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dc.contributor.authorBlundell, S. A.en_US
dc.contributor.authorNguyen, T. P. T.en_US
dc.contributor.authorGuet, Claudeen_US
dc.identifier.citationBlundell, S. A., Nguyen, T. P. T. & Guet, C. (2021). Calculation of two-photon absorption by nanocrystals of CsPbBr3. Physical Review B, 103(4), 045415-.
dc.description.abstractWe present calculations of the two-photon absorption cross section σ(2)(ω) for nanocrystals (NCs) of the inorganic perovskite CsPbBr3 for photon energies ω ranging from the absorption threshold at 2ω≈2.3eV up to 2ω=3.1eV. The calculations employ a 4×4k⋅p envelope-function model, with final-state excitons described in a self-consistent Hartree-Fock approximation. The k⋅p corrections to σ(2)(ω) are found to be rather large, giving a reduction of about 30% in the cross section at the largest energies considered. The cross section is shown to be independent of polarization in the effective-mass approximation (EMA), but including k⋅p corrections leads to a small difference in σ(2)(ω) between circular and linear polarization, which rises to about 16% at 2ω=3.1eV. The theoretical cross section follows closely a power-law dependence on NC size, σ(2)(ω)∝Lα, with theoretical exponents α=3.4 (EMA) or α=3.2 (4×4k⋅p model), in excellent agreement with experiment. The dominant contribution to the exponent α is shown to be the number of final-state excitons per unit energy. Measured values of the absolute (normalized) cross section σ(2)(ω) show a large spread of values, differing by as much as a factor of 25 for some NC sizes. Our calculations strongly favor a group of measurements at the lower end of the reported range of σ(2)(ω).en_US
dc.description.sponsorshipNational Research Foundation (NRF)en_US
dc.relation.ispartofPhysical Review Ben_US
dc.rights© 2021 American Physical Society (APS). All rights reserved. This paper was published in Physical Review B and is made available with permission of American Physical Society (APS).en_US
dc.titleCalculation of two-photon absorption by nanocrystals of CsPbBr3en_US
dc.typeJournal Articleen
dc.contributor.schoolSchool of Materials Science and Engineeringen_US
dc.contributor.researchEnergy Research Institute @ NTU (ERI@N)en_US
dc.description.versionPublished versionen_US
dc.subject.keywordsElectronic Structureen_US
dc.description.acknowledgementThe authors would like to thank Sum T. C. for helpful discussions. They acknowledge the France-Singapore Merlion Project 2.05.16 for supporting mutual visits. T.P.T.N. and S.A.B. are grateful to F. Schuster of the CEA's PTMA program for financial support. C.G. gratefully acknowledges financial support from the National Research Foundation through the Competitive Research Program, Grant No. NRF-CRP14-2014-03.en_US
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