Article, 2024

Tailoring Auger Recombination Dynamics in CsPbI3 Perovskite Nanocrystals via Transition Metal Doping

Nano Letters, ISSN 1530-6984, 1530-6992, Volume 24, 27, Pages 8386-8393, 10.1021/acs.nanolett.4c02032

Contributors

Meng, Jie 0000-0002-3813-5221 [1] [2] Lan, Zhenyun 0000-0001-7943-5936 (Corresponding author) [1] [3] Lin, Weihua 0000-0003-3623-0353 [2] Castelli, Ivano Eligio 0000-0001-5880-5045 [1] Pullerits, Tõnu 0000-0003-1428-5564 (Corresponding author) [2] Zheng, Kaibo 0000-0002-7236-1070 (Corresponding author) [1] [2]

Affiliations

  1. [1] Technical University of Denmark
    2. [NORA names: DTU Technical University of Denmark; University; Denmark; Europe, EU; Nordic; OECD];
  2. [2] Lund University
    3. [NORA names: Sweden; Europe, EU; Nordic; OECD];
  3. [3] Hefei University of Technology
    4. [NORA names: China; Asia, East]

Abstract

Auger recombination is a pivotal process for semiconductor nanocrystals (NCs), significantly affecting charge carrier generation and collection in optoelectronic devices. This process depends mainly on the NCs' electronic structures. In our study, we investigated Auger recombination dynamics in manganese (Mn2+)-doped CsPbI3 NCs using transient absorption (TA) spectroscopy combined with theoretical and experimental structural characterization. Our results show that Mn2+ doping accelerates Auger recombination, reducing the biexciton lifetime from 146 to 74 ps with increasing Mn doping concentration up to 10%. This accelerated Auger recombination in Mn-doped NCs is attributed to increased band edge wave function overlap of excitons and a larger density of final states of Auger recombination due to Mn orbital involvement. Moreover, Mn doping reduces the dielectric screening of the excitons, which also contributes to the accelerated Auger recombination. Our study demonstrates the potential of element doping to regulate Auger recombination rates by modifying the materials' electronic structure.

Keywords

Auger, Auger recombination, Auger recombination rate, CsPbI3, CsPbI3 perovskite nanocrystals, Mn doping, Mn doping concentration, Mn-doped nanocrystals, absorption, biexciton lifetime, carrier generation, characterization, charge carrier generation, collection, concentration, density, devices, dielectric screening, doping, doping concentration, dynamics, electronic structure, element doping, excitons, experimental structural characterization, generation, increasing Mn doping concentration, involvement, lifetime, manganese, material's electronic structure, materials, metal doping, nanocrystal electronic structure, nanocrystals, optoelectronic devices, orbital involvement, perovskite nanocrystals, potential, process, rate, recombination, recombination dynamics, recombination rate, results, screening, semiconductor, semiconductor nanocrystals, state, structural characterization, structure, study, transient absorption, transition, transition metal doping

Funders

  • Swedish Energy Agency
  • Swedish Research Council
  • Carl Tryggers stiftelse för vetenskaplig forskning
  • Royal Physiographic Society of Lund
  • The Velux Foundations

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