Giant single-step upconversion via sub–35-fs phonon dynamics in the nonlinear optical regime

Phonon-assisted upconversion (UC) for anti-Stokes photoluminescence stands as a fundamental and widely studied process, central to both ultrafast electron-phonon coupling physics and diverse photonic applications. However, the ultrafast dynamics limit of UC has yet to be addressed, preventing its integration into the nonlinear optical regime. Here, we find a giant single-step UC of ~200 milli-electron volts via sub-35-femtosecond phonon dynamics in two-dimensional hybrid organic-inorganic perovskites in the nonlinear regime. The single-step UC approaches the phonon dynamics limit of ~23 femtoseconds and gains energy about eight times the room-temperature thermal energy (~25 milli-electron volts), enabling its synergistic integration into the nonlinear regime. Benefiting from the unique electron-phonon coupling between organic vibrations and excitons in inorganic lattices, the UC demonstrates distinctive signatures of Raman anisotropy and strong nonlinearity. This work opens new avenues for studying uncharted phonon dynamics and nonlinear optical mechanisms, offering substantial advantages in optical refrigeration, upconverting energy harvesting and optical microscopy.

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Publication Details

Journal
Science Advances
Published
2025-10-15
DOI
https://doi.org/10.1126/sciadv.adx1686
Primary Topic
Optical properties and cooling technologies in crystalline materials
Type
article
Field-Weighted Citation Impact
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article

Giant single-step upconversion via sub–35-fs phonon dynamics in the nonlinear optical regime

Jingjing Yao, Yahui Li, Xiaoze Liu, Heyuan Liu et al.
Science Advances
Optical properties and cooling technologies in crystalline materials
article

Giant single-step upconversion via sub–35-fs phonon dynamics in the nonlinear optical regime

Jingjing Yao, Yahui Li, Xiaoze Liu, Heyuan Liu, Xia‐Guang Zhang, Enzheng Shi, Ming Xia, Qiu Wang, Jun Yi, Hailong Chen, Jeongmin Kim, Chong Hu
article en

Abstract

Phonon-assisted upconversion (UC) for anti-Stokes photoluminescence stands as a fundamental and widely studied process, central to both ultrafast electron-phonon coupling physics and diverse photonic applications. However, the ultrafast dynamics limit of UC has yet to be addressed, preventing its integration into the nonlinear optical regime. Here, we find a giant single-step UC of ~200 milli-electron volts via sub-35-femtosecond phonon dynamics in two-dimensional hybrid organic-inorganic perovskites in the nonlinear regime. The single-step UC approaches the phonon dynamics limit of ~23 femtoseconds and gains energy about eight times the room-temperature thermal energy (~25 milli-electron volts), enabling its synergistic integration into the nonlinear regime. Benefiting from the unique electron-phonon coupling between organic vibrations and excitons in inorganic lattices, the UC demonstrates distinctive signatures of Raman anisotropy and strong nonlinearity. This work opens new avenues for studying uncharted phonon dynamics and nonlinear optical mechanisms, offering substantial advantages in optical refrigeration, upconverting energy harvesting and optical microscopy.

Science AdvancesVol. 11(42)
Seoul National University (KR), Xiamen University (CN), Wuhan University of Technology (CN), Westlake University (CN), Wuhan University (CN), City University of Hong Kong, Shenzhen Research Institute (CN), Songshan Lake Materials Laboratory (CN), FZU ‒ Institute of Physics of the Academy of Sciences of the Czech Republic (CZ), Wuhan National Laboratory for Optoelectronics (CN), Tan Kah Kee Innovation Laboratory (CN), Collaborative Innovation Center of Chemistry for Energy Materials (CN), University of Chinese Academy of Sciences (CN), Xiamen University of Technology (CN), Henan Normal University (CN), Wuhan Institute of Technology (CN)
Openalex Percentile: Top 77%
Optical properties and cooling technologies in crystalline materials
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