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<p>Photo-induced dynamics of electronic processes are driven by the coupling between electronic and nuclear degrees of freedom. Here, we construct one- and two-dimensional organic-inorganic tin halides to investigate how dimensionality controls exciton-phonon coupling and exciton self-trapping. The results show that a one-dimensional system has strong exciton-phonon coupling leading to excitation-independent self-trapped exciton emission, whereas a two-dimensional system exhibits over ten times weaker coupling resulting in free exciton emission. The difference originates from enhanced Anderson localization in a one-dimensional system. Femtosecond transient absorption experiments directly resolve room-temperature vibrational wavepackets in a one-dimensional system, some of which propagate along the self-trapped-exciton potential energy surface. A combination of wagging and asymmetric stretching motions (~106 cm<sup>-1</sup>) in tin iodide is identified as such a mode, inducing exciton self-trapping. While no room-temperature wavepackets are observed in a two-dimensional system. These findings uncover the interplay between dimensionality-dependent exciton-phonon coupling and electronic/nuclear dynamics, offering constructive guidance to develop multifunctional organic-inorganic metal halides.</p>

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Dimensionality-dependent electronic and vibrational dynamics in low-dimensional organic-inorganic tin halides

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月15日

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  • Yanmei He,
  • Xinyi Cai,
  • Rafael B. Araujo,
  • Yibo Wang,
  • Sankaran Ramesh,
  • Junsheng Chen,
  • Muyi Zhang,
  • Tomas Edvinsson,
  • Feng Gao,
  • Tönu Pullerits

摘要

Photo-induced dynamics of electronic processes are driven by the coupling between electronic and nuclear degrees of freedom. Here, we construct one- and two-dimensional organic-inorganic tin halides to investigate how dimensionality controls exciton-phonon coupling and exciton self-trapping. The results show that a one-dimensional system has strong exciton-phonon coupling leading to excitation-independent self-trapped exciton emission, whereas a two-dimensional system exhibits over ten times weaker coupling resulting in free exciton emission. The difference originates from enhanced Anderson localization in a one-dimensional system. Femtosecond transient absorption experiments directly resolve room-temperature vibrational wavepackets in a one-dimensional system, some of which propagate along the self-trapped-exciton potential energy surface. A combination of wagging and asymmetric stretching motions (~106 cm-1) in tin iodide is identified as such a mode, inducing exciton self-trapping. While no room-temperature wavepackets are observed in a two-dimensional system. These findings uncover the interplay between dimensionality-dependent exciton-phonon coupling and electronic/nuclear dynamics, offering constructive guidance to develop multifunctional organic-inorganic metal halides.