Abstract
Two types of coupling between electromagnetic radiation and a crystal lattice have so far been identified experimentally. The first is the direct coupling of light to infrared-active vibrations carrying an electric dipole. The second is indirect, involving electron–phonon coupling and occurring through excitation of the electronic system; stimulated Raman scattering1,2,3 is one example. A third path, ionic Raman scattering (IRS; refs 4, 5), was proposed 40 years ago. It was posited that excitation of an infrared-active phonon could serve as the intermediate state for Raman scattering, a process that relies on lattice anharmonicities rather than electron–phonon interactions6. Here, we report an experimental demonstration of IRS using femtosecond excitation and coherent detection of the lattice response. We show how this mechanism is relevant to ultrafast optical control in solids: a rectified phonon field can exert a directional force onto the crystal, inducing an abrupt displacement of the atoms from their equilibrium positions. IRS opens up a new direction for the optical control of solids in their electronic ground state7,8,9, different from carrier excitation10,11,12,13,14.
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References
Dhar, L., Rogers, J. A. & Nelson, K. A. Time-resolved vibrational spectroscopy in the impulsive limit. Chem. Rev. 94, 157–193 (1994).
Merlin, R. Generating coherent THz phonons with light pulses. Solid State Commun. 102, 207–220 (1997).
Dekorsy, T., Cho, G. C. & Kurz, H. in Light Scattering in Solids VIII Vol. 76 (eds Cardona, M. & Güntherodt, G.) 169–209 (Topics in Appl. Phys., Springer, 2000).
Wallis, R. F. & Maradudin, A. A. Ionic Raman effect II. The first-order ionic Raman effect. Phys. Rev. B 3, 2063–2075 (1971).
Martin, T. P. & Genzel, L. Ionic Raman scattering and ionic frequency mixing. Phys. Status Solide B 61, 493–502 (1974).
Mills, D. L. Ionic contribution to the Raman tensor of insulators. Phys. Rev. B 35, 9278–9283 (1987).
Rini, M. et al. Control of the electronic phase of a manganite by mode-selective vibrational excitation. Nature 449, 72–74 (2007).
Tobey, R. I., Prabhakaran, D., Boothroyd, A. T. & Cavalleri, A. Ultrafast electronic phase transition in La1/2Sr3/2MnO4 by coherent vibrational excitation: Evidence for non-thermal melting of orbital order. Phys. Rev. Lett. 101, 197404 (2008).
Fausti, D. et al. Light induced superconductivity in a striped-ordered cuprate. Science 331, 189–191 (2011).
Miyano, K., Tanaka, T., Tomioka, Y. & Tokura, Y. Photoinduced insulator-to-metal transition in a perovskite manganite. Phys. Rev. Lett. 78, 4257–4260 (1997).
Fiebig, M., Miyano, K., Tomioka, Y. & Tokura, Y. Visualization of the local insulator-metal transition in Pr0.7Ca0.3MnO3 . Science 280, 1925–1928 (1998).
Cavalleri, A. et al. Femtosecond structural dynamics in VO2 during an ultrafast solid–solid phase transition. Phys. Rev. Lett. 87, 237401 (2001).
Cavalleri, A., Rini, M. & Schoenlein, R. W. Ultra-broadband femtosecond measurements of the photo-induced phase transition in VO2: From the mid-infrared to the hard X-rays. J. Phys. Soc. Jpn 75, 011004 (2007).
Perfetti, L. et al. Time evolution of the electronic structure of 1T–TaS2 through the insulator-metal transition. Phys. Rev. Lett. 97, 067402 (2006).
Von der Linde, D. & Lambrich, R. Direct measurement of hot-electron relaxation by picosecond spectroscopy. Phys. Rev. Lett. 42, 1090–1093 (1979).
Kuznetsov, A. V. & Stanton, C. J. Theory of coherent phonon oscillations in semiconductors. Phys. Rev. Lett. 73, 3243–3246 (1994).
Garrett, G. A., Albrecht, T. F., Whitaker, J. F. & Merlin, R. Coherent THz phonons driven by light pulses and the Sb problem: What is the mechanism? Phys. Rev. Lett. 77, 3661–3664 (1996).
Stevens, T. E., Kuhl, J. & Merlin, R. Coherent phonon generation and the two stimulated Raman tensors. Phys. Rev. B 65, 144304 (2002).
Mayer, A. & Keilmann, F. Far-infrared nonlinear optics. I. χ(2) near ionic resonance. Phys. Rev. B 33, 6954–6961 (1986).
Dekorsy, T., Yakovlev, V. A., Seidel, W., Helm, M. & Keilmann, F. Infrared-phonon–polariton resonance of the nonlinear susceptibility in GaAs. Phys. Rev. Lett. 90, 055508 (2003).
Hase, M., Kitajima, M., Nakashima, S-I. & Mizoguchi, K. Dynamics of coherent anharmonic phonons in bismuth using high density photoexcitation. Phys. Rev. Lett. 88, 067401 (2002).
Zener, C. Interaction between the d-shells in the transition metals. II. Ferromagnetic compounds of manganese with perovskite structure. Phys. Rev. 82, 403–405 (1951).
Anderson, P. W. & Hasegawa, H. Considerations on double exchange. Phys. Rev. 100, 675–681 (1955).
De Gennes, P. G. Effects of double exchange in magnetic crystals. Phys. Rev. 118, 141–154 (1960).
Okimoto, Y., Katsufuji, T., Ishikawa, T., Arima, T. & Tokura, Y. Variation of electronic structure in La1−x Sr x MnO3 (0=x=0.3) as investigated by optical conductivity spectra. Phys. Rev. B 55, 4206–4214 (1997).
Abrashev, M. V. et al. Comparative study of optical phonons in the rhombohedrally distorted perovskites LaAlO3 and LaMnO3 . Phys. Rev. B 59, 4146–4153 (1999).
Granado, E. et al. Phonon Raman scattering in R1−x A x MnO3+δ (R=La,Pr;A=Ca,Sr). Phys. Rev. B 58, 11435–11440 (1998).
Ogasawara, T. et al. Photoinduced spin dynamics in La0.6Sr0.4MnO3 observed by time-resolved magneto-optical Kerr spectroscopy. Phys. Rev. B 68, 180407 (2003).
Zeiger, H. J. et al. Theory for displacive excitation of coherent phonons. Phys. Rev. B 45, 768–778 (1992).
Manzoni, C., Först, M., Ehrke, H. & Cavalleri, A. Single-Shot detection and direct control of carrier phase drift of mid-infrared pulses. Opt. Lett. 35, 757–759 (2010).
Acknowledgements
This work was funded by the Max Planck Society through institutional support for the Max Planck Research Group for Structural Dynamics at the University of Hamburg, and was further supported in part by the US Air Force Office of Scientific Research under contract FA 9550-08-01-0340 through the Multidisciplinary University Research Initiative Program.
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A.C. and M.F. conceived and coordinated the project. M.F. and C.M. developed the experimental apparatus and carried out the experiments. Y. Tomioka and Y. Tokura provided the samples. M.F., C.M., and S.K. analysed the experimental data and interpreted these together with A.C. and R.M.. R.M. developed the analytic theory of Raman scattering. M.F., R.M., and A.C. wrote the manuscript.
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Först, M., Manzoni, C., Kaiser, S. et al. Nonlinear phononics as an ultrafast route to lattice control. Nature Phys 7, 854–856 (2011). https://doi.org/10.1038/nphys2055
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DOI: https://doi.org/10.1038/nphys2055
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