Snapshots of electronic structure by
Time and Angle Resolved Photo-emission
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Charge density waves (CDW) underpin the electronic properties of many complex materials. Near-equilibrium CDW order is linearly coupled to a periodic, atomic-structural distortion, and the dynamics is understood in terms of amplitude and phase modes. |
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Figure: Snapshots of momentum-dependent photoemission intensity. In the first panel the equilibrium band positions are marked. As the insulator-metal transition proceeds, transfer of intensity across the Fermi level is evident throughout both Brillouin zones. The gap between bands at the zone boundary collapses on sub-vibrational timescales.
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However, at the shortest timescales lattice and charge order may become de-coupled, highlighting the electronic nature of this many-body ground state. Using time and angle resolved photoemission spectroscopy with sub-30-fs XUV pulses near 20 eV photon energy, we have mapped the time- and momentum-dependent electronic structure in photo-stimulated 1T-TaS2, a two-dimensional charge density wave compound. Contrary to what was expected, we found that CDW order, melted well before relaxation of the underlying structural distortion [1].
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Figure: Time-resolved maps of photoemission intensity at Γ and M-point of the CDW compound after optical excitation. The collapse of the Mott gap is highlighted by the prompt transfer of intensity across the Fermi level (EB=0 meV) at different points of the Brillouin zone. The destruction of CDW order appears as the collapse of two distinct bands into a single feature. (see also the right diagram, showing individual energy distribution curves before and after photoexcitation). |
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These studies were combined with ultrabroadband optical spectroscopy to connect the physics of this unconventional photo-excited state with the polaronic transport in these transiently photometallic compounds [2].
In the future, we plan to extend studies of complex many-electron dynamics to few femtoseconds or even attosecond timescales, in a collaborative effort with the extreme timescales group of Adrian Cavalieri. |
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Related Publications:
| [1] Clocking the Melting Transition of Charge and Lattice Order in 1T-TaS2 with Ultrafast Extreme-Ultraviolet Angle-Resolved Photoemission Spectroscopy | |
| J. C. Petersen, S. Kaiser, N. Dean, A. Simoncig, H. Y. Liu, A. L. Cavalieri, C. Cacho, I. C. E. Turcu, E. Springate, F. Frassetto, L. Poletto, S. S. Dhesi, H. Berger, and A. Cavalleri | |
| Physical Review Letters 107, 177402 (2011) | |
| → press release | |
| [2] Polaronic Conductivity in the Photoinduced Phase of 1T-TaS2 | |
| N. Dean, J. C. Petersen, D. Fausti, R. I. Tobey, S. Kaiser, L. V. Gasparov, H. Berger, and A. Cavalleri | |
| Phys. Rev. Lett. 106, 016401 (2011) | |
| →more | |
| Experiment: |