Wee Goh: School of Physical and Mathematical Sciences, Nanyang Technological University
Muduli Subas Kumar: Energy Research Institute @ NTU (ERI@N)
Natalia Yantara: Energy Research Institute @ NTU (ERI@N)
Michael Grätzel: Energy Research Institute @ NTU (ERI@N)
Subodh Mhaisalkar: Energy Research Institute @ NTU (ERI@N)
Nripan Mathews: Energy Research Institute @ NTU (ERI@N)
Tze Chien Sum: School of Physical and Mathematical Sciences, Nanyang Technological University

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract Hot-carrier solar cells can overcome the Shockley-Queisser limit by harvesting excess energy from hot carriers. Inorganic semiconductor nanocrystals are considered prime candidates. However, hot-carrier harvesting is compromised by competitive relaxation pathways (for example, intraband Auger process and defects) that overwhelm their phonon bottlenecks. Here we show colloidal halide perovskite nanocrystals transcend these limitations and exhibit around two orders slower hot-carrier cooling times and around four times larger hot-carrier temperatures than their bulk-film counterparts. Under low pump excitation, hot-carrier cooling mediated by a phonon bottleneck is surprisingly slower in smaller nanocrystals (contrasting with conventional nanocrystals). At high pump fluence, Auger heating dominates hot-carrier cooling, which is slower in larger nanocrystals (hitherto unobserved in conventional nanocrystals). Importantly, we demonstrate efficient room temperature hot-electrons extraction (up to ∼83%) by an energy-selective electron acceptor layer within 1 ps from surface-treated perovskite NCs thin films. These insights enable fresh approaches for extremely thin absorber and concentrator-type hot-carrier solar cells.

Date: 2017
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DOI: 10.1038/ncomms14350

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