Scholarlink

<p>The optical response of semiconductors is governed by coupled electronic and vibrational excitations. In lead-halide perovskite nanocrystals, strong exciton–phonon interaction forms a ladder of exciton-polaron states accessible by femtosecond laser pulses. We demonstrate a fully coherent regime of exciton-polaron dynamics with long optical coherence times (<i>T</i><sub>2</sub>&#xa0;≈&#xa0;300 ps) in CsPbI<sub>3</sub> nanocrystals embedded in glass. Using transient two-pulse photon echo at a temperature of 2 K, we observe quantum beats between exciton-polaron states, with decay determined by optical phonon lifetimes of 5-15 ps. Within a four-level model, we directly quantify the exciton–phonon coupling strength through Huang–Rhys factors of 0.05&#xa0;−&#xa0;0.12 and 0.02&#xa0;−&#xa0;0.04 for low-energy optical phonons with energies of 3.2 and 5.1 meV, respectively. The pronounced size dependence of both coupling strengths and phonon lifetimes offers a route to tune the optical transitions between exciton-polaron states and tailor the coherent optical dynamics in perovskite semiconductors for solid-state quantum technologies.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Quantum beats of exciton-polarons in CsPbI3 perovskite nanocrystals

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年5月26日

查看全文
  • Artur V. Trifonov,
  • Mikhail O. Nestoklon,
  • M. Alex Hollberg,
  • Stefan Grisard,
  • Dennis Kudlacik,
  • Elena V. Kolobkova,
  • Maria S. Kuznetsova,
  • Serguei V. Goupalov,
  • Jan M. Kaspari,
  • Doris E. Reiter,
  • Dmitri R. Yakovlev,
  • Manfred Bayer,
  • Ilya A. Akimov

摘要

The optical response of semiconductors is governed by coupled electronic and vibrational excitations. In lead-halide perovskite nanocrystals, strong exciton–phonon interaction forms a ladder of exciton-polaron states accessible by femtosecond laser pulses. We demonstrate a fully coherent regime of exciton-polaron dynamics with long optical coherence times (T2 ≈ 300 ps) in CsPbI3 nanocrystals embedded in glass. Using transient two-pulse photon echo at a temperature of 2 K, we observe quantum beats between exciton-polaron states, with decay determined by optical phonon lifetimes of 5-15 ps. Within a four-level model, we directly quantify the exciton–phonon coupling strength through Huang–Rhys factors of 0.05 − 0.12 and 0.02 − 0.04 for low-energy optical phonons with energies of 3.2 and 5.1 meV, respectively. The pronounced size dependence of both coupling strengths and phonon lifetimes offers a route to tune the optical transitions between exciton-polaron states and tailor the coherent optical dynamics in perovskite semiconductors for solid-state quantum technologies.