Preprints
https://doi.org/10.5194/mr-2025-2
https://doi.org/10.5194/mr-2025-2
14 Feb 2025
 | 14 Feb 2025
Status: a revised version of this preprint is currently under review for the journal MR.

Automated wideline nuclear quadrupole resonance of mixed-cation lead halide perovskites

Jop W. Wolffs, Jennifer Gomez, Gerrit E. Janssen, Gilles A. de Wijs, and Arno P. M. Kentgens

Abstract. Nuclear quadrupole resonance (NQR) is a sister technique to NMR that is extremely sensitive to local crystal composition and structure. Unfortunately, in disordered materials this sensitivity also leads to very large linewidths, presenting a technical challenge and requiring a serious time investment to get a full spectrum. Here we describe our newly developed, automated NQR setup to acquire high-quality wideline spectra. Using this setup, we carried out 127I NQR on three mixed cation lead halide perovskites (LHPs) of the form MAxFA1−xPbI3 (MA = methylammonium, FA = formamidinium, x = 0.25,0.50,0.75) at various temperatures. We achieve a signal-to-noise of up to ~ 400 for lineshapes with a full-width-half-maximum of ~ 2.5 MHz acquired with a spectral width of 20 MHz in the course of two to three days. The spectra, which at least partially exhibit features encoding structural information, are interpreted using a statistical model. This model finds a degree of MA–MA, FA–FA clustering (0.2 ≤ S ≤ 0.35). This proof-of-principle for both the wideline NQR setup and the statistical model widens the applicability of an underutilised avenue of non-invasive structural research.

Competing interests: At least one of the (co-)authors is a member of the editorial board of Magnetic Resonance.

Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this preprint. The responsibility to include appropriate place names lies with the authors.
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Jop W. Wolffs, Jennifer Gomez, Gerrit E. Janssen, Gilles A. de Wijs, and Arno P. M. Kentgens

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on mr-2025-2', Anonymous Referee #1, 27 Feb 2025
    • AC1: 'Reply on RC1', Arno Kentgens, 23 Mar 2025
  • RC2: 'Comment on mr-2025-2', Anonymous Referee #2, 28 Feb 2025
    • AC2: 'Reply on RC2', Arno Kentgens, 23 Mar 2025
Jop W. Wolffs, Jennifer Gomez, Gerrit E. Janssen, Gilles A. de Wijs, and Arno P. M. Kentgens
Jop W. Wolffs, Jennifer Gomez, Gerrit E. Janssen, Gilles A. de Wijs, and Arno P. M. Kentgens

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Short summary
Nuclear quadrupole resonance is a sensitive technique for studying local structure. However, materials whose local structure is disordered can produce very wide spectra that are both technically challenging and require a lot of human-hours to measure. We present a setup that acquires these spectra automatically over a wide frequency range. We demonstrate this setup on several lead halide perovskites at variable temperatures and discuss the details uncovered by high resolution spectra.
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