journal article·2026-05-01

Field-resolved observation of exciton coherence in a van der Waals magnet

Matthew Yeung, Alexander von Hoegen, Emil Viñas Boström, Fangzhou Zhao, Felix Ritzkowsky, Jack B. Maier, Gian Luca Dolso, Christian Heide, Daniel G. Chica, Xavier Roy, Karl K. Berggren, Angel Rubio, Phillip D. Keathley, Nuh Gedik

Publisher page

Abstract

The emergence of coherence among electronic quasiparticles underlies collective quantum phenomena from superconductivity to superradiance. In semiconductors, exciton coherence is generally thought to decay rapidly due to scattering and dephasing, limiting its persistence on ultrafast timescales. Here we demonstrate a light-field-driven mechanism that creates and stabilizes exciton coherence in the layered antiferromagnet CrSBr. We directly record the coherent optical field emitted by excitons and track in real time how a deterministic phase, imprinted by the excitation laser, drives incoherent excitons to synchronize into a collective state. This ensemble remains phase coherent for more than 2 ps, whereas its resonance energy undergoes an ultrafast modulation mediated by spin and lattice interactions. The time-resolved field evolution indicates that the multiple peaks seen in conventional spectra originate from a single excitonic resonance subject to dynamic energy modulation. Our findings establish optical phase imprinting as a mechanism to control and sustain collective order in semiconducting magnets, bridging light-driven dynamics with excitonic and magnetic correlations in layered quantum materials.
Source: europepmc · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Chemical and Physical Properties of Materials · 2D Materials and Applications · Electronic and Structural Properties of Oxides

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (59)

Show source-provided references
1. Strogatz, S. H. From Kuramoto to Crawford: exploring the onset of synchronization in populations of coupled oscillators. Phys. D 143, 1–20 (2000).10.1016/S0167-2789(00)00094-4 ↗
2. Bardeen, J., Cooper, L. N. & Schrieffer, J. R. Theory of superconductivity. Phys. Rev. 108, 1175–1204 (1957).10.1103/PhysRev.108.1175 ↗
3. van Delft, D. & Kes, P. The discovery of superconductivity. Phys. Today 63, 38–43 (2010).10.1063/1.3490499 ↗
4. Anderson, M. H., Ensher, J. R., Matthews, M. R., Wieman, C. E. & Cornell, E. A. Observation of Bose-Einstein condensation in a dilute atomic vapor. Science 269, 198–201 (1995).10.1126/science.269.5221.198 ↗
5. Dicke, R. H. Coherence in spontaneous radiation processes. Phys. Rev. 93, 99–110 (1954).10.1103/PhysRev.93.99 ↗
6. Burnham, D. C. & Chiao, R. Y. Coherent resonance fluorescence excited by short light pulses. Phys. Rev. 188, 667–675 (1969).10.1103/PhysRev.188.667 ↗
7. Bonifacio, R. & Lugiato, L. A. Cooperative radiation processes in two-level systems: superfluorescence. Phys. Rev. A 11, 1507–1521 (1975).10.1103/PhysRevA.11.1507 ↗
8. Heinzen, D. J., Thomas, J. E. & Feld, M. S. Coherent ringing in superfluorescence. Phys. Rev. Lett. 54, 677–680 (1985).10.1103/PhysRevLett.54.677 ↗
9. Rainò, G. et al. Superfluorescence from lead halide perovskite quantum dot superlattices. Nature 563, 671–675 (2018).10.1038/s41586-018-0683-0 ↗
10. Biliroglu, M. et al. Unconventional solitonic high-temperature superfluorescence from perovskites. Nature 642, 71–77 (2025).10.1038/s41586-025-09030-x ↗
11. Mueller, T. & Malic, E. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors. npj 2D Mater. Appl. 2, 29 (2018).10.1038/s41699-018-0074-2 ↗
12. Selig, M. et al. Dark and bright exciton formation, thermalization, and photoluminescence in monolayer transition metal dichalcogenides. 2D Mater. 5, 035017 (2018).10.1088/2053-1583/aabea3 ↗
13. Jakubczyk, T. et al. Radiatively limited dephasing and exciton dynamics in MoSe2 monolayers revealed with four-wave mixing microscopy. Nano Lett. 16, 5333–5339 (2016).10.1021/acs.nanolett.6b01060 ↗
14. Martin, E. W. et al. Encapsulation narrows and preserves the excitonic homogeneous linewidth of exfoliated monolayer MoSe2. Phys. Rev. Appl.14, 021002 (2020).10.1103/PhysRevApplied.14.021002 ↗
15. Siday, T. et al. Ultrafast nanoscopy of high-density exciton phases in WSe2. Nano Lett. 22, 2561–2568 (2022).10.1021/acs.nanolett.1c04741 ↗
16. Meineke, C. et al. Ultrafast exciton dynamics in the atomically thin van der Waals magnet CrSBr. Nano Lett. 24, 4101–4107 (2024).10.1021/acs.nanolett.3c05010 ↗
17. Steinleitner, P. et al. Direct observation of ultrafast exciton formation in a monolayer of WSe2. Nano Lett. 17, 1455–1460 (2017).10.1021/acs.nanolett.6b04422 ↗
18. Merkl, P. et al. Ultrafast transition between exciton phases in van der Waals heterostructures. Nat. Mater. 18, 691–696 (2019).10.1038/s41563-019-0337-0 ↗
19. Liebich, M. et al. Controlling Coulomb correlations and fine structure of quasi-one-dimensional excitons by magnetic order. Nat. Mater. 24, 384–390 (2025).10.1038/s41563-025-02120-1 ↗
20. Cundiff, S. T. Coherent spectroscopy of semiconductors. Opt. Express 16, 4639–4664 (2008).10.1364/OE.16.004639 ↗
21. Rather, S. R., Weingartz, N. P., Kromer, S., Castellano, F. N. & Chen, L. X. Spin–vibronic coherence drives singlet–triplet conversion. Nature 620, 776–781 (2023).10.1038/s41586-023-06233-y ↗
22. Timmer, D. et al. Ultrafast coherent exciton couplings and many-body interactions in monolayer WS2. Nano Lett. 24, 8117–8125 (2024).10.1021/acs.nanolett.4c01991 ↗
23. Schiffrin, A. et al. Optical-field-induced current in dielectrics. Nature 493, 70–74 (2013).10.1038/nature11567 ↗
24. Schultze, M. et al. Controlling dielectrics with the electric field of light. Nature 493, 75–78 (2013).10.1038/nature11720 ↗
25. Keiber, S. et al. Electro-optic sampling of near-infrared waveforms. Nat. Photon. 10, 159–162 (2016).10.1038/nphoton.2015.269 ↗
26. Park, S. B. et al. Direct sampling of a light wave in air. Optica 5, 402–408 (2018).10.1364/OPTICA.5.000402 ↗
27. Bionta, M. R. et al. On-chip sampling of optical fields with attosecond resolution. Nat. Photon. 15, 456–460 (2021).10.1038/s41566-021-00792-0 ↗
28. Liu, Y., Beetar, J. E., Nesper, J., Gholam-Mirzaei, S. & Chini, M. Single-shot measurement of few-cycle optical waveforms on a chip. Nat. Photon. 16, 109–112 (2022).10.1038/s41566-021-00924-6 ↗
29. Ridente, E. et al. Electro-optic characterization of synthesized infrared-visible light fields. Nat. Commun. 13, 1111 (2022).10.1038/s41467-022-28699-6 ↗
30. Blöchl, J. et al. Spatiotemporal sampling of near-petahertz vortex fields. Optica 9, 755–761 (2022).10.1364/OPTICA.459612 ↗
31. Altwaijry, N. et al. Broadband photoconductive sampling in gallium phosphide. Adv. Opt. Mater. 11, 2202994 (2023).10.1002/adom.202202994 ↗
32. Yeung, M. et al. Lightwave-electronic harmonic frequency mixing. Sci. Adv.10, eadq0642 (2024).10.1126/sciadv.adq0642 ↗
33. Srivastava, A. et al. Near-petahertz fieldoscopy of liquid. Nat. Photon. 18, 1320–1326 (2024).10.1038/s41566-024-01548-2 ↗
34. Yeung, M. et al. Bandwidth of lightwave-driven electronic response from metallic nanoantennas. Nano Lett. 25, 5250–5257 (2025).10.1021/acs.nanolett.4c06536 ↗
35. Heinzerling, A. M. et al. Field-resolved attosecond solitons. Nat. Photon. 19, 772–777 (2025).10.1038/s41566-025-01658-5 ↗
36. Telford, E. J. et al. Layered antiferromagnetism induces large negative magnetoresistance in the van der Waals semiconductor CrSBr. Adv. Mater. 32, 2003240 (2020).10.1002/adma.202003240 ↗
37. Lin, K. et al. Strong exciton–phonon coupling as a fingerprint of magnetic ordering in van der Waals layered CrSBr. ACS Nano 18, 2898–2905 (2024).10.1021/acsnano.3c07236 ↗
38. Wilson, N. P. et al. Interlayer electronic coupling on demand in a 2D magnetic semiconductor. Nat. Mater. 20, 1657–1662 (2021).10.1038/s41563-021-01070-8 ↗
39. Bae, Y. J. et al. Exciton-coupled coherent magnons in a 2D semiconductor. Nature 609, 282–286 (2022).10.1038/s41586-022-05024-1 ↗
40. 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 semiconductor CrSBr in the two-dimensional limit. ACS Nano 17, 13224–13231 (2023).10.1021/acsnano.3c00375 ↗
41. Shao, Y. et al. Magnetically confined surface and bulk excitons in a layered antiferromagnet. Nat. Mater. 24, 391–398 (2025).10.1038/s41563-025-02129-6 ↗
42. Dirnberger, F. et al. Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons. Nature 620, 533–537 (2023).10.1038/s41586-023-06275-2 ↗
43. Li, C. et al. 2D CrSBr enables magnetically controllable exciton-polaritons in an open cavity. Adv. Funct. Mater. 34, 2411589 (2024).10.1002/adfm.202411589 ↗
44. Ziebel, M. E. et al. CrSBr: an air-stable, two-dimensional magnetic semiconductor. Nano Lett. 24, 4319–4329 (2024).10.1021/acs.nanolett.4c00624 ↗
45. Datta, B. et al. Magnon-mediated exciton–exciton interaction in a van der Waals antiferromagnet. Nat. Mater. 24, 1027–1033 (2025).10.1038/s41563-025-02183-0 ↗
46. 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).10.1038/s41467-025-56457-x ↗
47. Yeung, M. Lightwave Electronics Based on Nanoantenna Networks. PhD thesis, Massachusetts Institute of Technology (2024).
48. Göser, O., Paul, W. & Kahle, H. G. Magnetic properties of CrSBr. J. Magn. Magn. Mater. 92, 129–136 (1990).10.1016/0304-8853(90)90689-N ↗
49. Klein, J. et al. The bulk van der Waals layered magnet CrSBr is a quasi-1D material. ACS Nano 17, 5316–5328 (2023).10.1021/acsnano.2c07316 ↗
50. López-Paz, S. A. et al. Dynamic magnetic crossover at the origin of the hidden-order in van der Waals antiferromagnet CrSBr. Nat. Commun. 13, 4745 (2022).10.1038/s41467-022-32290-4 ↗
51. Adak, P. C. et al. Directional flow of confined polaritons in CrSBr. Adv. Mater. 37, e12557 (2025).10.1002/adma.202512557 ↗
52. Ritzkowsky, F. et al. High-repetition-rate CEP-stable 2 μm optical parametric amplifier. J. Opt. Soc. Am. B 43, 207–212 (2026).10.1364/JOSAB.580422 ↗
53. Scheie, A. et al. Spin waves in the magnetic semiconductor CrSBr. Adv. Sci. 25, 2202467 (2022).10.1002/advs.202202467 ↗
54. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).10.1103/PhysRevLett.77.3865 ↗
55. Giannozzi, P. et al. QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials. J. Phys. Condens. Matter 21, 395502 (2009).10.1088/0953-8984/21/39/395502 ↗
56. Deslippe, J. et al. BerkeleyGW: a massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures. Comput. Phys. Commun. 183, 1269–1289 (2012).10.1016/j.cpc.2011.12.006 ↗
57. Hybertsen, M. S. & Louie, S. G. Electron correlation in semiconductors and insulators: band gaps and quasiparticle energies. Phys. Rev. B 34, 5390–5413 (1986).10.1103/PhysRevB.34.5390 ↗
58. Rohlfing, M. & Louie, S. G. Electron-hole excitations and optical spectra from first principles. Phys. Rev. B 62, 4927–4944 (2000).10.1103/PhysRevB.62.4927 ↗
59. Tabataba-Vakili, F. et al. Doping-control of excitons and magnetism in CrSBr. Nat. Commun. 15, 4735 (2024).10.1038/s41467-024-49048-9 ↗