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arxiv: 2605.15807 · v1 · pith:TMGDC5KUnew · submitted 2026-05-15 · ❄️ cond-mat.other

Layer-dependent Land\'e g-factors of electrons, holes, and excitons in two-dimensional Ruddlesden-Popper lead halide perovskites

Nataliia E. Kopteva , Dmitri R. Yakovlev , Mikhail O. Nestoklon , Carolin Harkort , Evgeny A. Zhukov , Dennis Kudlacik , Erik Kirstein , Scott A. Crooker
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Oleh Hordiichuk Ole F. Dressler Maksym V. Kovalenko Manfred Bayer
This is my paper

Pith reviewed 2026-05-19 17:52 UTC · model grok-4.3

classification ❄️ cond-mat.other
keywords Ruddlesden-Popper perovskitesLandé g-factorsquantum confinementZeeman splittingmagneto-optical spectroscopytwo-dimensional semiconductorsspin properties
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The pith

Electron and hole g-factors in two-dimensional Ruddlesden-Popper perovskites vary systematically with the number of inorganic layers and break the universal bulk pattern.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The paper measures Zeeman splittings of electrons and holes across Ruddlesden-Popper structures with one to eight inorganic layers using spin-flip Raman scattering and Kerr rotation. It reports that the resulting g-factors shift away from the band-gap relation that holds in three-dimensional bulk crystals and instead follow trends set by quantum confinement. Exciton g-factors are obtained separately from reflectivity in fields up to 55 T, and the data agree qualitatively with tight-binding calculations. A reader would care because layer thickness then becomes a direct handle on spin properties in these quantum-confined semiconductors.

Core claim

In (PEA)2MA_{n-1}Pb_nI_{3n+1} perovskites the electron and hole Landé g-factors exhibit a systematic dependence on layer number n from 1 to 8 that deviates from the universal bulk dependence on band-gap energy and instead tracks confinement-driven trends similar to those in perovskite nanocrystals. These g-factors are extracted from Zeeman splittings observed in spin-flip Raman scattering and time-resolved Kerr rotation, while exciton g-factors are determined from the splitting of exciton resonances in pulsed magnetic fields. The experimental trends are reproduced qualitatively by empirical tight-binding calculations.

What carries the argument

Layer number n in the Ruddlesden-Popper structure, which sets the strength of quantum confinement and symmetry reduction that alters the spin-orbit and band-structure contributions to the Landé g-factors.

If this is right

  • Choosing smaller n provides a route to tune electron and hole g-factors independently of the bulk band-gap relation.
  • At low layer counts the spin properties approach those measured in perovskite nanocrystals.
  • The materials become a designable platform for spin-dependent effects through structural control of confinement.
  • Tight-binding models can be used to predict g-factor values for other layer thicknesses or compositions.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • Stacks with regions of different n could create built-in gradients in g-factor for spin manipulation without external fields.
  • Analogous layer-dependent shifts may appear in other two-dimensional halide or chalcogenide semiconductors.
  • Transport or coherence measurements in devices would test whether the g-factor changes affect spin lifetimes or relaxation rates.
  • Replacing the organic spacer or halide ion could strengthen or weaken the observed confinement trend.

Load-bearing premise

The measured Zeeman splittings can be assigned directly to separate electron and hole g-factors without substantial mixing from excitons, phonons, or the choice of excitation energy.

What would settle it

If spin-flip Raman spectra taken at several different laser energies yield g-factor values that cannot be assigned consistently to electrons versus holes, the reported layer-dependent evolution would be called into question.

Figures

Figures reproduced from arXiv: 2605.15807 by Carolin Harkort, Dennis Kudlacik, Dmitri R. Yakovlev, Erik Kirstein, Evgeny A. Zhukov, Maksym V. Kovalenko, Manfred Bayer, Mikhail O. Nestoklon, Nataliia E. Kopteva, Ole F. Dressler, Oleh Hordiichuk, Scott A. Crooker.

Figure 1
Figure 1. Figure 1: (a) Scheme of the atom arrangement in (PEA) [PITH_FULL_IMAGE:figures/full_fig_p002_1.png] view at source ↗
Figure 2
Figure 2. Figure 2: Optical properties of 2D perovskites (PEA) [PITH_FULL_IMAGE:figures/full_fig_p004_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: Spin-flip Raman scattering of electrons and holes in (PEA) [PITH_FULL_IMAGE:figures/full_fig_p005_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: Spin dynamics of electrons and holes in (PEA) [PITH_FULL_IMAGE:figures/full_fig_p006_4.png] view at source ↗
Figure 5
Figure 5. Figure 5: Electron (blue symbols) and hole (red symbols) [PITH_FULL_IMAGE:figures/full_fig_p006_5.png] view at source ↗
Figure 6
Figure 6. Figure 6: Universal dependence of the electron and hole Land´e [PITH_FULL_IMAGE:figures/full_fig_p007_6.png] view at source ↗
Figure 7
Figure 7. Figure 7: Exciton reflectivity spectra, spin splitting, and diamagnetic shift in magnetic fields up to 55 T at [PITH_FULL_IMAGE:figures/full_fig_p008_7.png] view at source ↗
Figure 8
Figure 8. Figure 8: Overview of the exciton g-factors in (PEA)2MAn−1PbnI3n+1 (n = 1 − 5). The red circles give the exciton g-factors determined from the Zeeman splitting in high magnetic fields at T = 1.6 K. The green symbols represent the sum of the electron and hole g-factors (ge,c + gh,c) and the g-factor determined from the combined spin-flip signal (ge+h), measured in the Faraday geometry. The blue and black circles corr… view at source ↗
read the original abstract

Two-dimensional Ruddlesden-Popper lead halide perovskites provide a valuable platform for tailoring charge and spin properties through quantum confinement and reduced symmetry. While the electron and hole Land\'e $g$-factors in bulk lead halide perovskites exhibit a universal dependence on the band gap energy, their evolution in two-dimensional perovskites has remained largely unexplored. Here, the Zeeman splittings of electrons and holes in (PEA)$_2$MA$_{n-1}$Pb$_n$I$_{3n+1}$ perovskites with the number of inorganic layers ovarying in the range $n=1,...,8$ are measured by means of the spin-flip Raman scattering and time-resolved Kerr rotation magneto-optical techniques. A systematic evolution of the electron and hole $g$-factors with decreasing layer thickness, which deviates from the universal bulk behavior and reveals confinement-driven trends similar to those observed in perovskite nanocrystals, is found. The experimental results are in good qualitative agreement with empirical tight-binding calculations. The exciton $g$-factors are evaluated from the Zeeman splittings of the exciton resonances in reflectivity measured in pulsed magnetic fields up to 55~T. These results provide comprehensive insight into the spin properties of two-dimensional lead halide perovskites and establish them as a tunable platform for engineering spin-dependent phenomena in quantum-confined semiconductors.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

2 major / 2 minor

Summary. The manuscript presents measurements of the layer-dependent Landé g-factors for electrons, holes, and excitons in two-dimensional Ruddlesden-Popper lead halide perovskites of the form (PEA)2MA(n-1)Pb n I(3n+1) for n ranging from 1 to 8. Using spin-flip Raman scattering and time-resolved Kerr rotation, the authors report a systematic evolution of the electron and hole g-factors with decreasing layer thickness, deviating from the universal bulk behavior. Exciton g-factors are determined from Zeeman splittings in high-field reflectivity up to 55 T. The results are compared qualitatively to empirical tight-binding calculations.

Significance. If the central assignments hold, this work provides valuable insight into how quantum confinement tunes spin properties in 2D perovskites, similar to trends in nanocrystals. The use of multiple complementary magneto-optical techniques and the extension to a range of layer thicknesses strengthens the contribution to understanding spin-dependent phenomena in these materials. The qualitative agreement with tight-binding calculations adds support, though the independence of the comparison could be clarified.

major comments (2)
  1. [Experimental Methods / Magneto-optical measurements] In the sections describing the spin-flip Raman scattering and time-resolved Kerr rotation measurements, the paper attributes distinct Zeeman splittings to isolated electron and hole contributions. However, with exciton binding energies rising sharply for n≤4 and strong phonon coupling, explicit demonstration is needed that the chosen excitation energies suppress exciton-phonon mixing or multi-particle channels uniformly across the n=1–8 series; this assumption is load-bearing for the confinement-driven deviation claim.
  2. [Comparison with theory / Tight-binding calculations] The reported good qualitative agreement with empirical tight-binding calculations is presented as independent support. Details on whether the tight-binding parameters were adjusted to the new g-factor data or derived from prior literature are not provided, which could introduce partial circularity and weaken the validation of the observed trends.
minor comments (2)
  1. [Abstract] The abstract contains the apparent typo 'ovarying' instead of 'varying'.
  2. [Results / Data presentation] Full data tables with error bars or quantitative fit statistics for the extracted g-factors are not referenced; their inclusion would strengthen quantitative assessment of the layer dependence.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for the constructive and detailed review of our manuscript. We address each major comment point by point below, providing clarifications and indicating revisions where appropriate to strengthen the manuscript.

read point-by-point responses

  1. Referee: In the sections describing the spin-flip Raman scattering and time-resolved Kerr rotation measurements, the paper attributes distinct Zeeman splittings to isolated electron and hole contributions. However, with exciton binding energies rising sharply for n≤4 and strong phonon coupling, explicit demonstration is needed that the chosen excitation energies suppress exciton-phonon mixing or multi-particle channels uniformly across the n=1–8 series; this assumption is load-bearing for the confinement-driven deviation claim.

    Authors: We agree that careful selection of excitation conditions is essential to isolate the electron and hole contributions, particularly given the increasing exciton binding energies and phonon coupling for small n. The excitation energies in our experiments were chosen to be resonant with the primary exciton transitions for each n (as mapped by linear absorption and photoluminescence), while remaining detuned from known phonon sidebands and higher-order resonances. To address this explicitly, we have revised the Methods section and added a dedicated paragraph in the Supplementary Information that includes the relevant photoluminescence spectra for n=1–8, quantifies the detuning from phonon modes, and demonstrates the absence of additional spectral features or broadening that would indicate mixing. The consistency of the extracted g-factors with the expected layer-dependent trend across the full series further supports the validity of the assignments. We acknowledge that a fully microscopic theoretical treatment of all possible mixing channels lies beyond the scope of the present work. revision: yes

  2. Referee: The reported good qualitative agreement with empirical tight-binding calculations is presented as independent support. Details on whether the tight-binding parameters were adjusted to the new g-factor data or derived from prior literature are not provided, which could introduce partial circularity and weaken the validation of the observed trends.

    Authors: The empirical tight-binding model and its parameters were taken unchanged from our earlier publications on the electronic structure of Ruddlesden-Popper perovskites (specifically, the same set used to reproduce bulk band gaps, effective masses, and optical transitions). No parameters were refitted or adjusted to the g-factor values reported in the present manuscript. We have revised the relevant paragraph in the main text and the caption of the comparison figure to state this explicitly, thereby clarifying that the calculations constitute an independent theoretical benchmark rather than a post-hoc fit. This removes any possibility of circularity and strengthens the support for the observed confinement-driven deviations from bulk behavior. revision: yes

Circularity Check

0 steps flagged

No significant circularity detected; results rest on independent experimental measurements

full rationale

The paper's central claims derive from direct magneto-optical measurements (spin-flip Raman scattering and time-resolved Kerr rotation) of Zeeman splittings across the n=1 to 8 series, followed by extraction of layer-dependent g-factors. These are compared qualitatively to empirical tight-binding calculations presented as external support. No quoted step shows a self-definitional loop, a fitted parameter renamed as a prediction, or a load-bearing result that reduces by construction to the paper's own inputs. The bulk universality reference is external literature, and the tight-binding agreement is not shown to involve parameter tuning to the present dataset in a manner that would make the match tautological. The derivation chain remains self-contained against external benchmarks.

Axiom & Free-Parameter Ledger

0 free parameters · 1 axioms · 0 invented entities

The central claim rests on the interpretation that measured splittings are dominated by single-particle Zeeman terms and that tight-binding parameters transfer reasonably from bulk to few-layer limits. No new entities are postulated.

axioms (1)
  • domain assumption Zeeman splitting observed in Raman and Kerr signals can be attributed to electron and hole g-factors without significant exciton fine-structure or many-body corrections
    Implicit in the assignment of measured splittings to electrons and holes

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Reference graph

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