Light-induced ultrafast dynamics in two-dimensional (2D) magnetic systems demonstrate substantial advancements in spintronics. Here, using the real-time time-dependent density functional theory (rt-TDDFT), we applied laser pulses with various frequencies, from terahertz (THz) to optical pulse, to systematically study the interlayer spin transfer dynamics in 2D van der Waals nonmagnetic-ferromagnetic heterostructures, including graphene-Fe3GeTe2 (Gr/FGT) and silicene-Fe3GeTe2 (Si/FGT). Our results demonstrate that low-frequency THz pulses are particularly effective in facilitating interlayer spin injection from the ferromagnetic FGT layers to the Si or Gr layers. On the contrary, high-frequency optical pulses exhibit a minimal influence on this process. Such an effect is attributed to the low-frequency THz pulses inducing in-phase oscillations of the electron charge density around atomic centers, leading to a highly efficient interlayer spin transfer. Our results provide a new insight into ultrafast THz radiation control intralayer spin transfer and magnetic proximity dynamics in the 2D limit.

Department of Physical and Macromolecular Chemistry Faculty of Science Charles University Prague 12843 Czech Republic

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Sander D; Valenzuela S O; Makarov D; Marrows C H; Fullerton E E; Fischer P; McCord J; Vavassori P; Mangin S; Pirro P; Hillebrands B; Kent A D; Jungwirth T; Gutfleisch O; Kim C G; Berger A The 2017 magnetism roadmap. J. Phys. D: Appl. Phys. 2017, 50 (36), 36300110.1088/1361-6463/aa81a1. DOI

Vedmedenko E Y; Kawakami R K; Sheka D D; Gambardella P; Kirilyuk A; Hirohata A; Binek C; Chubykalo-Fesenko O; Sanvito S; Kirby B J; Grollier J; Everschor-Sitte K; Kampfrath T; You C-Y; Berger A The 2020 magnetism roadmap. J. Phys. D: Appl. Phys. 2020, 53 (45), 45300110.1088/1361-6463/ab9d98. DOI

Beaurepaire E.; Merle J. C.; Daunois A.; Bigot J. Y. Ultrafast Spin Dynamics in Ferromagnetic Nickel. Phys. Rev. Lett. 1996, 76 (22), 4250–4253. 10.1103/PhysRevLett.76.4250. PubMed DOI

Koopmans B.; van Kampen M.; Kohlhepp J. T.; de Jonge W. J. M. Ultrafast Magneto-Optics in Nickel: Magnetism or Optics?. Phys. Rev. Lett. 2000, 85 (4), 844–847. 10.1103/PhysRevLett.85.844. PubMed DOI

Kirilyuk A.; Kimel A. V.; Rasing T. Ultrafast optical manipulation of magnetic order. Rev. Mod. Phys. 2010, 82 (3), 2731–2784. 10.1103/RevModPhys.82.2731. DOI

Kampfrath T.; Tanaka K.; Nelson K. A. Resonant and nonresonant control over matter and light by intense terahertz transients. Nat. Photonics 2013, 7 (9), 680–690. 10.1038/nphoton.2013.184. DOI

Vicario C.; Ruchert C.; Ardana-Lamas F.; Derlet P. M.; Tudu B.; Luning J.; Hauri C. P. Off-resonant magnetization dynamics phase-locked to an intense phase-stable terahertz transient. Nat. Photonics 2013, 7 (9), 720–723. 10.1038/nphoton.2013.209. DOI

Shalaby M.; Donges A.; Carva K.; Allenspach R.; Oppeneer P. M.; Nowak U.; Hauri C. P. Coherent and incoherent ultrafast magnetization dynamics in 3d ferromagnets driven by extreme terahertz fields. Phys. Rev. B 2018, 98 (1), 01440510.1103/PhysRevB.98.014405. DOI

Lee H.; Weber C.; Fähnle M.; Shalaby M. Ultrafast Electron Dynamics in Magnetic Thin Films. Appl. Sci. 2021, 11 (20), 9753.10.3390/app11209753. DOI

Huang B.; Clark G.; Navarro-Moratalla E.; Klein D. R.; Cheng R.; Seyler K. L.; Zhong D.; Schmidgall E.; McGuire M. A.; Cobden D. H.; Yao W.; Xiao D.; Jarillo-Herrero P.; Xu X. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 2017, 546 (7657), 270–273. 10.1038/nature22391. PubMed DOI

Gong C.; Li L.; Li Z.; Ji H.; Stern A.; Xia Y.; Cao T.; Bao W.; Wang C.; Wang Y.; Qiu Z. Q.; Cava R. J.; Louie S. G.; Xia J.; Zhang X. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 2017, 546 (7657), 265–269. 10.1038/nature22060. PubMed DOI

Deng Y.; Yu Y.; Song Y.; Zhang J.; Wang N. Z.; Sun Z.; Yi Y.; Wu Y. Z.; Wu S.; Zhu J.; Wang J.; Chen X. H.; Zhang Y. Gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2. Nature 2018, 563 (7729), 94–99. 10.1038/s41586-018-0626-9. PubMed DOI

Fei Z.; Huang B.; Malinowski P.; Wang W.; Song T.; Sanchez J.; Yao W.; Xiao D.; Zhu X.; May A. F.; Wu W.; Cobden D. H.; Chu J.-H.; Xu X. Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2. Nat. Mater. 2018, 17 (9), 778–782. 10.1038/s41563-018-0149-7. PubMed DOI

Bonilla M.; Kolekar S.; Ma Y.; Diaz H. C.; Kalappattil V.; Das R.; Eggers T.; Gutierrez H. R.; Phan M.-H.; Batzill M. Strong room-temperature ferromagnetism in VSe2 monolayers on van der Waals substrates. Nat. Nanotechnol. 2018, 13 (4), 289–293. 10.1038/s41565-018-0063-9. PubMed DOI

Liu B.; Liu S.; Yang L.; Chen Z.; Zhang E.; Li Z.; Wu J.; Ruan X.; Xiu F.; Liu W.; et al. Light-Tunable Ferromagnetism in Atomically Thin Fe3GeTe2 Driven by Femtosecond Laser Pulse. Phys. Rev. Lett. 2020, 125 (26), 26720510.1103/PhysRevLett.125.267205. PubMed DOI

Zhang P.; Chung T.-F.; Li Q.; Wang S.; Wang Q.; Huey W. L.; Yang S.; Goldberger J. E.; Yao J.; Zhang X. All-optical switching of magnetization in atomically thin CrI3. Nat. Mater. 2022, 21 (12), 1373–1378. 10.1038/s41563-022-01354-7. PubMed DOI

Liu Y.; Huang Y.; Duan X. Van der Waals integration before and beyond two-dimensional materials. Nature 2019, 567 (7748), 323–333. 10.1038/s41586-019-1013-x. PubMed DOI

Gibertini M.; Koperski M.; Morpurgo A. F.; Novoselov K. S. Magnetic 2D materials and heterostructures. Nat. Nanotechnol. 2019, 14 (5), 408–419. 10.1038/s41565-019-0438-6. PubMed DOI

Alghamdi M.; Lohmann M.; Li J.; Jothi P. R.; Shao Q.; Aldosary M.; Su T.; Fokwa B. P.; Shi J. Highly efficient spin–orbit torque and switching of layered ferromagnet Fe3GeTe2. Nano Lett. 2019, 19 (7), 4400–4405. 10.1021/acs.nanolett.9b01043. PubMed DOI

Wang X.; Tang J.; Xia X.; He C.; Zhang J.; Liu Y.; Wan C.; Fang C.; Guo C.; Yang W.; Guang Y.; Zhang X.; Xu H.; Wei J.; Liao M.; Lu X.; Feng J.; Li X.; Peng Y.; Wei H.; Yang R.; Shi D.; Zhang X.; Han Z.; Zhang Z.; Zhang G.; Yu G.; Han X. Current-driven magnetization switching in a van der Waals ferromagnet Fe3GeTe2. Sci. Adv. 2019, 5 (8), eaaw890410.1126/sciadv.aaw8904. PubMed DOI PMC

Albarakati S.; Tan C.; Chen Z.-J.; Partridge J. G.; Zheng G.; Farrar L.; Mayes E. L. H.; Field M. R.; Lee C.; Wang Y.; Xiong Y.; Tian M.; Xiang F.; Hamilton A. R.; Tretiakov O. A.; Culcer D.; Zhao Y.-J.; Wang L. Antisymmetric magnetoresistance in van der Waals Fe3GeTe2/graphite/Fe3GeTe2 trilayer heterostructures. Sci. Adv. 2019, 5 (7), eaaw040910.1126/sciadv.aaw0409. PubMed DOI PMC

Shen Z.-X.; Bo X.; Cao K.; Wan X.; He L. Magnetic ground state and electron-doping tuning of Curie temperature in Fe3GeTe2: First-principles studies. Phys. Rev. B 2021, 103 (8), 08510210.1103/PhysRevB.103.085102. DOI

Niu W.; Cao Z.; Wang Y.; Wu Z.; Zhang X.; Han W.; Wei L.; Wang L.; Xu Y.; Zou Y.; et al. Antisymmetric magnetoresistance in Fe3GeTe2 nanodevices of inhomogeneous thickness. Phys. Rev. B 2021, 104 (12), 12542910.1103/PhysRevB.104.125429. DOI

Seyler K. L.; Zhong D.; Huang B.; Linpeng X.; Wilson N. P.; Taniguchi T.; Watanabe K.; Yao W.; Xiao D.; McGuire M. A.; Fu K.-M. C.; Xu X. Valley manipulation by optically tuning the magnetic proximity effect in WSe2/CrI3 heterostructures. Nano Lett. 2018, 18 (6), 3823–3828. 10.1021/acs.nanolett.8b01105. PubMed DOI

Dewhurst J. K.; Elliott P.; Shallcross S.; Gross E. K. U.; Sharma S. Laser-Induced Intersite Spin Transfer. Nano Lett. 2018, 18 (3), 1842–1848. 10.1021/acs.nanolett.7b05118. PubMed DOI

Siegrist F.; Gessner J. A.; Ossiander M.; Denker C.; Chang Y.-P.; Schroder M. C.; Guggenmos A.; Cui Y.; Walowski J.; Martens U.; Dewhurst J. K.; Kleineberg U.; Munzenberg M.; Sharma S.; Schultze M. Light-wave dynamic control of magnetism. Nature 2019, 571 (7764), 240–244. 10.1038/s41586-019-1333-x. PubMed DOI

Steil D.; Walowski J.; Gerhard F.; Kiessling T.; Ebke D.; Thomas A.; Kubota T.; Oogane M.; Ando Y.; Otto J.; Mann A.; Hofherr M.; Elliott P.; Dewhurst J. K.; Reiss G.; Molenkamp L.; Aeschlimann M.; Cinchetti M.; Munzenberg M.; Sharma S.; Mathias S. Efficiency of ultrafast optically induced spin transfer in Heusler compounds. Phys. Rev. Res. 2020, 2 (2), 02319910.1103/PhysRevResearch.2.023199. DOI

Willems F.; von Korff Schmising C.; Struber C.; Schick D.; Engel D. W.; Dewhurst J. K.; Elliott P.; Sharma S.; Eisebitt S. Optical inter-site spin transfer probed by energy and spin-resolved transient absorption spectroscopy. Nat. Commun. 2020, 11 (1), 871.10.1038/s41467-020-14691-5. PubMed DOI PMC

Hofherr M.; Hauser S.; Dewhurst J. K.; Tengdin P.; Sakshath S.; Nembach H. T.; Weber S. T.; Shaw J. M.; Silva T. J.; Kapteyn H. C.; Cinchetti M.; Rethfeld B.; Murnane M. M.; Steil D.; Stadtmuller B.; Sharma S.; Aeschlimann M.; Mathias S. Ultrafast optically induced spin transfer in ferromagnetic alloys. Sci. Adv. 2020, 6 (3), eaay871710.1126/sciadv.aay8717. PubMed DOI PMC

Tengdin P.; Gentry C.; Blonsky A.; Zusin D.; Gerrity M.; Hellbruck L.; Hofherr M.; Shaw J.; Kvashnin Y.; Delczeg-Czirjak E. K.; Arora M.; Nembach H.; Silva T. J.; Mathias S.; Aeschlimann M.; Kapteyn H. C.; Thonig D.; Koumpouras K.; Eriksson O.; Murnane M. M. Direct light–induced spin transfer between different elements in a spintronic Heusler material via femtosecond laser excitation. Sci. Adv. 2020, 6 (3), eaaz110010.1126/sciadv.aaz1100. PubMed DOI PMC

He J.; Li S.; Bandyopadhyay A.; Frauenheim T. Unravelling Photoinduced Interlayer Spin Transfer Dynamics in Two-Dimensional Nonmagnetic-Ferromagnetic van der Waals Heterostructures. Nano Lett. 2021, 21 (7), 3237–3244. 10.1021/acs.nanolett.1c00520. PubMed DOI

He J.; Li S.; Zhou L.; Frauenheim T. Ultrafast Light-Induced Ferromagnetic State in Transition Metal Dichalcogenides Monolayers. J. Phys. Chem. Lett. 2022, 13 (12), 2765–2771. 10.1021/acs.jpclett.2c00443. PubMed DOI

Chen H.; Li B.; Yang J. Proximity effect induced spin injection in phosphorene on magnetic insulator. ACS Appl. Mater. Interfaces 2017, 9 (44), 38999–39010. 10.1021/acsami.7b11454. PubMed DOI

Dewhurst J. K. S. S.; et al.Elk code. elk.sourceforge.net (accessed Oct 1, 2020).

Dewhurst J.; Shallcross S.; Gross E.; Sharma S. Substrate-controlled ultrafast spin injection and demagnetization. Phys. Rev. Appl. 2018, 10 (4), 04406510.1103/PhysRevApplied.10.044065. DOI

Chen J.; Bovensiepen U.; Eschenlohr A.; Müller T.; Elliott P.; Gross E.; Dewhurst J.; Sharma S. Competing spin transfer and dissipation at Co/Cu (001) interfaces on femtosecond timescales. Phys. Rev. Lett. 2019, 122, 06720210.1103/PhysRevLett.122.067202. PubMed DOI

Pellegrini C.; Sharma S.; Dewhurst J. K.; Sanna A. Ab initio study of ultrafast demagnetization of elementary ferromagnets by terahertz versus optical pulses. Phys. Rev. B 2022, 105 (13), 13442510.1103/PhysRevB.105.134425. DOI

Wang K.; Ren K.; Hou Y.; Cheng Y.; Zhang G. Physical insights into enhancing magnetic stability of 2D magnets. J. Appl. Phys. 2023, 133 (11), 11090210.1063/5.0135908. DOI

Optical-Helicity-Dependent Orbital and Spin Dynamics in Two-Dimensional Ferromagnets