Excitonic optical interface for GHz-THz collective excitations in a van der Waals magnet

Alberto Brambilla; Alessandro Ferretti; Alexey V. Scherbakov; David Maximilian Janas; Mattia Benini; Mirko Cinchetti; Rafael R. Rojas-Lopez; Richard Leven; Sophie Bork; Swagata Acharya

arxiv: 2511.20268 · v2 · pith:EVHRA237new · submitted 2025-11-25 · ❄️ cond-mat.mtrl-sci

Excitonic optical interface for GHz-THz collective excitations in a van der Waals magnet

Sophie Bork , Richard Leven , Vincent Wirsd\"orfer , Alessandro Ferretti , Rafael R. Rojas-Lopez , Mattia Benini , David Maximilian Janas , Umut Parlak

show 4 more authors

Alberto Brambilla Alexey V. Scherbakov Swagata Acharya Mirko Cinchetti

This is my paper

Pith reviewed 2026-05-25 07:45 UTC · model grok-4.3

classification ❄️ cond-mat.mtrl-sci

keywords CrSBrexcitonsmagnonsphononstransient reflectivityvan der Waals magnetoptical interfacecollective excitations

0 comments

The pith

Excitonic resonances in CrSBr create a broadband optical interface for GHz magnons and THz phonons through an emergent resonance at 1.46 eV with pi-phase inversion.

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

The paper establishes that excitons in the van der Waals antiferromagnet CrSBr couple optically to collective spin and lattice excitations spanning GHz to THz frequencies. Femtosecond broadband transient reflectivity shows that both magnons and phonons modulate the dielectric response to produce the same new resonance at 1.46 eV, which is invisible in steady-state spectra and displays a characteristic pi-phase inversion. This signature is explained by the excitations transferring spectral weight from a nominally dark exciton into an observable optical channel without any equilibrium oscillator strength. Many-body calculations identify the feature as a higher-energy exciton with distinct momentum and orbital character whose optical matrix elements are strongly suppressed.

Core claim

Excitonic resonances in the van der Waals antiferromagnet CrSBr provide a broadband optical interface for GHz magnon and THz phonon modes. These excitations give rise to an emergent resonance at 1.46 eV that is absent in steady-state spectra and exhibits a pi-phase inversion. The behaviour arises from boson-driven modulation of the dielectric response, which transiently transfers spectral weight from a nominally dark exciton into an observable channel. Many-body calculations assign the feature to a higher-energy exciton with distinct momentum and orbital character and strongly suppressed optical matrix elements.

What carries the argument

Boson-driven modulation of the dielectric response that transfers spectral weight from a nominally dark exciton to generate the emergent 1.46 eV resonance

If this is right

Both GHz magnons and THz phonons produce the identical emergent optical resonance despite their different origins and frequencies.
The optical interface functions without requiring any finite equilibrium oscillator strength.
The mechanism enables detection of collective excitations across GHz, THz and optical scales through the same excitonic channel.
Many-body calculations confirm the assignment of the 1.46 eV feature to a higher-energy exciton with suppressed matrix elements.

Where Pith is reading between the lines

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

The same excitonic modulation approach could be tested in other van der Waals magnets to enable optical readout of spin dynamics at room temperature.
Time-resolved spectra might uncover additional dark excitonic states in related layered materials through analogous boson-driven weight transfer.
Integration with optical waveguides could allow hybrid devices where magnon or phonon information is converted to light signals at the 1.46 eV energy.

Load-bearing premise

The 1.46 eV feature corresponds to a higher-energy exciton with distinct momentum and orbital character whose optical matrix elements are strongly suppressed at equilibrium.

What would settle it

Direct observation of finite oscillator strength for the 1.46 eV transition in equilibrium absorption spectra, or the lack of pi-phase inversion in the transient reflectivity response, would falsify the spectral-weight-transfer mechanism.

read the original abstract

Collective spin and lattice excitations in quantum materials span energy scales from GHz to THz, yet establishing a unified optical interface for these modes remains a central challenge. Here we show that excitonic resonances in the van der Waals antiferromagnet CrSBr provide a broadband optical interface for such excitations. Using femtosecond broadband transient reflectivity, we resolve coherent GHz magnon and THz phonon modes that modulate the dielectric response over a wide spectral range. Despite their distinct microscopic origin and frequency scales, both excitations give rise to the same emergent optical signature: a resonance at 1.46 eV that is absent in steady-state spectra and exhibits a characteristic {\pi}-phase inversion, identifying it as a discrete excitonic transition. We attribute this behaviour to boson-driven modulation of the dielectric response, which transiently transfers spectral weight from a nominally dark exciton into an observable channel without requiring a finite equilibrium oscillator strength. Supported by many-body calculations, we assign this feature to a higher-energy exciton with distinct momentum and orbital character and strongly suppressed optical matrix elements. These results establish excitonic resonances in van der Waals magnets as a platform for interfacing collective excitations across GHz, THz and optical frequency scales.

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.

Desk Editor's Note private letter to a colleague

The paper finds that both magnons and phonons in CrSBr create the same 1.46 eV emergent resonance with pi-phase inversion through spectral weight transfer from a dark exciton.

read the letter

The central observation is that driving either the GHz magnon or the THz phonon in CrSBr produces an identical new resonance at 1.46 eV in the transient reflectivity, with a characteristic pi phase inversion. This feature does not appear in the steady-state spectrum. The authors interpret it as transient spectral weight transfer from a nominally dark exciton into an observable channel, driven by the modulation of the dielectric response by the collective modes. This is new in showing a single excitonic platform that interfaces with collective excitations over three decades in frequency. The experiment resolves the coherent oscillations across a broad spectral window, and the shared signature for spin and lattice modes is the key result. The phase inversion helps identify it as a discrete excitonic transition rather than a continuum effect. The work is supported by many-body calculations that assign the 1.46 eV feature to a higher-energy exciton with distinct momentum and orbital character and suppressed optical matrix elements. This assignment explains why the resonance emerges only under boson driving. The main soft spot is the dependence on those calculations for the mechanism. The stress test note points out that if the matrix elements are misestimated or if other transient contributions are present, the weight transfer picture weakens. Without seeing the full data, error bars, and calculation details, it's difficult to gauge how unique this attribution is. The abstract presents the result cleanly but leaves the quantitative support for the full manuscript. This paper is for people working on van der Waals magnets, excitonics, and ultrafast spectroscopy. A specialist reader would find the experimental demonstration useful and the proposed broadband interface worth considering. It shows clear thinking on the literature and the problem. I think it deserves peer review so that referees can check the calculations and the robustness of the data against alternative explanations.

Referee Report

2 major / 1 minor

Summary. The manuscript claims that excitonic resonances in the van der Waals antiferromagnet CrSBr provide a broadband optical interface for coherent GHz magnon and THz phonon modes. Femtosecond broadband transient reflectivity reveals an emergent resonance at 1.46 eV (absent in steady-state spectra) with characteristic π-phase inversion; this is attributed to boson-driven modulation of the dielectric response that transfers spectral weight from a nominally dark higher-energy exciton (distinct momentum/orbital character, strongly suppressed matrix elements) into an observable channel, as assigned by many-body calculations.

Significance. If the central attribution holds, the result would establish excitonic resonances in van der Waals magnets as a unified platform for interfacing collective excitations across GHz–THz and optical scales without requiring equilibrium oscillator strength.

major comments (2)

[many-body calculations section] The assignment of the 1.46 eV feature and the spectral-weight-transfer mechanism rest on many-body calculations that identify a higher-energy exciton with suppressed optical matrix elements; however, the manuscript provides no details on the method, basis set, convergence, or how matrix elements were computed (abstract and main-text discussion of calculations). This is load-bearing for distinguishing the mechanism from other transient contributions such as heating or coherent population effects.
[experimental results] No quantitative experimental metrics (error bars, signal amplitudes, phase-extraction uncertainties, or fit parameters) are reported for the emergent resonance, phase inversion, or mode amplitudes (abstract and experimental-results description). This weakens assessment of whether the π-phase inversion is robust against noise or alternative explanations.

minor comments (1)

[abstract] The abstract states the resonance 'is absent in steady-state spectra' but does not specify the exact steady-state measurement conditions or spectral resolution used for this comparison.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for their careful reading of our manuscript and for the constructive comments. We address each major point below and will incorporate the requested details in the revised version.

read point-by-point responses

Referee: [many-body calculations section] The assignment of the 1.46 eV feature and the spectral-weight-transfer mechanism rest on many-body calculations that identify a higher-energy exciton with suppressed optical matrix elements; however, the manuscript provides no details on the method, basis set, convergence, or how matrix elements were computed (abstract and main-text discussion of calculations). This is load-bearing for distinguishing the mechanism from other transient contributions such as heating or coherent population effects.

Authors: We agree that the manuscript as submitted lacks sufficient methodological details on the many-body calculations. In the revised manuscript we will add a dedicated paragraph (or supplementary note) specifying the computational approach (GW+BSE), the basis set, k-point sampling, convergence criteria, and the explicit procedure used to evaluate the optical matrix elements. These additions will strengthen the distinction between the proposed spectral-weight-transfer mechanism and alternative transient contributions. revision: yes
Referee: [experimental results] No quantitative experimental metrics (error bars, signal amplitudes, phase-extraction uncertainties, or fit parameters) are reported for the emergent resonance, phase inversion, or mode amplitudes (abstract and experimental-results description). This weakens assessment of whether the π-phase inversion is robust against noise or alternative explanations.

Authors: We acknowledge that quantitative metrics were not reported in the abstract or the main-text experimental description. In the revised manuscript we will include error bars on the transient spectra, measured signal amplitudes, uncertainties associated with the phase extraction, and the fit parameters used for the coherent modes. These additions will allow a direct evaluation of the robustness of the observed π-phase inversion. revision: yes

Circularity Check

0 steps flagged

No circularity; experimental signatures and attribution remain independent of calculations

full rationale

The paper's central derivation rests on femtosecond transient reflectivity measurements that directly observe a new resonance at 1.46 eV with π-phase inversion absent from steady-state spectra. This is attributed to boson-driven dielectric modulation transferring weight from a dark exciton, with many-body calculations used only for post-hoc assignment of orbital/momentum character and matrix-element suppression. No equations, fits, or self-citations are shown that reduce the observed phase inversion or spectral-weight transfer to a fitted input or prior author result by construction. The experimental signature is presented as falsifiable independently of the supporting calculations, satisfying the criteria for a self-contained, non-circular chain.

Axiom & Free-Parameter Ledger

0 free parameters · 1 axioms · 0 invented entities

Abstract-only review provides no explicit free parameters, axioms, or invented entities; the central claim rests on standard many-body theory assumptions and the experimental identification of the resonance.

axioms (1)

domain assumption Many-body calculations can reliably assign momentum and orbital character to the higher-energy exciton responsible for the 1.46 eV feature.
Invoked to support the spectral weight transfer interpretation.

pith-pipeline@v0.9.0 · 5793 in / 1296 out tokens · 21990 ms · 2026-05-25T07:45:29.066483+00:00 · methodology

discussion (0)

Reference graph

Works this paper leans on

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Sears, J. et al. Observation of Anisotropic Dispersive Dark-Exciton Dynamics in CrSBr. Phys. Rev. Lett. 135, 146503 (2025)

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Klein, J. et al. Sensing the Local Magnetic Environment through Optically Active Defects in a Layered Magnetic Semiconductor. ACS Nano 17, 288–299 (2023)

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Smolenski, S. et al. Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization. Nat. Commun. 16, 1134 (2025)

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Klein, J. et al. The Bulk van der Waals Layered Magnet CrSBr is a Quasi-1D Material. ACS Nano 17, 5316–5328 (2023)

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Mertens, F. et al. Wide spectral range ultrafast pump-probe magneto-optical spectrometer at low temperature, high-magnetic and electric fields. Rev. Sci. Instrum. 91, 113001 (2020)

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[1] [1]

Rojas-Lopeza, Mattia Beninia, David Maximilian Janasa, Umut Parlakc, Alberto Brambillab, Alexey V

1 Magnetic Order Unlocks Optical Access to Dark Excitons in CrSBr Sophie Borka, Richard Levena, Vincent Wirsdörfera, Alessandro Ferrettib, Rafael R. Rojas-Lopeza, Mattia Beninia, David Maximilian Janasa, Umut Parlakc, Alberto Brambillab, Alexey V. Scherbakova, Mirko Cinchettia,* aDepartment of Physics, TU Dortmund University, Dortmund, Germany bDipartimen...

work page 2020

[2] [2]

Datta, B. et al. Magnon-mediated exciton–exciton interaction in a van der Waals antiferromagnet. Nat. Mater. 24, 1027–1033 (2025)

work page 2025

[3] [3]

Zhang, X.-X., You, Y., Zhao, S. Y. F. & Heinz, T. F. Experimental Evidence for Dark Excitons in 9 Monolayer WSe₂. Phys. Rev. Lett. 115, 257403 (2015)

work page 2015

[4] [4]

Chand, S. B. et al. Interaction-driven transport of dark excitons in 2D semiconductors with phonon-mediated optical readout. Nat. Commun. 14, 3712 (2023)

work page 2023

[5] [5]

Bossini, D. et al. Ultrafast Amplification and Nonlinear Magnetoelastic Coupling of Coherent Magnon Modes in an Antiferromagnet. Phys. Rev. Lett. 127, 77202 (2021)

work page 2021

[6] [6]

& Nakamura, Y

Lachance-Quirion, D., Tabuchi, Y., Gloppe, A., Usami, K. & Nakamura, Y. Hybrid quantum systems based on magnonics. Appl. Phys. Express 12, 070101 (2019)

work page 2019

[7] [7]

Gibertini, M., Koperski, M., Morpurgo, A. F. & Novoselov, K. S. Magnetic 2D materials and heterostructures. Nat. Nanotechnol. 14, 408–419 (2019)

work page 2019

[8] [8]

Gong, C. et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 546, 265–269 (2017)

work page 2017

[9] [9]

Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 546, 270–273 (2017)

work page 2017

[10] [10]

& Zhang, X

Gong, C. & Zhang, X. Two-dimensional magnetic crystals and emergent heterostructure devices. Science (80-. ). 363, eaav4450 (2019)

work page 2019

[11] [11]

Wang, G. et al. Colloquium: Excitons in atomically thin transition metal dichalcogenides. Rev. Mod. Phys. 90, 21001 (2018)

work page 2018

[12] [12]

Benini, M. et al. Light-driven modulation of proximity-enhanced functionalities in hybrid nano-scale systems. Nat. Commun. 16, 7297 (2025)

work page 2025

[13] [13]

Selig, M. et al. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides. Nat. Commun. 7, 13279 (2016)

work page 2016

[14] [14]

& Cui, X

Zhu, B., Chen, X. & Cui, X. Exciton binding energy of monolayer WS2. Sci. Rep. 5, 9218 (2015)

work page 2015

[15] [15]

& Zhang, X

Xiao, J., Zhao, M., Wang, Y. & Zhang, X. Excitons in atomically thin 2D semiconductors and their applications. Nanophotonics 6, 1309–1328 (2017)

work page 2017

[16] [16]

Barré, E. et al. Optical absorption of interlayer excitons in transition-metal dichalcogenide heterostructures. Science (80-. ). 376, 406–410 (2022)

work page 2022

[17] [17]

Madéo, J. et al. Directly visualizing the momentum-forbidden dark excitons and their dynamics in atomically thin semiconductors. Science (80-. ). 370, 1199–1204 (2020)

work page 2020

[18] [18]

Schmitt, D. et al. Ultrafast nano-imaging of dark excitons. Nat. Photonics 19, 187–194 (2025)

work page 2025

[19] [19]

Yang, K., Wang, G., Liu, L., Lu, D. & Wu, H. Triaxial magnetic anisotropy in the two-dimensional ferromagnetic semiconductor CrSBr. Phys. Rev. B 104, 144416 (2021)

work page 2021

[20] [20]

Torres, K. et al. Probing Defects and Spin-Phonon Coupling in CrSBr via Resonant Raman Scattering. Adv. Funct. Mater. 33, 2211366 (2023)

work page 2023

[21] [21]

& Ross, F

Klein, J. & Ross, F. M. Materials beyond monolayers: The magnetic quasi-1D semiconductor CrSBr. J. Mater. Res. 39, 3045–3056 (2024)

work page 2024

[22] [22]

& Kahle, H

Göser, O., Paul, W. & Kahle, H. G. Magnetic properties of CrSBr. J. Magn. Magn. Mater. 92, 129–136 (1990)

work page 1990

[23] [23]

Über Chalkogenidhalogenide des Chroms Synthese, Kristallstruktur und Magnetismus von Chromsulfidbromid, CrSBr

Beck, J. Über Chalkogenidhalogenide des Chroms Synthese, Kristallstruktur und Magnetismus von Chromsulfidbromid, CrSBr. ZAAC - J. Inorg. Gen. Chem. 585, 157–167 (1990)

work page 1990

[24] [24]

Scheie, A. et al. Spin Waves and Magnetic Exchange Hamiltonian in CrSBr. Adv. Sci. 9, 2202467 (2022)

work page 2022

[25] [25]

Liu, W. et al. A Three-Stage Magnetic Phase Transition Revealed in Ultrahigh-Quality van der Waals Bulk Magnet CrSBr. ACS Nano 16, 15917–15926 (2022)

work page 2022

[26] [26]

Telford, E. J. et al. Layered Antiferromagnetism Induces Large Negative Magnetoresistance in the van der Waals Semiconductor CrSBr. Adv. Mater. 32, 2003240 (2020)

work page 2020

[27] [27]

Wilson, N. P. et al. Interlayer electronic coupling on demand in a 2D magnetic semiconductor. Nat. Mater. 20, 1657–1662 (2021)

work page 2021

[28] [28]

Wang, T. et al. Magnetically-dressed CrSBr exciton-polaritons in ultrastrong coupling regime. Nat. Commun. 14, 5966 (2023)

work page 2023

[29] [29]

& Coronado, E

Marques-Moros, F., Boix-Constant, C., Mañas-Valero, S., Canet-Ferrer, J. & Coronado, E. Interplay between Optical Emission and Magnetism in the van der Waals Magnetic 10 Semiconductor CrSBr in the Two-Dimensional Limit. ACS Nano 17, 13224–13231 (2023)

work page 2023

[30] [30]

Meineke, C. et al. Ultrafast Exciton Dynamics in the Atomically Thin van der Waals Magnet CrSBr. Nano Lett. 24, 4101–4107 (2024)

work page 2024

[31] [31]

Bae, Y. J. et al. Exciton-coupled coherent magnons in a 2D semiconductor. Nature 609, 282–286 (2022)

work page 2022

[32] [32]

Sun, Y. et al. Dipolar spin wave packet transport in a van der Waals antiferromagnet. Nat. Phys. 20, 794–800 (2024)

work page 2024

[33] [33]

Sears, J. et al. Observation of Anisotropic Dispersive Dark-Exciton Dynamics in CrSBr. Phys. Rev. Lett. 135, 146503 (2025)

work page 2025

[34] [34]

Klein, J. et al. Sensing the Local Magnetic Environment through Optically Active Defects in a Layered Magnetic Semiconductor. ACS Nano 17, 288–299 (2023)

work page 2023

[35] [35]

Smolenski, S. et al. Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization. Nat. Commun. 16, 1134 (2025)

work page 2025

[36] [36]

Klein, J. et al. The Bulk van der Waals Layered Magnet CrSBr is a Quasi-1D Material. ACS Nano 17, 5316–5328 (2023)

work page 2023

[37] [37]

Linhart, W. M. et al. Optical markers of magnetic phase transition in CrSBr. J. Mater. Chem. C 11, 8423–8430 (2023)

work page 2023

[38] [38]

Afanasiev, D. et al. Controlling the anisotropy of a van der Waals antiferromagnet with light. Sci. Adv. 7, eabf3096 (2021)

work page 2021

[39] [39]

Mertens, F. et al. Wide spectral range ultrafast pump-probe magneto-optical spectrometer at low temperature, high-magnetic and electric fields. Rev. Sci. Instrum. 91, 113001 (2020)

work page 2020

[40] [40]

Adv. Mater. 35, 2208355 (2023)

work page 2023