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      Petahertz non-linear current in a centrosymmetric organic superconductor

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          Abstract

          Charge acceleration during an intense light field application to solids attracts much attention as elementary processes in high-harmonic generation and photoelectron emission. For manipulating such attosecond dynamics of charge, carrier-envelope-phase (CEP: relative phase between carrier oscillation of light field and its envelope function) control has been employed in insulators, nanometal and graphene. In superconducting materials, collective control of charge motion is expected because of its strongly coherent nature of quasi-particles. Here we report that, in a layered organic superconductor, a non-linear petahertz current driven by a single-cycle 6 femtosecond near infrared field shows up as second harmonic generation (SHG), which is in contrast to the common belief that even harmonics are forbidden in the centrosymmetric system. The SHG represents a CEP sensitive nature and an enhancement near the superconducting temperature. The result and its quantum many-body analysis indicate that a polarized current is induced by non-linear acceleration of charge, which is amplified by superconducting fluctuations. This will lead to petahertz functions of superconductors and of strongly correlated systems.

          Abstract

          Here the authors show second harmonic generation (SHG) from a centrosymmetric organic superconductor κ-(BEDT-TTF) 2Cu[N(CN) 2]Br. They find unusual temperature dependence and CEP-sensitive nature of the SHG which are explained in terms of nonlinear current.

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          Most cited references28

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          Observation of high-order harmonic generation in a bulk crystal

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            Extreme ultraviolet high-harmonic spectroscopy of solids.

            Extreme ultraviolet (EUV) high-harmonic radiation emerging from laser-driven atoms, molecules or plasmas underlies powerful attosecond spectroscopy techniques and provides insight into fundamental structural and dynamic properties of matter. The advancement of these spectroscopy techniques to study strong-field electron dynamics in condensed matter calls for the generation and manipulation of EUV radiation in bulk solids, but this capability has remained beyond the reach of optical sciences. Recent experiments and theoretical predictions paved the way to strong-field physics in solids by demonstrating the generation and optical control of deep ultraviolet radiation in bulk semiconductors, driven by femtosecond mid-infrared fields or the coherent up-conversion of terahertz fields to multi-octave spectra in the mid-infrared and optical frequencies. Here we demonstrate that thin films of SiO2 exposed to intense, few-cycle to sub-cycle pulses give rise to wideband coherent EUV radiation extending in energy to about 40 electronvolts. Our study indicates the association of the emitted EUV radiation with intraband currents of multi-petahertz frequency, induced in the lowest conduction band of SiO2. To demonstrate the applicability of high-harmonic spectroscopy to solids, we exploit the EUV spectra to gain access to fine details of the energy dispersion profile of the conduction band that are as yet inaccessible by photoemission spectroscopy in wide-bandgap dielectrics. In addition, we use the EUV spectra to trace the attosecond control of the intraband electron motion induced by synthesized optical transients. Our work advances lightwave electronics in condensed matter into the realm of multi-petahertz frequencies and their attosecond control, and marks the advent of solid-state EUV photonics.
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              Optical-field-induced current in dielectrics.

              The time it takes to switch on and off electric current determines the rate at which signals can be processed and sampled in modern information technology. Field-effect transistors are able to control currents at frequencies of the order of or higher than 100 gigahertz, but electric interconnects may hamper progress towards reaching the terahertz (10(12) hertz) range. All-optical injection of currents through interfering photoexcitation pathways or photoconductive switching of terahertz transients has made it possible to control electric current on a subpicosecond timescale in semiconductors. Insulators have been deemed unsuitable for both methods, because of the need for either ultraviolet light or strong fields, which induce slow damage or ultrafast breakdown, respectively. Here we report the feasibility of electric signal manipulation in a dielectric. A few-cycle optical waveform reversibly increases--free from breakdown--the a.c. conductivity of amorphous silicon dioxide (fused silica) by more than 18 orders of magnitude within 1 femtosecond, allowing electric currents to be driven, directed and switched by the instantaneous light field. Our work opens the way to extending electronic signal processing and high-speed metrology into the petahertz (10(15) hertz) domain.
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                Author and article information

                Contributors
                s-iwai@tohoku.ac.jp
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                18 August 2020
                18 August 2020
                2020
                : 11
                : 4138
                Affiliations
                [1 ]GRID grid.69566.3a, ISNI 0000 0001 2248 6943, Department of Physics, , Tohoku University, ; Sendai, 980-8578 Japan
                [2 ]GRID grid.27476.30, ISNI 0000 0001 0943 978X, Department of Applied Physics, , Nagoya University, ; Nagoya, 464-8603 Japan
                [3 ]GRID grid.69566.3a, ISNI 0000 0001 2248 6943, Institute for Materials Research, , Tohoku University, ; Sendai, 980-8577 Japan
                [4 ]GRID grid.467196.b, ISNI 0000 0001 2285 6123, Institute for Molecular Science, ; Okazaki, 444-8585 Japan
                [5 ]GRID grid.444568.f, ISNI 0000 0001 0672 2184, Department of Applied Physics, , Okayama University of Science, ; Okayama, 700-0005 Japan
                [6 ]GRID grid.443595.a, ISNI 0000 0001 2323 0843, Department of Physics, , Chuo University, ; Tokyo, 112-8551 Japan
                Author information
                http://orcid.org/0000-0002-0767-5428
                http://orcid.org/0000-0002-5686-5156
                http://orcid.org/0000-0002-5713-1859
                Article
                17776
                10.1038/s41467-020-17776-3
                7434879
                32811820
                66b66bdf-93cc-4d3b-9a91-af75d67cd755
                © The Author(s) 2020

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 5 March 2020
                : 20 July 2020
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                © The Author(s) 2020

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                nonlinear optics,organic molecules in materials science,high-harmonic generation

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