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Systematic investigation of CO₂ : NH₃ ice mixtures using mid-IR and VUV spectroscopy - part 1: thermal processing.

ABSTRACT: The adjustment of experimental parameters in interstellar ice analogues can have profound effects on molecular synthesis within an ice system. We demonstrated this by systematically investigating the stoichiometric mixing ratios of CO₂ : NH₃ ices as a function of thermal processing using mid-IR and VUV spectroscopy. We observed that the type of CO₂ bonding environment was dependent on the different stoichiometric mixing ratios and that this pre-determined the NH₃ crystallite structure after phase change. The thermal reactivity of the ices was linked to the different chemical and physical properties of the stoichiometric ratios. Our results provide new details into the chemical and physical properties of the different stoichiometric CO₂ : NH₃ ices enhancing our understanding of the thermally induced molecular synthesis within this ice system.

SUBMITTER: James RL

PROVIDER: S-EPMC9057146 | biostudies-literature | 2020 Oct

REPOSITORIES: biostudies-literature

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Systematic investigation of CO2 : NH3 ice mixtures using mid-IR and VUV spectroscopy - part 1: thermal processing.

James Rachel L RL Ioppolo Sergio S Hoffmann Søren V SV Jones Nykola C NC Mason Nigel J NJ Dawes Anita A

RSC advances 20201012 61

The adjustment of experimental parameters in interstellar ice analogues can have profound effects on molecular synthesis within an ice system. We demonstrated this by systematically investigating the stoichiometric mixing ratios of CO2 : NH3 ices as a function of thermal processing using mid-IR and VUV spectroscopy. We observed that the type of CO2 bonding environment was dependent on the different stoichiometric mixing ratios and that this pre-determined the NH< ...[more]

PMID: 35521284

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Project description:One of the most effective approaches to optimizing the performance of perovskite solar cells is to fully understand the ultrafast carrier dynamics at the interfaces between absorber and transporting layers at both the molecular and atomic levels. Here, the injection dynamics of hot and relaxed charge carriers at the interface between the hybrid perovskite, formamidinium lead bromide (FAPbBr3), and the organic electron acceptor, IEICO-4F, are investigated and deciphered by using femtosecond (fs) mid-infrared (IR), transient absorption (TA), and fluorescence spectroscopies. The visible femtosecond-TA measurements reveal the generation of hot carriers and their transition to free carriers in the pure FAPbBr3 film. Meanwhile, the efficient extraction of hot carriers in the mixed FAPbBr3/IEICO-4F film is clearly evidenced by the complete disappearance of their spectral signature. More specifically, the time-resolved results reveal that hot carriers are injected from FAPbBr3 to IEICO-4F within 150 fs, while the transfer time for the relaxed carriers is about 205 fs. The time-resolved mid-IR experiments also demonstrate the ultrafast formation of two peaks at 2115 and 2233 cm-1, which can be attributed to the C≡N symmetrical and asymmetrical vibrational modes of anionic IEICO-4F, thus providing crystal clear evidence for the electron transfer process between the donor and acceptor units. Moreover, photoluminescence (PL) lifetime measurements reveal an approximately 10-fold decrease in the donor lifetime in the presence of IEICO-4F, thereby confirming the efficient electron injection from the perovskite to the acceptor unit. In addition, the efficient electron injection at the FAPbBr3/IEICO-4F interface and its impact on the C≡N bond character are experimentally evidenced and align with density functional theory (DFT) calculations. This work offers new insights into the electron injection process at the FAPbBr3/IEICO-4F interface, which is crucial for developing efficient optoelectronic devices.

Dataset Information

Systematic investigation of CO₂ : NH₃ ice mixtures using mid-IR and VUV spectroscopy - part 1: thermal processing.

Publications

Systematic investigation of CO<sub>2</sub> : NH<sub>3</sub> ice mixtures using mid-IR and VUV spectroscopy - part 1: thermal processing.

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