Attosecond nonlinear polarization and light-matter energy transfer in solids

A. Sommer, E. M. Bothschafter, S. A. Sato, C. Jakubeit, T. Latka, O. Razskazovskaya, H. Fattahi, M. Jobst, W. Schweinberger, V. Shirvanyan, V. S. Yakovlev, R. Kienberger, K. Yabana, N. Karpowicz, M. Schultze, F. Krausz

Research output: Contribution to journalArticleResearchpeer-review

Abstract

Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization1,2 produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques3,4,5,6,7,8 have provided experimental access to this important observable up to frequencies of several terahertz9,10,11,12,13. Here we demonstrate that attosecond metrology14 extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750 nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light–matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible–infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.
Original languageEnglish
Pages (from-to)86-90
JournalNature
Volume534
Issue number7605
DOIs
Publication statusPublished - 2 Jun 2016
Externally publishedYes

Fields of Expertise

  • Advanced Materials Science

Cite this

Sommer, A., Bothschafter, E. M., Sato, S. A., Jakubeit, C., Latka, T., Razskazovskaya, O., ... Krausz, F. (2016). Attosecond nonlinear polarization and light-matter energy transfer in solids. Nature, 534(7605), 86-90. https://doi.org/10.1038/nature17650

Attosecond nonlinear polarization and light-matter energy transfer in solids. / Sommer, A.; Bothschafter, E. M.; Sato, S. A.; Jakubeit, C.; Latka, T.; Razskazovskaya, O.; Fattahi, H.; Jobst, M.; Schweinberger, W.; Shirvanyan, V.; Yakovlev, V. S.; Kienberger, R.; Yabana, K.; Karpowicz, N.; Schultze, M.; Krausz, F.

In: Nature, Vol. 534, No. 7605, 02.06.2016, p. 86-90.

Research output: Contribution to journalArticleResearchpeer-review

Sommer, A, Bothschafter, EM, Sato, SA, Jakubeit, C, Latka, T, Razskazovskaya, O, Fattahi, H, Jobst, M, Schweinberger, W, Shirvanyan, V, Yakovlev, VS, Kienberger, R, Yabana, K, Karpowicz, N, Schultze, M & Krausz, F 2016, 'Attosecond nonlinear polarization and light-matter energy transfer in solids' Nature, vol. 534, no. 7605, pp. 86-90. https://doi.org/10.1038/nature17650
Sommer A, Bothschafter EM, Sato SA, Jakubeit C, Latka T, Razskazovskaya O et al. Attosecond nonlinear polarization and light-matter energy transfer in solids. Nature. 2016 Jun 2;534(7605):86-90. https://doi.org/10.1038/nature17650
Sommer, A. ; Bothschafter, E. M. ; Sato, S. A. ; Jakubeit, C. ; Latka, T. ; Razskazovskaya, O. ; Fattahi, H. ; Jobst, M. ; Schweinberger, W. ; Shirvanyan, V. ; Yakovlev, V. S. ; Kienberger, R. ; Yabana, K. ; Karpowicz, N. ; Schultze, M. ; Krausz, F. / Attosecond nonlinear polarization and light-matter energy transfer in solids. In: Nature. 2016 ; Vol. 534, No. 7605. pp. 86-90.
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AU - Bothschafter, E. M.

AU - Sato, S. A.

AU - Jakubeit, C.

AU - Latka, T.

AU - Razskazovskaya, O.

AU - Fattahi, H.

AU - Jobst, M.

AU - Schweinberger, W.

AU - Shirvanyan, V.

AU - Yakovlev, V. S.

AU - Kienberger, R.

AU - Yabana, K.

AU - Karpowicz, N.

AU - Schultze, M.

AU - Krausz, F.

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N2 - Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization1,2 produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques3,4,5,6,7,8 have provided experimental access to this important observable up to frequencies of several terahertz9,10,11,12,13. Here we demonstrate that attosecond metrology14 extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750 nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light–matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible–infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.

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