Terahertz-driven phonon upconversion in srtio3

ABSTRACT Direct manipulation of the atomic lattice using intense long-wavelength laser pulses has become a viable approach to create new states of matter in complex materials.

Conventionally, a high-frequency vibrational mode is driven resonantly by a mid-infrared laser pulse and the lattice structure is modified through indirect coupling of this infrared-active

phonon to other, lower-frequency lattice modulations. Here, we drive the lowest-frequency optical phonon in the prototypical transition metal oxide SrTiO3 well into the anharmonic regime

with an intense terahertz field. We show that it is possible to transfer energy to higher-frequency phonon modes through nonlinear coupling. Our observations are carried out by directly

mapping the lattice response to the coherent drive field with femtosecond X-ray pulses, enabling direct visualization of the atomic displacements. Access through your institution Buy or

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EXCITATION OF A COHERENT RAMAN-ACTIVE PHONON IN V2O3 Article Open access 28 April 2022 NONLOCAL NONLINEAR PHONONICS Article Open access 07 March 2022 ULTRAFAST TERAHERTZ EMISSION FROM

EMERGING SYMMETRY-BROKEN MATERIALS Article Open access 01 June 2023 DATA AVAILABILITY The data that support the findings of this study are available from the corresponding author upon

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Google Scholar  Download references ACKNOWLEDGEMENTS Use of the Linac Coherent Light Source, SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of

Science, Office of Basic Energy Sciences, under contract no. DE-AC02-76SF00515. M.K. and M.C.H. are supported by the US Department of Energy, Office of Science, Office of Basic Energy

Sciences, under award no. 2015-SLAC-100238-Funding. U.S. acknowledges support from the National Center of Competence in Research: Ultrafast Science and Technology (NCCR MUST) of the Swiss

National Science Foundation. S.B. acknowledges support from the Knut and Alice Wallenberg Foundation. Work at the University of Fribourg was supported by the Schweizer Nationalfonds (SNF) by

grant no. 200020-172611. M.K. and M.C.H. extend thanks to W. Chueh and A. Baclig for annealing the sample and to Z. Wu for assistance with the terahertz experiments. M.F. extends thanks to

M. Först for fruitful discussions about modelling the STO system. AUTHOR INFORMATION AUTHORS AND AFFILIATIONS * Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park,

CA, USA M. Kozina, T. van Driel, J. M. Glownia, D. Zhu & M. C. Hoffmann * Max Planck Institute for the Structure and Dynamics of Matter, Hamburg, Germany M. Fechner * Department of

Physics, University of Fribourg, Fribourg, Switzerland P. Marsik & C. Bernhard * Swiss Light Source, Paul Scherrer Institut, Villigen, Switzerland M. Radovic & U. Staub * Department

of Physics, Stockholm University, Stockholm, Sweden S. Bonetti Authors * M. Kozina View author publications You can also search for this author inPubMed Google Scholar * M. Fechner View

author publications You can also search for this author inPubMed Google Scholar * P. Marsik View author publications You can also search for this author inPubMed Google Scholar * T. van

Driel View author publications You can also search for this author inPubMed Google Scholar * J. M. Glownia View author publications You can also search for this author inPubMed Google

Scholar * C. Bernhard View author publications You can also search for this author inPubMed Google Scholar * M. Radovic View author publications You can also search for this author inPubMed 

Google Scholar * D. Zhu View author publications You can also search for this author inPubMed Google Scholar * S. Bonetti View author publications You can also search for this author

inPubMed Google Scholar * U. Staub View author publications You can also search for this author inPubMed Google Scholar * M. C. Hoffmann View author publications You can also search for this

author inPubMed Google Scholar CONTRIBUTIONS M.K. and M.C.H. conceived the experiment and performed the final data analysis. M.F. provided DFT calculations and theory support. T.v.D. and

S.B. helped with on-line data analysis. M.K., M.C.H., J.M.G. and D.Z. performed the time-resolved X-ray experiment. U.S. provided sample expertise and additional X-ray data. M.R. prepared

the sample. P.M. and C.B. carried out the terahertz ellipsometry measurements of the sample. The paper was written by M.K. and M.C.H., with substantial contributions from M.F., U.S. and S.B,

as well as with discussions from other authors. CORRESPONDING AUTHOR Correspondence to M. Kozina. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing interests.

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SUPPLEMENTARY INFORMATION Supplementary Figures 1–4, Supplementary Tables 1–5 and Supplementary References 1–3. SUPPLEMENTARY VIDEO 1 Animation of terahertz-driven phonon upconversion in

SrTiO3. RIGHTS AND PERMISSIONS Reprints and permissions ABOUT THIS ARTICLE CITE THIS ARTICLE Kozina, M., Fechner, M., Marsik, P. _et al._ Terahertz-driven phonon upconversion in SrTiO3.

_Nat. Phys._ 15, 387–392 (2019). https://doi.org/10.1038/s41567-018-0408-1 Download citation * Received: 27 July 2018 * Accepted: 11 December 2018 * Published: 21 January 2019 * Issue Date:

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