Dispersive Dark Excitons in van der Waals Ferromagnet CrI3

He, Wei; Sears, J.; Barantani, F.; Kim, T.; Villanova, Jack W.; Berlijn, Tom; Lajer, M.; McGuire, Michael A.; Pelliciari, J.; Bisogni, Valentina; Johnston, Steve; Baldini, Edoardo; Mitrano, Matteo; Dean, Mark P. M.

doi:10.1103/physrevx.15.011042

Dispersive Dark Excitons in van der Waals Ferromagnet CrI₃

Journal Article · Tue Feb 25 00:00:00 EST 2025 · Physical Review. X

DOI:https://doi.org/10.1103/physrevx.15.011042· OSTI ID:2530879

^[1]; ^[2]; ^[3]; Kim, T. ^[2]; Villanova, Jack W. ^[4]; ^[4]; ^[2]; ^[4]; ^[2]; ^[2]; ^[5]; ^[3]; ^[6]; ^[2]

Brookhaven National Laboratory (BNL), Upton, NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Univ. of Texas, Austin, TX (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Harvard Univ., Cambridge, MA (United States)

Spin-flip dark excitons are optical-dipole-forbidden quasiparticles with remarkable potential in optoelectronics, especially when they are realized within cleavable van der Waals materials. Despite this potential, dark excitons have not yet been definitively identified in ferromagnetic van der Waals materials. Here, we report two dark excitons in a model ferromagnetic material CrI₃ using high-resolution resonant inelastic x-ray scattering and show that they feature narrower linewidths compared to the bright excitons previously reported in this material. These excitons are shown to have spin-flip character, to disperse as a function of momentum, and to change through the ferromagnetic transition temperature. Given the versatility of van der Waals materials, these excitons hold promise for new types of magneto-optical functionality.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); Swiss National Science Foundation (SNSF); US Army Research Office (ARO); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725; SC0012704; SC0022311

OSTI ID:: 2530879

Alternate ID(s):: OSTI ID: 2575269

Report Number(s):: BNL--227681-2025-JAAM

Journal Information:: Physical Review. X, Journal Name: Physical Review. X Journal Issue: 1 Vol. 15; ISSN 2160-3308

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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