Vibrational and Electronic Properties of Np2O5 from Experimental Spectroscopy and First Principles Calculations

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Main Authors: Rai, Binod K, Zhou, Shuxiang, Heiner, Benjamin R., Tran, Gia Thinh, Szymanowski, Jennifer E. S., KC, Santosh, Shehee, Thomas C., Burns, Peter C., Beaux II, Miles F., Sadergaski, Luke R
Format: Preprint
Published: 2026
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author Rai, Binod K
Zhou, Shuxiang
Heiner, Benjamin R.
Tran, Gia Thinh
Szymanowski, Jennifer E. S.
KC, Santosh
Shehee, Thomas C.
Burns, Peter C.
Beaux II, Miles F.
Sadergaski, Luke R
author_facet Rai, Binod K
Zhou, Shuxiang
Heiner, Benjamin R.
Tran, Gia Thinh
Szymanowski, Jennifer E. S.
KC, Santosh
Shehee, Thomas C.
Burns, Peter C.
Beaux II, Miles F.
Sadergaski, Luke R
contents High-valence actinide oxides are critical to understanding the behavior of 5f-electrons, yet their structural and electronic properties remain poorly understood due to challenges in synthesis and handling. We report the first Raman spectroscopic study of single-crystalline Np2O5 and the first scanning tunneling spectroscopy (STS) measurement on any neptunium-containing material. Hydrothermally synthesized crystals were structurally verified by X-ray diffraction. Raman spectra revealed sharply resolved vibrational features, including previously unreported low-frequency modes. STS measurements revealed a band gap of 1.5 eV. Density functional theory (DFT) enables vibrational mode assignments, reveals neptunium-dominated low-frequency phonons, oxygen-dominated high-frequency modes, and predicts an indirect band gap of 1.68 eV. This predicted value is in excellent agreement with the experimentally measured STS gap. This combined Raman, DFT, and STS approach provides a robust framework for correlating lattice dynamics and electronic structure in actinide materials, providing benchmark data for Np2O5, and opening new avenues for probing structure-property relationships in complex f-electron materials.
format Preprint
id arxiv_https___arxiv_org_abs_2601_20242
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Vibrational and Electronic Properties of Np2O5 from Experimental Spectroscopy and First Principles Calculations
Rai, Binod K
Zhou, Shuxiang
Heiner, Benjamin R.
Tran, Gia Thinh
Szymanowski, Jennifer E. S.
KC, Santosh
Shehee, Thomas C.
Burns, Peter C.
Beaux II, Miles F.
Sadergaski, Luke R
Materials Science
Strongly Correlated Electrons
High-valence actinide oxides are critical to understanding the behavior of 5f-electrons, yet their structural and electronic properties remain poorly understood due to challenges in synthesis and handling. We report the first Raman spectroscopic study of single-crystalline Np2O5 and the first scanning tunneling spectroscopy (STS) measurement on any neptunium-containing material. Hydrothermally synthesized crystals were structurally verified by X-ray diffraction. Raman spectra revealed sharply resolved vibrational features, including previously unreported low-frequency modes. STS measurements revealed a band gap of 1.5 eV. Density functional theory (DFT) enables vibrational mode assignments, reveals neptunium-dominated low-frequency phonons, oxygen-dominated high-frequency modes, and predicts an indirect band gap of 1.68 eV. This predicted value is in excellent agreement with the experimentally measured STS gap. This combined Raman, DFT, and STS approach provides a robust framework for correlating lattice dynamics and electronic structure in actinide materials, providing benchmark data for Np2O5, and opening new avenues for probing structure-property relationships in complex f-electron materials.
title Vibrational and Electronic Properties of Np2O5 from Experimental Spectroscopy and First Principles Calculations
topic Materials Science
Strongly Correlated Electrons
url https://arxiv.org/abs/2601.20242