2022Nano LettersOpen access

Area-Independence of the Biexciton Oscillator Strength in CdSe Colloidal Nanoplatelets

Carmelita Rodà, Pieter Geiregat, Alessio Di Giacomo, Iwan Moreels, Zeger Hens

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Abstract

Colloidal CdSe nanoplatelets (NPLs) are unique systems to study two-dimensional excitons and excitonic complexes. However, while absorption and emission of photons through exciton formation and recombination have been extensively quantified, few studies have addressed the exciton–biexciton transition. Here, we use cross-polarized pump–probe spectroscopy to measure the absorption coefficient spectrum of this transition and determine the biexciton oscillator strength ( f BX ). We show that f BX is independent of the NPL area and that the concomitant biexciton area ( S BX ) agrees with predictions of a short-range interaction model. Moreover, we show that f BX is comparable to the oscillator strength of forming localized excitons at room temperature while being unaffected itself by center-of-mass localization. These results confirm the relevance of biexcitons for light–matter interaction in NPLs. Moreover, the quantification of the exciton–biexciton transition introduced here will enable researchers to rank 2D materials by the strength of this transition and to compare experimental results with theoretical predictions.

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Colloidal CdSe nanoplatelets (NPLs) are unique systems to study two-dimensional excitons and excitonic complexes. However, while absorption and emission of photons through exciton formation and recombination have been extensively quantified, few studies have addressed the exciton–biexciton transition. Here, we use cross-polarized pump–probe spectroscopy to measure the absorption coefficient spectrum of this transition and determine the biexciton oscillator strength ( f BX ). We show that f BX is independent of the NPL area and that the concomitant biexciton area ( S BX ) agrees with predictions of a short-range interaction model. Moreover, we show that f BX is comparable to the oscillator strength of forming localized excitons at room temperature while being unaffected itself by center-of-mass localization. These results confirm the relevance of biexcitons for light–matter interaction in NPLs. Moreover, the quantification of the exciton–biexciton transition introduced here will enable researchers to rank 2D materials by the strength of this transition and to compare experimental results with theoretical predictions.

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Available abstract

Colloidal CdSe nanoplatelets (NPLs) are unique systems to study two-dimensional excitons and excitonic complexes. However, while absorption and emission of photons through exciton formation and recombination have been extensively quantified, few studies have addressed the exciton–biexciton transition. Here, we use cross-polarized pump–probe spectroscopy to measure the absorption coefficient spectrum of this transition and determine the biexciton oscillator strength ( f BX ). We show that f BX is independent of the NPL area and that the concomitant biexciton area ( S BX ) agrees with predictions of a short-range interaction model. Moreover, we show that f BX is comparable to the oscillator strength of forming localized excitons at room temperature while being unaffected itself by center-of-mass localization. These results confirm the relevance of biexcitons for light–matter interaction in NPLs. Moreover, the quantification of the exciton–biexciton transition introduced here will enable researchers to rank 2D materials by the strength of this transition and to compare experimental results with theoretical predictions.

Key concepts: Biexciton, Oscillator strength, Exciton, Materials science, Absorption (acoustics), Molecular physics, Condensed matter physics, Physics

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