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Collapse of long-range charge order tracked by time-resolved photoemission at high momenta

Nature volume 471, pages 490–493 (2011)Cite this article

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Abstract

Intense femtosecond (10−15 s) light pulses can be used to transform electronic, magnetic and structural order in condensed-matter systems on timescales of electronic and atomic motion1,2,3. This technique is particularly useful in the study4,5 and in the control6 of materials whose physical properties are governed by the interactions between multiple degrees of freedom. Time- and angle-resolved photoemission spectroscopy is in this context a direct and comprehensive, energy- and momentum-selective probe of the ultrafast processes that couple to the electronic degrees of freedom7,8,9,10. Previously, the capability of such studies to access electron momentum space away from zero momentum was, however, restricted owing to limitations of the available probing photon energy10,11. Here, using femtosecond extreme-ultraviolet pulses delivered by a high-harmonic-generation source, we use time- and angle-resolved photoemission spectroscopy to measure the photoinduced vaporization of a charge-ordered state in the potential excitonic insulator 1T-TiSe2 (refs 12, 13). By way of stroboscopic imaging of electronic band dispersions at large momentum, in the vicinity of the edge of the first Brillouin zone, we reveal that the collapse of atomic-scale periodic long-range order happens on a timescale as short as 20 femtoseconds. The surprisingly fast response of the system is assigned to screening by the transient generation of free charge carriers. Similar screening scenarios are likely to be relevant in other photoinduced solid-state transitions and may generally determine the response times. Moreover, as electron states with large momenta govern fundamental electronic properties in condensed matter systems14, we anticipate that the experimental advance represented by the present study will be useful to study the ultrafast dynamics and microscopic mechanisms of electronic phenomena in a wide range of materials.

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Figure 1: CDW phase transition of 1T-TiSe2.
Figure 2: Tracking the photoinduced transition by femtosecond time-resolved ARPES.
Figure 3: Fluence dependence of the photoinduced transition.

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References

  1. Yonemitsu, K. & Nasu, K. Theory of photoinduced phase transitions in itinerant electron systems. Phys. Rep. 465, 1–60 (2008)

    Article  ADS  CAS  Google Scholar 

  2. Bargheer, M., Zhavoronkov, N., Woerner, M. & Elsaesser, T. Recent progress in ultrafast X-ray diffraction. ChemPhysChem 7, 783–792 (2006)

    Article  CAS  Google Scholar 

  3. Bigot, J.-Y., Vomir, M. & Beaurepaire, E. Coherent ultrafast magnetism induced by femtosecond laser pulses. Nature Phys. 5, 515–520 (2009)

    Article  ADS  CAS  Google Scholar 

  4. Chollet, M. et al. Gigantic photoresponse in ¼-filled-band organic salt (EDO-TTF)2PF6 . Science 307, 86–89 (2005)

    Article  ADS  CAS  Google Scholar 

  5. Demsar, J., Biljakovic´, K. & Mihailovic, D. Single particle and collective excitations in the one-dimensional charge density wave solid K0. 3MoO3 probed in real time by femtosecond spectroscopy. Phys. Rev. Lett. 83, 800–803 (1999)

    Article  ADS  CAS  Google Scholar 

  6. Rini, M. et al. Control of the electronic phase of a manganite by mode-selective vibrational excitation. Nature 449, 72–74 (2007)

    Article  ADS  CAS  Google Scholar 

  7. Haight, R. & Silbermann, J. A. Surface intervalley scattering on GaAs(110): direct observation with picosecond laser photoemission. Phys. Rev. Lett. 62, 815–818 (1989)

    Article  ADS  CAS  Google Scholar 

  8. Fann, W. S., Storz, R., Tom, H. W. K. & Bokor, J. Electron thermalization in gold. Phys. Rev. B 46, 13592–13595 (1992)

    Article  ADS  CAS  Google Scholar 

  9. Bauer, M. et al. Direct observation of surface chemistry using ultrafast soft-X-ray pulses. Phys. Rev. Lett. 87, 025501 (2001)

    Article  ADS  Google Scholar 

  10. Perfetti, L. et al. Time evolution of the electronic structure of 1T-TaS2 through the insulator-metal transition. Phys. Rev. Lett. 97, 067402 (2006)

    Article  ADS  CAS  Google Scholar 

  11. Schmitt, F. et al. Transient electronic structure and melting of a charge density wave in TbTe3 . Science 321, 1649–1652 (2008)

    Article  ADS  CAS  Google Scholar 

  12. Cercellier, H. et al. Evidence for an excitonic insulator phase in 1T-TiSe2 . Phys. Rev. Lett. 99, 146403 (2007)

    Article  ADS  CAS  Google Scholar 

  13. Di Salvo, F. J., Moncton, D. E. & Waszczak, J. V. Electronic properties and superlattice formation in the semimetal TiSe2 . Phys. Rev. B 14, 4321–4328 (1976)

    Article  ADS  CAS  Google Scholar 

  14. Ashcroft, N. W. & Mermin, N. D. Solid State Physics (Brooks/Cole, Belmont, 1976)

    MATH  Google Scholar 

  15. Ohta, T., Bostwick, A., Seyller, T., Horn, K. & Rotenberg, E. Controlling the electronic structure of bilayer graphene. Science 313, 951–954 (2006)

    Article  ADS  CAS  Google Scholar 

  16. Kondo, T., Khasanov, R., Takeuchi, T., Schmalian, J. & Kaminski, A. Competition between the pseudogap and superconductivity in the high-T c copper oxides. Nature 457, 296–300 (2009)

    Article  ADS  CAS  Google Scholar 

  17. Mazin, I. Superconductivity gets an iron boost. Nature 464, 183–186 (2010)

    Article  ADS  CAS  Google Scholar 

  18. Rossnagel, K., Kipp, L. & Skibowski, M. Charge-density-wave phase transition in 1T-TiSe2: excitonic insulator versus band-type Jahn-Teller mechanism. Phys. Rev. B 65, 235101 (2002)

    Article  ADS  Google Scholar 

  19. Kidd, T. E., Miller, T., Chou, M. Y. & Chiang, T.-C. Electron-hole coupling and the charge density wave transition in TiSe2 . Phys. Rev. Lett. 88, 226402 (2002)

    Article  ADS  CAS  Google Scholar 

  20. Rundquist, A. et al. Phase matching of soft-X-ray harmonic emission in hollow-core fibers. Science 280, 1412–1415 (1998)

    Article  ADS  CAS  Google Scholar 

  21. Anisimov, S. I., Kapeliovich, B. L. & Perel’man, T. L. Electron-emission from surface of metals induced by ultrashort laser pulses. Sov. Phys. JETP 39, 375–377 (1974)

    ADS  Google Scholar 

  22. Cavalleri, A. et al. Evidence for a structurally-driven insulator-to-metal transition in VO2: a view from the ultrafast timescale. Phys. Rev. B 70, 161102(R) (2004)

    Article  ADS  Google Scholar 

  23. Wall, S. et al. Quantum interference between charge excitation paths in a solid-state Mott insulator. Nature Phys. advance online publication. 10.1038/nphys1831 (5 December 2010)

  24. Holy, J. A., Woo, K. C., Klein, M. V. & Brown, F. C. Raman and infrared studies of superlattice formation in TiSe2 . Phys. Rev. B 16, 3628–3637 (1977)

    Article  ADS  CAS  Google Scholar 

  25. El Sayed, K., Schuster, S., Haug, H., Herzel, F. & Henneberger, K. Subpicosecond plasmon response: buildup of screening. Phys. Rev. B 49, 7337–7344 (1994)

    Article  ADS  CAS  Google Scholar 

  26. Bányai, L., Vu, Q. T., Mieck, B. & Haug, H. Ultrafast quantum kinetics of time-dependent RPA-screened Coulomb scattering. Phys. Rev. Lett. 81, 882–885 (1998)

    Article  ADS  Google Scholar 

  27. Huber, R. et al. How many-particle interactions develop after ultrafast excitation of an electron-hole plasma. Nature 414, 286–289 (2001)

    Article  ADS  CAS  Google Scholar 

  28. Sokolowski-Tinten, K. et al. Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit. Nature 422, 287–289 (2003)

    Article  ADS  CAS  Google Scholar 

  29. Siwick, B. J., Dwyer, J. R., Jordan, R. E. & Miller, R. J. D. An atomic-level view of melting using femtosecond electron diffraction. Science 302, 1382–1385 (2003)

    Article  ADS  CAS  Google Scholar 

  30. Miaja-Avila, L. et al. Laser-assisted photoelectric effect from surfaces. Phys. Rev. Lett. 97, 113604 (2006)

    Article  ADS  CAS  Google Scholar 

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Acknowledgements

M.B. and S.M. thank M. Aeschlimann for support and discussion. M.B. and S.M. also thank M. Murnane and H. Kapteyn for their support through the NSF EUV ERC. A.C. acknowledges support from the JILA Physics Frontier Center. This work was supported by the German Science Foundation (DFG) within the SFB 855 (C.S., M.B., L.K., K.R.) and by the European Community's FP7 under Marie Curie International Outgoing Fellowship GA 253316 (S.M.). Operation of the Advanced Light Source is supported by the US Department of Energy, Office of Basic Energy Sciences.

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Author notes

  1. Timm Rohwer and Stefan Hellmann: These authors contributed equally to this work.

Authors and Affiliations

  1. Institute of Experimental and Applied Physics, University of Kiel, Kiel, 24118, Germany

    Timm Rohwer, Stefan Hellmann, Martin Wiesenmayer, Christian Sohrt, Ankatrin Stange, Bartosz Slomski, Matthias Kalläne, Lutz Kipp, Kai Rossnagel & Michael Bauer

  2. JILA, University of Colorado and NIST, Boulder, 80309-0440, Colorado, USA

    Adra Carr & Stefan Mathias

  3. University of California, Berkeley, NSF ERC Extreme Ultraviolet Science and Technology, Berkeley, 94720, California, USA

    Yanwei Liu

  4. Center for X-Ray Optics, Lawrence Berkeley National Laboratory, Berkeley, 94720, California, USA

    Yanwei Liu

  5. Center for Nano and Molecular Science, University of Texas at Austin, Austin, 78722, Texas, USA

    Luis Miaja Avila

  6. Department of Physics and Research Center OPTIMAS, University of Kaiserslautern, Kaiserslautern, 67663, Germany

    Stefan Mathias

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Contributions

M.B. and K.R. conceived the experiment and wrote the paper. T.R., S.H., M.W., B.S., S.M., L.K., M.B. and K.R. realized the experimental time-resolved ARPES setup. A.C., L.M.A. and Y.L. designed and fabricated the EUV multilayer mirrors. T.R., S.H., M.W., C.S. and A.S. collected the time-resolved photoemission data and performed the data analysis. M.K. and K.R. collected and analysed the static photoemission data at the Advanced Light Source. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Kai Rossnagel or Michael Bauer.

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The authors declare no competing financial interests.

Supplementary information

Supplementary Information

The file contains Supplementary Text, Supplementary Figures 1-5 with legends and additional references. (PDF 911 kb)

Supplementary Movie 1

The movie shows photo-induced phase transition (see Supplementary Information S1 for full legend). (MOV 5118 kb)

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Rohwer, T., Hellmann, S., Wiesenmayer, M. et al. Collapse of long-range charge order tracked by time-resolved photoemission at high momenta. Nature 471, 490–493 (2011). https://doi.org/10.1038/nature09829

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