Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites

Joshi, Prakriti Pradhan; Maehrlein, Sebastian F.; Zhu, Xiaoyang

doi:10.1002/adma.201803054

Title: Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites

Journal Article · Wed Jan 23 00:00:00 EST 2019 · Advanced Materials

DOI:https://doi.org/10.1002/adma.201803054· OSTI ID:1491924

Joshi, Prakriti Pradhan ^[1]; Maehrlein, Sebastian F. ^[1];

^[1]

Department of Chemistry Columbia University New York NY 10027 USA

Abstract Among the exceptional properties of lead halide perovskites (LHPs) is the ultraslow cooling of hot carriers. Carrier densities below the Mott density for large polarons (≤ ≈10 ¹⁸ cm ⁻³ ) are focused on here. As in other semiconductors, a nascent hot electron distribution initially cools down via emission of longitudinal optical (LO) phonons on the 10 ⁻¹⁴ –10 ⁻¹³ s timescale. What distinguishes LHPs from conventional semiconductors is the exceptionally efficient screening in the former. The dielectric screening in LHPs on the 10 ⁻¹³ s timescale results in an order‐of‐magnitude reduction in the Coulomb potential upon the formation of a large polaron, likely with ferroelectric‐like local ordering. Further LO‐phonon emission is inhibited, and this leads to partial retention of hot electron energy on the 10 ⁻¹² s timescale, more so in hybrid LHPs than in their all‐inorganic counterparts. Further cooling of hot polarons occurs on the 10 ⁻¹⁰ s timescale, and this can be attributed to the slow diffusion of heat out of the large polaron volume due to the low thermal conductivity of LHPs. Like other carrier properties, slow hot carrier cooling in LHPs can be intimately related to efficient screening in a soft, anharmonic, and dynamically disordered lattice.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: N00014‐18‐1‐2080; DE‐SC0010692

OSTI ID:: 1491924

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Vol. 31 Journal Issue: 47; ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 76 works

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