Chirality-selective second-harmonic response with Floquet engineering
Symmetry breaking profoundly influences the macroscopic physical properties of materials. For instance, inversion symmetry breaking in monolayer transition metal dichalcogenides enables the emergence of chiral selection rules, featuring distinct optical chirality-selective electronic properties. Here, we demonstrate ultrafast, coherent manipulation of chirality-selective nonlinear optics in monolayer molybdenum disulfide (MoS 2 ) through time-reversal symmetry breaking via Floquet engineering. By using sub-bandgap, circularly polarized ultrafast optical pulses, we introduce nondegenerate, chirality-selective optical Stark and Bloch-Siegert shifts. This approach effectively lifts the energy degeneracy, leading to pronounced chirality-selective second-harmonic generation. Furthermore, we reveal that the Floquet-engineered chirality-selective states can be finely tuned using optical parameters such as intensity and chirality. Our results show a method for manipulating the energy degree of freedom, paving the way for ultrafast nonlinear photonics.
Authors
- Zhipei Sun (ORCID: https://orcid.org/0000-0002-9771-5293)
- Yi Zhang (ORCID: https://orcid.org/0000-0002-1704-4144)
- Youqiang Huang (ORCID: https://orcid.org/0009-0000-3809-1647)
- Xuetao Gan (ORCID: https://orcid.org/0000-0003-2469-5807)
- F. Javier Garcı́a de Abajo (ORCID: https://orcid.org/0000-0002-4970-4565)
- Luojun Du (ORCID: https://orcid.org/0000-0002-2420-8258)
- Dong Mao (ORCID: https://orcid.org/0000-0002-5744-6316)
- Xueyin Bai (ORCID: https://orcid.org/0000-0002-2254-5701)
- Nianze Shang (ORCID: https://orcid.org/0000-0001-5840-1024)
- Peng Li (ORCID: https://orcid.org/0000-0001-8780-5554)
- Jianlin Zhao (ORCID: https://orcid.org/0000-0002-4619-1215)
- Sheng Meng (ORCID: https://orcid.org/0000-0002-1553-1432)
- Haijun Cao
Institutions
- Institució Catalana de Recerca i Estudis Avançats (ES)
- Northwestern Polytechnical University (CN)
- Institute of Photonic Sciences (ES)
- Chinese Academy of Sciences (CN)
- Barcelona Institute of Science and Technology (ES)
- Institute of Physics (CN)
- University of Chinese Academy of Sciences (CN)
- Ministry of Industry and Information Technology (CN)
- Aalto University (FI)
Publication Details
- Journal
- Science Advances
- Published
- 2026-10-30
- DOI
- https://doi.org/10.1126/sciadv.aed6149
- Primary Topic
- Laser-Matter Interactions and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Natural Science Foundation of China