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 (2^nd 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 Gd_x(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 (1^st Funding Period 2018 - 2021)

• 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