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DOE OSTI · 3372079

A metastable tetragonal phase in two-dimensional halide perovskite lattices driven by a coherent Higgs mode

Shukla, Ayushi [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0009000302729030)·Agrawal, Sraddha [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000322950632)·Peifer, Shoshanna [Northwestern Univ., Evanston, IL (United States); International Institute for Nanotechnology, Evanston, IL (United States)]·Kanatzidis, Mercouri G. [Northwestern Univ., Evanston, IL (United States); International Institute for Nanotechnology, Evanston, IL (United States); Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000320374168)·Darancet, Pierre [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000258461673)·Schaller, Richard D. [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM); Northwestern Univ., Evanston, IL (United States); International Institute for Nanotechnology, Evanston, IL (United States)] (ORCID:0000000196968830)
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Abstract

The optoelectronic properties of metal halide perovskites are defined by their coupled structural and photophysical properties, yet their lattice behaviour remains underexplored. Here, using impulsive stimulated Raman spectroscopy, we study light-induced phonon dynamics of two-dimensional butylammonium lead iodide ((BA) 2 PbI 4 ) films under varying excitation intensities, photon energies and temperatures. We reveal that, whereas (BA) 2 PbI 4 exhibits two thermally accessible orthorhombic phases, optically excited phonons transiently direct the lattice to a distinct, higher symmetry tetragonal phase. We show that bandgap oscillations arise from simultaneous distortions of in-plane and out-of-plane octahedral tilt angles with oscillations following a low-to-high symmetry pathway, marked by two vibrational frequencies independent of intensity—a signature of an optically excited Higgs mode. Notably, the Higgs mode at below-bandgap excitation induces a fourfold larger spectral shift than above-bandgap, where photogenerated charge carriers drive the system away from the optically induced tetragonal phase. This study illustrates how optomechanical coupling influences the optical properties of two-dimensional perovskites.

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Shukla, Ayushi [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0009000302729030), Agrawal, Sraddha [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000322950632), Peifer, Shoshanna [Northwestern Univ., Evanston, IL (United States); International Institute for Nanotechnology, Evanston, IL (United States)], Kanatzidis, Mercouri G. [Northwestern Univ., Evanston, IL (United States); International Institute for Nanotechnology, Evanston, IL (United States); Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000320374168), Darancet, Pierre [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000258461673), Schaller, Richard D. [Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials (CNM); Northwestern Univ., Evanston, IL (United States); International Institute for Nanotechnology, Evanston, IL (United States)] (ORCID:0000000196968830). 2026-01-05. A metastable tetragonal phase in two-dimensional halide perovskite lattices driven by a coherent Higgs mode. https://doi.org/10.1038/s41563-025-02433-1

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