A04 - Ultrafast spin dynamics combined with nuclear dynamics in 2D and 3D
One of the most significant impediments to understand ultrafast spin-manipulation is that the experimentalists’ tools of choice – time-resolved magneto-optical Kerr effect (MOKE), magnetic circular dichroism (MCD), and angle-resolved photoemission spectroscopy (ARPES) - remain beyond the reach of ab-initio simulations for solids. A direct comparison between theory and experiment, the bedrock of progress in other branches of solid state physics, is therefore absent in the field of ultrafast spin manipulation. This project aims to rectify this by (i) developing an ab-initio theory of these experimental techniques, i.e., a theory of time-resolved MOKE, MCD, as well as a working theory for time-resolved (AR)PES and (ii) implementing this theory in a state-of-the-art time-dependent density functional theory (TDDFT) code. With these tools in hand the project then aims, in close collaboration with experiments, to (iii) elucidate the underlying physical mechanisms behind the ultrafast dynamics of spin and charge and, (iv), study and design new materials such as ferromagnetic/anti-ferromagnetic (FM/AFM), anti-ferromagnetic/non-magnetic (AFM/NM) and FM/NM interfaces with a view to control spin by light.
Publications (2nd Funding Period 2022 - 2025)
- Kohn-Sham-Proca equations for ultrafast exciton dynamics
J. K. Dewhurst, D. Gill, S. Shallcross, and S. Sharma
Phys. Rev. B 111, L060302 (2025) - DOI: 10.1103/PhysRevB.111.L060302
- Creation and control of valley currents in graphene by few cycle light pulses
D. Gill, S. Sharma, J. K. Dewhurst and S. Shallcross
npj Comput. Mater. 11, 185 (2025)- DOI: 10.1038/s41524-025-01689-0
- Pure spin currents via antisymmetric light
D. Gill, S. Sharma, and S. Shallcross
Nano Lett. 25, 25, 9913-9917 (2025) - DOI: 10.1021/acs.nanolett.5c00637
- Ultrafast all-optical generation of pure spin and valley currents
D. Gill, S. Sharma, J. K. Dewhurst and S. Shallcross
npj 2D Mater Appl 9, 49 (2025) - DOI: 10.1038/s41699-025-00558-0
- Combining THz and infrared light to control valley charge and current in gapless graphene
S. Sharma, D. Gill, J. Krishna, J.K. Dewhurst, P. Elliott, and S. Shallcross
Nano Lett. 25, 3791–3798 (2025) - DOI: 10.1021/acs.nanolett.4c05487
- Partially deorbitalized meta-GGA
P. Bonfà, S. Sharma, and J. K. Dewhurst
Comput. Mater. Today 1, 100002 (2024) - DOI: 10.1016/j.commt.2024.100002
- Spin dynamics across metallic layers at the few-femtosecond timescale
R. Géneaux, H.-T. Chang, A. Guggenmos, R. Delaunay,. F. Legare, K. Legare, J. Lüning, T. Parpiiev, I. J. Porter, B. R. Roulet, M. W. Zuerch, S. Sharma, M. Schultze, and S. R. Leone
Phys. Rev. Lett 133, 106902 (2024) - DOI: 10.1103/PhysRevLett.133.106902
- Spin vacuum switching
E. I. Harris-Lee, J. K. Dewhurst, S. Shallcross, and S. Sharma
Sci. Adv. 10, eado6390 (2024) - DOI: 10.1126/sciadv.ado6390
- Verification of ultrafast spin transfer effects in iron-nickel alloys
C. Möller, H. Probst, G. S. M. Jansen, M. Schumacher, M. Brede, J. K. Dewhurst, M. Reutzel, D. Steil, S. Sharma, and S. Mathias
Commun. Phys. 7: 74 (2024) - DOI: 10.1038/s42005-024-01555-3
- Unraveling femtosecond spin and charge dynamics with extreme ultraviolet transverse MOKE spectroscopy
H. Probst, C. Möller, M. Schumacher, T. Brede, J. K. Dewhurst, M. Reutzel, D. Steil, S. Sharma, G. S. M. Jansen, and S. Mathias
Phys. Rev. Res. 6, 013107 (2024) - DOI: 10.1103/PhysRevResearch.6.013107
- Direct coupling of light to valley current
S. Sharma, D. Gill, J. Krishna, J. K. Dewhurst, and S. Shallcross
Nat. Commun. 15, 7579 (2024) - DOI: 10.1038/s41467-024-51968-5
- Applicability and breakdown of transient magnetic linear dichroism
E. I. Harris-Lee, J. K. Dewhurst, P. Elliott, S. Shallcross, and S. Sharma
Phys. Rev. B 108, L100303 (2023) - DOI: 10.1103/PhysRevB.108.L100303
- Ultrafast and terahertz spintronics: Guest editorial
T. Kampfrath, A. Kirilyuk, S. Mangin, S. Sharma, and M. Weinelt
Appl. Phys. Lett. 123, 050401 (2023) - DOI:10.1063/5.0167151
- Ultrafast laser-induced magneto-optical changes in resonant magnetic x-ray reflectivity
I. Kumberg, E. Golias, S. E. Hadjadj, R. Hosseinifar, S. Thakur, T. Shinwari, I. Gelen, N. Pontius, C. Schüßler-Langeheine, C. von Korff Schmising, S. Sharma, and W. Kuch
Phys. Rev. B 108, 054439 (2023) - DOI: 10.1103/PhysRevB.108.054439
- Light-shaping of valley states
S. Sharma, J. K. Dewhurst, and S. Shallcross
Nano Lett. 23, 11533 (2023) - DOI: 10.1021/acs.nanolett.3c03245
- THz induced giant spin and valley currents
S. Sharma, P. Elliott, and S. Shallcross
Sci. Adv. 9, eadf3673 (2023) - DOI: 10.1126/sciadv.adf3673
- Giant and controllable valley currents in graphene by double pumped THz light
S. Sharma, D. Gill, and S. Shallcross
Nano Lett. 23, 10305 (2023) - DOI: 10.1021/acs.nanolett.3c02874
- Ultrafast behavior of induced and intrinsic magnetic moments in CoFeB/Pt bilayers probed by element-specific measurements in the extreme ultraviolet spectral range
C. von Korff Schmising, S. Jana, K. Yao, M. Hennecke, P. Scheid, S. Sharma, M. Viret, J.-Y. Chauleau, D. Schick, and S. Eisebitt
Phys. Rev. Res. 5, 013147 (2023) - DOI: 10.1103/PhysRevResearch.5.013147
- Magnetic phase diagram of the austenitic Mn-rich Ni–Mn–(In, Sn) Heusler alloys
P. Bonfà, S. Chicco, F. Cugini, S. Sharma, J .K. Dewhurst , and G. Allodi
Electronic Structure 4, 024002 (2022) - DOI: 10.1088/2516-1075/ac5fbd
- Ab initio study of ultrafast spin dynamics in Gdx(FeCo)1-x alloys
J. K. Dewhurst, S. Shallcross, I. Radu, P. Elliott, C. von Korff Schmising, and S. Sharma
Appl. Phys. Lett. 120, 042401 (2022) - DOI: 10.1063/5.0075057
- Transient spin injection efficiencies at ferromagnet–metal interfaces
P. Elliott, A. Eschenlohr, J. Chen, S. Shallcross, U. Bovensiepen, J. K. Dewhurst, and S. Sharma
Adv. Mater. Interfaces 9, 2201233 (2022) - DOI: 10.1002/admi.202201233
- The 2022 magneto-optics roadmap
A. Kimel, A. Zvezdin, S. Sharma, S. Shallcross, N. de Sousa, A. Garcia-Martin, G. Salvan, J. Hamrle, O. Stejskal, J. McCord, S. Tacchi, G. Carlotti, P. Gambardella, G. Salis, M. Muenzenberg, M. Schultze, V. Temnov, I. V. Bychkov, L. N. Kotov, N. Maccaferri, D. Ignatyeva, V. Belotelov, C. Donnelly, A. Hierro Rodriguez, I. Matsuda, T. Ruchon, M. Fanciulli, M. Sacchi., C. Rita Du, H. Wang, N. P. Armitage, M. Schubert, V. Darakchieva, B. Liu, Z. Huang, B. Ding, A. Berger, and P. Vavassori
J. Phys. D: Appl. Phys. 55, 463003 (2022) - DOI: 10.1088/1361-6463/ac8da0
- Nanomechanical spectroscopy of 2D materials
J. N. Kirchhof, Y. Yu, G. Antheaume, G. Gordeev, D. Yagodkin, P. Elliott, D. B. de Araújo, S. Sharma, S. Reich, and K. I. Bolotin
Nano Lett. 22, 8037 (2022) - DOI: 10.1021/acs.nanolett.2c01289
- Ab initio study of ultrafast demagnetization of elementary ferromagnets by terahertz versus optical pulses
C. Pellegrini, S. Sharma, J. K. Dewhurst, and A. Sanna
Phys. Rev. B 105, 134425 (2022) - DOI: 10.1103/PhysRevB.105.134425
- Electronic origin of x-ray absorption peak shifts
S. Shallcross, C. v. Korff Schmising, P. Elliott, S. Eisebitt, J. K. Dewhurst, and S. Sharma
Phys. Rev. B 106, L060302 (2022) - DOI: 10.1103/PhysRevB.106.L060302
- Ultrafast optical control over spin and momentum in solids
S. Shallcross, Q. Z. Li, J. K. Dewhurst, S. Sharma, and P. Elliott
Appl. Phys. Lett. 120, 032403 (2022) - DOI: 10.1063/5.0076198
- Valley control by linearly polarized laser pulses: example of WSe2
S. Sharma, P. Elliott, and S. Shallcross
Optica 9, 947 (2022) - DOI: 10.1364/OPTICA.458991
- Making a case for femto-phono-magnetism with FePt
S. Sharma, S. Shallcross, P. Elliott, and J. K. Dewhurst
Sci. Adv. 8, eabq2021 (2022) - DOI: 10.1126/sciadv.abq2021
- Computational analysis of transient XMCD sum rules for laser pumped systems: When do they fail?
S. Sharma, S. Shallcross, P. Elliott, S. Eisebitt, C. von Korff Schmising, and J. K. Dewhurst
Appl. Phys. Lett. 120, 062409 (2022) - DOI: 10.1063/5.0080138
- Coupled Bogoliubov equations for electrons and phonons
C.-Y. Wang, S. Sharma, T. Müller, E. K. U. Gross, and J. K. Dewhurst
Phys. Rev. B 105, 174509 (2022) - DOI: 10.1103/PhysRevB.105.174509
- Dynamical Born effective charges
C.-Y. Wang, S. Sharma, E. K. U. Gross, J. K. Dewhurst
Phys. Rev. B 106, L180303 (2022) - DOI: 10.1103/PhysRevB.106.L180303
Publications (1st Funding Period 2018 - 2021)
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Angular momentum redistribution in laser-induced demagnetization
J. K. Dewhurst, S. Shallcross, P. Elliott, S. Eisebitt, C. v. Korff Schmising, and S. Sharma
Phys. Rev. B 104, 054438 (2021) - DOI: 10.1103/PhysRevB.104.054438 -
Spin/valley coupled dynamics of electrons and holes at the MoS2–MoSe2 interface
A. Kumar, D. Yagodkin, N. Stetzuhn, S. Kovalchuk, A. Melnikov, P. Elliott, S. Sharma, C. Gahl, and K. I. Bolotin
Nano Lett. 21, 7123 (2021) - DOI: 10.1021/acs.nanolett.1c01538 -
Manipulating magnons via ultrafast magnetization modulation
N. Singh, P. Elliott, J. K. Dewhurst, and S. Sharma
Phys. Rev. B 103, 134402 (2021) - DOI: 10.1103/PhysRevB.103.134402 -
Ultrafast optically induced ferromagnetic state in an elemental antiferromagnet
E. Golias, I. Kumberg, I. Gelen, S. Thakur, J. Gördes, R. Hosseinifar, Q. Guillet, J. K. Dewhurst, S. Sharma, C. Schüßler-Langeheine, N. Pontius, and W. Kuch
Phys. Rev. Lett. 126, 107202 (2021) - DOI: 10.1103/PhysRevLett.126.107202 -
Ab initio study of ultrafast charge dynamics in graphene
Q. Z. Li, P. Elliott, J. K. Dewhurst, S. Sharma, and S. Shallcross
Phys. Rev. B 103, L081102 (2021) - DOI: 10.1103/PhysRevB.103.L081102 -
Element-specific magnetization dynamics of complex magnetic systems probed by ultrafast magneto-optical spectroscopy
C. von Korff Schmising, F. Willems, S. Sharma, K. Yao, M. Borchert, M. Hennecke, D. Schick, I. Radu, C. Strüber, D. W. Engel, V. Shokeen, J. Buck, K. Bagschik, J. Viefhaus, G. Hartmann, B. Manschwetus, S. Grunewald, S. Düsterer, E. Jal, B. Vodungbo, J. Lüning, and S. Eisebitt
Appl. Sci. 10, 7580 (2020) - DOI: 10.3390/app10217580 -
Distinct spectral response in M-edge magnetic circular dichroism
K. Yao, F. Willems, C. von Korff Schmising, I. Radu, C. Strüber, D. Schick, D. Engel, A. Tsukamoto, J. K. Dewhurst, S. Sharma, and S. Eisebitt
Phys. Rev. B 102, 100405(R) (2020) - DOI: 10.1103/PhysRevB.102.100405 -
Efficiency of ultrafast optically induced spin transfer in Heusler compounds
D. Steil, J. Walowski, F. Gerhard, T. Kiessling, D. Ebke, A. Thomas, T. Kubota, M. Oogane, Y. Ando, J. Otto, A. Mann, M. Hofherr, P. Elliott, J. K. Dewhurst, G. Reiss, L. Molenkamp, M. Aeschlimann, M. Cinchetti, M. Münzenberg, S. Sharma, and S. Mathias
Phys. Rev. Res. 2, 023199 (2020) - DOI: 10.1103/PhysRevResearch.2.023199 -
The microscopic origin of spin-orbit mediated spin-flips
P. Elliott, N. Singh, K. Krieger, E. K. U. Gross, S. Sharma, and J. K. Dewhurst
J. Magn. Magn. Mater. 502, 166473 (2020) - DOI: 10.1016/j.jmmm.2020.166473 -
Element specificity of transient extreme ultraviolet magnetic dichroism
J. K. Dewhurst, F. Willems, P. Elliott, Q. Z. Li, C. von Korff Schmising, C. Strüber, D. W. Engel, S. Eisebitt, and S. Sharma
Phys. Rev. Lett. 124, 077203 (2020) - DOI: 10.1103/PhysRevLett.124.077203 -
Optical inter-site spin transfer probed by energy and spin-resolved transient absorption spectroscopy
F. Willems, C. v. Korff Schmising, C. Strüber, D. Schick, D. W. Engel, J. K. Dewhurst, P. Elliott, S. Sharma, and S. Eisebitt
Nat. Commun. 11: 871 (2020) - DOI: 10.1038/s41467-020-14691-5 -
Ultrafast optically induced spin transfer in ferromagnetic alloys
M. Hofherr, S. Häuser, J. K. Dewhurst, P. Tengdin, S. Sakshath, H. T. Nembach, S. T. Weber, J. M. Shaw, T. J. Silva, H. C. Kapteyn, M. Cinchetti, B. Rethfeld, M. M. Murnane, D. Steil, B. Stadtmüller, S. Sharma, M. Aeschlimann and S. Mathias
Sci. Adv. 6 : eaay8717 (2020) - DOI: 10.1126/sciadv.aay8717 -
Complete description of the magnetic ground state in spinel vanadates
J. Krishna, N. Singh, S. Shallcross, J. K. Dewhurst, E. K. U. Gross, T. Maitra, and S. Sharma
Phys. Rev. B 100, 081102(R) (2019) - DOI: 10.1103/PhysRevB.100.081102 -
Light-wave dynamic control of magnetism
F. Siegrist, J. A. Gessner, M. Ossiander, C. Denker, Y.-P. Chang, M. C. Schröder, A. Guggenmos, Y. Cui, J. Walowski, U. Martens, J. K. Dewhurst, U. Kleineberg, M. Münzenberg, S. Sharma, and M. Schultze
Nature 571, 240 (2019) - DOI: 10.1038/s41586-019-1333-x -
Magneto-optical functions at the 3p resonances of Fe, Co, and Ni: Ab initio description and experiment
F. Willems, S. Sharma, C. v. Korff Schmising, J. K. Dewhurst, L. Salemi, D. Schick, P. Hessing, C. Strüber, W. D. Engel, and S. Eisebitt
Phys. Rev. Lett. 122, 217202 (2019) - DOI: 10.1103/PhysRevLett.122.217202 -
Competing spin transfer and dissipation at Co/Cu(001) interfaces on femtosecond timescales
J. Chen, U. Bovensiepen, A. Eschenlohr, T. Müller, P. Elliott, E. K. U. Gross, J. K. Dewhurst, and S. Sharma
Phys. Rev. Lett 122, 067202 (2019) - DOI: 10.1103/PhysRevLett.122.067202 -
Real time scissor correction in TD-DFT
C.-Y. Wang, P. Elliott, S. Sharma, and J. K. Dewhurst
J. Phys.: Condens. Matter 31, 214002 (2019) - DOI: 10.1088/1361-648X/ab048a -
Substrate-controlled ultrafast spin injection and demagnetization
J. K. Dewhurst, S. Shallcross, E. K. U. Gross, and S. Sharma
Phys. Rev. Applied 10, 044065 (2018) - DOI: 10.1103/PhysRevApplied.10.0440