Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite

An understanding of charge-carrier recombination processes is essential for the development of hybrid metal halide perovskites for photovoltaic applications. We show that typical measurements of the radiative bimolecular recombination constant in CH3NH3PbI3 are strongly affected by photon re-absorpt...

Descripción completa

Detalles Bibliográficos
Autores principales: Crothers, T, Milot, R, Patel, J, Parrott, E, Schlipf, J, Muller-Buschbaum, P, Johnston, M, Herz, L
Formato: Journal article
Lenguaje:English
Publicado: American Chemical Society 2017
_version_ 1826289505835941888
author Crothers, T
Milot, R
Patel, J
Parrott, E
Schlipf, J
Muller-Buschbaum, P
Johnston, M
Herz, L
author_facet Crothers, T
Milot, R
Patel, J
Parrott, E
Schlipf, J
Muller-Buschbaum, P
Johnston, M
Herz, L
author_sort Crothers, T
collection OXFORD
description An understanding of charge-carrier recombination processes is essential for the development of hybrid metal halide perovskites for photovoltaic applications. We show that typical measurements of the radiative bimolecular recombination constant in CH3NH3PbI3 are strongly affected by photon re-absorption which masks a much larger intrinsic bimolecular recombination rate constant. By investigating a set of films whose thickness varies between 50nm and 533nm, we find that the bimolecular charge recombination rate appears to slow by an order of magnitude as the film thickness increases. However, by using a dynamical model that accounts for photon re-absorption and charge-carrier diffusion we determine that a single intrinsic bimolecular recombination coefficient, of value 6.8x10(-10)cm(3)s(-1), is common to all samples irrespective of film thickness. Hence we postulate that the wide range of literature values reported for such coefficients is partly to blame on differences in photon out-coupling between samples, with crystal grains or mesoporous scaffolds of different sizes influencing light scattering, while thinner films or index-matched surrounding layers can reduce the possibility for photon re-absorption. We discuss the critical role of photon confinement on free charge-carrier retention in thin photovoltaic layers and highlight an approach to assess the success of such schemes from transient spectroscopic measurement.
first_indexed 2024-03-07T02:29:54Z
format Journal article
id oxford-uuid:a6e09f1e-f508-4cde-8f5a-1bd19e9ca119
institution University of Oxford
language English
last_indexed 2024-03-07T02:29:54Z
publishDate 2017
publisher American Chemical Society
record_format dspace
spelling oxford-uuid:a6e09f1e-f508-4cde-8f5a-1bd19e9ca1192022-03-27T02:50:38ZPhoton Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 PerovskiteJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:a6e09f1e-f508-4cde-8f5a-1bd19e9ca119EnglishSymplectic Elements at OxfordAmerican Chemical Society2017Crothers, TMilot, RPatel, JParrott, ESchlipf, JMuller-Buschbaum, PJohnston, MHerz, LAn understanding of charge-carrier recombination processes is essential for the development of hybrid metal halide perovskites for photovoltaic applications. We show that typical measurements of the radiative bimolecular recombination constant in CH3NH3PbI3 are strongly affected by photon re-absorption which masks a much larger intrinsic bimolecular recombination rate constant. By investigating a set of films whose thickness varies between 50nm and 533nm, we find that the bimolecular charge recombination rate appears to slow by an order of magnitude as the film thickness increases. However, by using a dynamical model that accounts for photon re-absorption and charge-carrier diffusion we determine that a single intrinsic bimolecular recombination coefficient, of value 6.8x10(-10)cm(3)s(-1), is common to all samples irrespective of film thickness. Hence we postulate that the wide range of literature values reported for such coefficients is partly to blame on differences in photon out-coupling between samples, with crystal grains or mesoporous scaffolds of different sizes influencing light scattering, while thinner films or index-matched surrounding layers can reduce the possibility for photon re-absorption. We discuss the critical role of photon confinement on free charge-carrier retention in thin photovoltaic layers and highlight an approach to assess the success of such schemes from transient spectroscopic measurement.
spellingShingle Crothers, T
Milot, R
Patel, J
Parrott, E
Schlipf, J
Muller-Buschbaum, P
Johnston, M
Herz, L
Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite
title Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite
title_full Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite
title_fullStr Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite
title_full_unstemmed Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite
title_short Photon Re-Absorption Masks Intrinsic Bimolecular Charge-Carrier Recombination in CH3NH3PbI3 Perovskite
title_sort photon re absorption masks intrinsic bimolecular charge carrier recombination in ch3nh3pbi3 perovskite
work_keys_str_mv AT crotherst photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT milotr photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT patelj photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT parrotte photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT schlipfj photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT mullerbuschbaump photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT johnstonm photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite
AT herzl photonreabsorptionmasksintrinsicbimolecularchargecarrierrecombinationinch3nh3pbi3perovskite