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Understanding of dielectric properties of cellulose

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Abstract

The theoretical understanding of structural and optoelectronic properties is well-established for a range of inorganic materials; however, such a robust foundation is, in large part, absent in the case of cellulose. Existing literature reports a wide variance in experimentally observed properties for cellulose phases, which are often in contradiction to each other. Motivated by this, we perform an exhaustive first-principles investigation of the structural and optoelectronic properties of cellulose Iα and Iβ phases. Utilizing exchange–correlation functionals that accurately describe van der Waals interaction and leveraging state-of-the-art density functional theory methods, we strive to present a highly accurate periodic model for the cellulose phases. We integrate the framework of volume-average theory and the potential impact of water sorption to offer insights into the considerable discrepancies seen across different experimental outcomes. Thus, our study provides a reconciliatory perspective, bridging the gap between theoretical calculations and disparate experimental data.

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Acknowledgments

We gratefully acknowledge Poland’s high-performance computing infrastructure PLGrid (HPC Centers: ACK Cyfronet AGH) for providing computer facilities and support within computational grant no. PLG/2023/016228 and for awarding this project access to the LUMI supercomputer, owned by the EuroHPC Joint Undertaking, hosted by CSC (Finland) and the LUMI consortium through grant no. PLL/2023/4/016319.

Funding

This work is supported by the “ENSEMBLE3-Centre of Excellence for nanophotonics, advanced materials and novel crystal growth-based technologies” project (Grant Agreement No. MAB/2020/14), which is a part of the International Research Agendas programme of the Foundation for Polish Science. It receives co-financing from the European Union under the European Regional Development Fund and the European Union’s Horizon 2020 research and innovation programme, specifically through the Teaming for Excellence initiative (Grant Agreement No. 857543). The research work conducted by M.B. and O.I.M. in 2024 was supported through Project No. 2022/47/P/ST3/01236 co-funded by the National Science Centre and the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No. 945339.

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  1. Centre of Excellence ENSEMBLE3 Sp. z o. o., Wolczynska Str. 133, 01-919, Warsaw, Poland

    Asha Yadav, Mathias Boström & Oleksandr I. Malyi

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  1. Asha Yadav
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  2. Mathias Boström
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  3. Oleksandr I. Malyi
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Contributions

AY carried out the main calculations, part of the literature review, and main data analysis. AY prepared the main figures and edited the manuscript. MB supported the investigation and contributed to project development/manuscript editing. OIM designed the idea, wrote the original draft, provided supervision, and conducted verification of the main data analysis.

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Correspondence to Oleksandr I. Malyi.

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Yadav, A., Boström, M. & Malyi, O.I. Understanding of dielectric properties of cellulose. Cellulose 31, 2783–2794 (2024). https://doi.org/10.1007/s10570-024-05754-7

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