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<p>Excitons in recently discovered two-dimensional magnetic semiconductors have emerged as a promising vehicle for optoelectronic and spin-photonic applications. To exploit novel possibilities magnetic degrees of freedom offer, insight into the interplay of magnetism, lattice and optical excitations becomes essential. We consider Chromium Sulphur Bromide, which has two kinds of excitons, X<sub>B</sub> at 1.8 eV and X<sub>A</sub> at 1.38 eV. Here we show, through a combination of many body perturbation theory and experiment, that X<sub>B</sub> is an order of magnitude more sensitive to magnetic and lattice perturbations than X<sub>A</sub>. We trace the difference to the latter being localised (Frenkel-like), while the former is delocalised (Wannier-Mott-like) – a coexistence rarely seen in two-dimensional materials. This finding is supported by the strong temperature and magnetic field (up to 85 Tesla) dependent shifts in optical response for X<sub>B</sub> (much smaller for X<sub>A</sub>), and we show it is related to X<sub>B</sub>’s tendency for delocalisation (in-plane and out-of-plane) and enhanced coupling with A<i>g</i> phonon modes.</p>

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Distinct magneto-optical response of Frenkel and Wannier excitons in CrSBr

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月17日

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  • Maciej Śmiertka,
  • Michał Rygała,
  • Katarzyna Posmyk,
  • Paulina Peksa,
  • Mateusz Dyksik,
  • Dimitar Pashov,
  • Kseniia Mosina,
  • Zdeněk Sofer,
  • Mark van Schilfgaarde,
  • Florian Dirnberger,
  • Michał Baranowski,
  • Swagata Acharya,
  • Paulina Plochocka

摘要

Excitons in recently discovered two-dimensional magnetic semiconductors have emerged as a promising vehicle for optoelectronic and spin-photonic applications. To exploit novel possibilities magnetic degrees of freedom offer, insight into the interplay of magnetism, lattice and optical excitations becomes essential. We consider Chromium Sulphur Bromide, which has two kinds of excitons, XB at 1.8 eV and XA at 1.38 eV. Here we show, through a combination of many body perturbation theory and experiment, that XB is an order of magnitude more sensitive to magnetic and lattice perturbations than XA. We trace the difference to the latter being localised (Frenkel-like), while the former is delocalised (Wannier-Mott-like) – a coexistence rarely seen in two-dimensional materials. This finding is supported by the strong temperature and magnetic field (up to 85 Tesla) dependent shifts in optical response for XB (much smaller for XA), and we show it is related to XB’s tendency for delocalisation (in-plane and out-of-plane) and enhanced coupling with Ag phonon modes.