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

Li, Mingjie; Bhaumik, Saikat; Goh, Teck Wee; Muduli, Subas; Yantara, Natalia; Grätzel, Michaël; Mhaisalkar, Subodh; Mathews, Nripan; Sum, Tze Chien

doi:10.1038/ncomms14350

Cited by 338 publications

(565 citation statements)

References 40 publications

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“…TRPL (≈20 ps) Zhu et al [31] MAPbBr 3 films ≈0.7 ≈2.1 ≈350 <0.1 ≈15 ≈900 ≈0.8 TA (≈150 fs) Li et al [9] MAPbBr 3 NCs ≈2.6 ≈1650 ≈0.6 ≈3.5 ≈2200 ≈32…”

Section: Observations Of Slow Hc Cooling In Perovskitesmentioning

confidence: 99%

“…www.advmat.de www.advancedsciencenews.com dependence of photoexcited carrier density, [9,22,29,30,46,47] the initial HC excess energy, [22,29,46] cation species, [29][30][31]48] morphology, [49] and confinement effects (in nanocrystals) [9,50] on the HC cooling dynamics. Table 1 shows a comparison of the HC cooling times for halide perovskites and other conventional semiconductors.…”

Section: Observations Of Slow Hc Cooling In Perovskitesmentioning

confidence: 99%

“…A large atomic mass difference between the positively and negatively charged ions can lead to larger phononic bandgap and smaller ℏω LA-max . [9] Copyright 2017, Nature Publishing Group. 2) Lower Thermal Conductivity: Acoustic phonon uptransition is expected to be enhanced in perovskites by stronger localization of acoustic phonons and by blocking their propagation with lower thermal conductivities perovskites.…”

Section: Toolbox For Engineering Slow Hc Cooling In Halide Perovskitesmentioning

confidence: 99%

“…are candidates to exploit the confinement effects on the carriers, excitons, and phonons. [9] Adv. Previously, long-lived HCs in III-V semiconductor NWs were observed for CW excitation at high pump fluence.…”

Section: ) Perovskite Nanostructures and Quantum Confinementmentioning

confidence: 99%

“…

rapidly (within hundreds of femtoseconds), making HCs extraction extremely challenging. [9] Long HC transport lengths (≈600 nm) in MAPbI 3 thin films were visualized by Huang et al [10] These exciting findings forebode the potential of perovskite HCSCs that could dramatically boost perovskite solar cell efficiencies beyond their SQ limits. Since the first reports of slow HC cooling (≈0.4 ps) in MAPbI 3 polycrystalline thin films, [7,8] there have been growing interests about this novel phenomenon.

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confidence: 95%

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Slow Hot‐Carrier Cooling in Halide Perovskites: Prospects for Hot‐Carrier Solar Cells

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rapidly (within hundreds of femtoseconds), making HCs extraction extremely challenging. A reduced HC cooling rate in solar absorbers is therefore a key material criterion for realizing HCSC.Halide perovskites possess novel slow HC cooling properties favorable for development as HCSC. Since the first reports of slow HC cooling (≈0.4 ps) in MAPbI 3 polycrystalline thin films, [7,8] there have been growing interests about this novel phenomenon. Li et al. reported a drastic slowdown of HC cooling by a further two orders in MAPbBr 3 colloidal nanocrystals (≈30 ps) at high pump fluence and demonstrated efficient (≈83%) extraction of HCs with an energy-selective organic layer. [9] Long HC transport lengths (≈600 nm) in MAPbI 3 thin films were visualized by Huang et al. [10] These exciting findings forebode the potential of perovskite HCSCs that could dramatically boost perovskite solar cell efficiencies beyond their SQ limits. Presently, the origins and mechanisms of slow HC cooling in halide perovskites remain fragmented and confusing with disparate models being proposed. A clear understanding of the intrinsic photophysics of HC cooling is essential for further technological developments.In this review, we examine the milestones and advancements of slow HC cooling in halide perovskites and distill their photophysical mechanisms. We begin with a brief introduction of the operation principles of HCSCs and carrier relaxation processes, followed by highlighting the seminal experimental and theoretical works on slow HC cooling in halide perovskites, before explicating their origins and mechanisms. A developmental toolbox for engineering slow HC cooling in halide perovskites and developing new perovskite materials with slower HC cooling will also be discussed. Lastly, we highlight the challenges and opportunities for perovskite HCSCs. How Hot Carriers Can Be Used?We begin with a quick overview of the several concepts for highefficiency solar cells. Figure 1a illustrates the energy band diagram of a typical single junction solar cell with its major energy loss processes following light illumination. [11,12] In all solar cells, photons possessing energies greater than the semiconductor bandgap can create free carriers or excitons with excess energies above the bandgap. These carriers or excitons with a temperature higher than the lattice temperature are termed "hot Rapid hot-carrier cooling is a major loss channel in solar cells. Thermodynamic calculations reveal a 66% solar conversion efficiency for single junction cells (under 1 sun illumination) if these hot carriers are harvested before cooling to the lattice temperature. A reduced hot-carrier cooling rate for efficient extraction is a key enabler to this disruptive technology. Recently, halide perovskites emerge as promising candidates with favorable hot-carrier properties: slow hot-carrier cooling lifetimes several orders of magnitude longer than conventional solar cell absorbers, longrange hot-carrier transport (up to ≈600 nm), and highly efficient hot-carrier extractio...

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“…TRPL (≈20 ps) Zhu et al [31] MAPbBr 3 films ≈0.7 ≈2.1 ≈350 <0.1 ≈15 ≈900 ≈0.8 TA (≈150 fs) Li et al [9] MAPbBr 3 NCs ≈2.6 ≈1650 ≈0.6 ≈3.5 ≈2200 ≈32…”

Section: Observations Of Slow Hc Cooling In Perovskitesmentioning

confidence: 99%