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Room-Temperature Hot-Polaron Photovoltaics in the Charge-Ordered State of a Layered Perovskite Oxide Heterojunction

B. Kressdorf1, T. Meyer2, A. Belenchuk3,4, O. Shapoval3,4, M. ten Brink5, S. Melles1, U. Ross1, J. Hoffmann1, V. Moshnyaga3 et al.

M. Seibt2, P. Blöchl5,6, and C. Jooss1,*

  • 1University of Goettingen, Institute of Materials Physics, Friedrich-Hund-Platz 1, 37077 Goettingen, Germany
  • 2University of Goettingen, 4th Physical Institute – Solids and Nanostructures, Friedrich-Hund-Platz 1, 37077 Goettingen, Germany
  • 3University of Goettingen, 1st Physical Institute, Friedrich-Hund-Platz 1, 37077 Goettingen, Germany
  • 4IIEN, Academy of Sciences in Moldova, str. Academiei 3/3, MD-2028, Chisinau, Moldova
  • 5Institute for Theoretical Physics, University of Goettingen, Friedrich-Hund-Platz 1, 37077 Goettingen, Germany
  • 6Institute for Theoretical Physics, Clausthal University of Technology, Leibnizstr. 10, D-38678 Clausthal-Zellerfeld, Germany

  • *cjooss@gwdg.de

Phys. Rev. Applied 14, 054006 – Published 4 November, 2020

DOI: https://doi.org/10.1103/PhysRevApplied.14.054006

Abstract

Harvesting of solar energy by hot carriers from optically induced intraband transitions offers new perspectives for photovoltaic energy conversion. Clearly, mechanisms slowing down hot-carrier thermalization constitute a fundamental core of such pathways of third-generation photovoltaics. The intriguing concept of hot polarons stabilized by long-range phonon correlations in charge-ordered strongly correlated three-dimensional metal-oxide perovskite films has emerged and been demonstrated for Pr0.7Ca0.3MnO3 at low temperature. In this work, a tailored approach to extending such processes to room temperature is presented. It consists of a specially designed epitaxial growth of two-dimensional Ruddlesden-Popper Pr0.5Ca1.5MnO4 films on Nb:SrTiO3 with a charge-ordering transition at TCO ∼ 320 K. This opens the route to a different phonon-bottleneck strategy of slowing down carrier relaxation by strong coupling of electrons to cooperative lattice modes.

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