Extreme Terahertz Nonlinear Phononics by Coherence-Imprinted Control of Hybrid Order
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| Main Authors: | , , , , , , , , , , , , , , |
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| Format: | Preprint |
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2026
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| _version_ | 1866911594598891520 |
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| author | Luo, Liang Khatri, Avinash Mootz, Martin Jiang, Tao Yang, Liu Chen, Zijing Huang, Chuankun Chong, Zhi Xiang Park, Joongmok Perakis, Ilias E. Wang, Zhiwei Yao, Yugui Xiang, Dao Yao, Yong-Xin Wang, Jigang |
| author_facet | Luo, Liang Khatri, Avinash Mootz, Martin Jiang, Tao Yang, Liu Chen, Zijing Huang, Chuankun Chong, Zhi Xiang Park, Joongmok Perakis, Ilias E. Wang, Zhiwei Yao, Yugui Xiang, Dao Yao, Yong-Xin Wang, Jigang |
| contents | Coherent control of quantum materials has progressed along two major fronts: nonlinear phononics, which reshapes lattices to induce emergent states, and Floquet engineering, which tailors electronic band reconstruction via time-periodic driving. Both mechanisms face fundamental limitations at terahertz (THz) frequencies: phononic nonlinearities are intrinsically weak in standard lattices, while electronic Floquet states are often constrained by rapid decoherence upon light-off and by a scarcity of coherence-resolved, multi-correlation probes beyond (quasi-)stationary band structures. Here we report an extreme THz nonlinear-phononics mechanism in $\text{Ta}_\text{2}\text{NiSe}_\text{5}$, where a highly susceptible non-equilibrium electronic correlation bath dramatically amplifies lattice nonlinearities under coherent driving. Utilizing THz two-dimensional spectroscopy as a coherence-tomography tool, we resolve an exceptionally rich landscape of approximately 30 distinct multi-order quantum pathways, including high-harmonic phonon generation, multi-quantum coherences, and multi-wave anharmonic cross-mode mixing. The density and complexity of this extreme manifold establishes a new benchmark for THz nonlinear phononics, as the multi-order quantum pathways surpass the limits of conventional lattice responses. These high-order signals collapse above ~100~K, defining an electronic correlation scale of a coherence-imprinted hybrid electronic-phonon order that governs the sustainability of high-order quantum correlations and nonlinear pathways beyond linear and equilibrium responses. Our results establish a route for correlation-boosted, phonon-anchored periodic Hamiltonian engineering and for certifying such periodically-driven states via multi-correlation coherence tomography. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2604_13429 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Extreme Terahertz Nonlinear Phononics by Coherence-Imprinted Control of Hybrid Order Luo, Liang Khatri, Avinash Mootz, Martin Jiang, Tao Yang, Liu Chen, Zijing Huang, Chuankun Chong, Zhi Xiang Park, Joongmok Perakis, Ilias E. Wang, Zhiwei Yao, Yugui Xiang, Dao Yao, Yong-Xin Wang, Jigang Strongly Correlated Electrons Materials Science Optics Coherent control of quantum materials has progressed along two major fronts: nonlinear phononics, which reshapes lattices to induce emergent states, and Floquet engineering, which tailors electronic band reconstruction via time-periodic driving. Both mechanisms face fundamental limitations at terahertz (THz) frequencies: phononic nonlinearities are intrinsically weak in standard lattices, while electronic Floquet states are often constrained by rapid decoherence upon light-off and by a scarcity of coherence-resolved, multi-correlation probes beyond (quasi-)stationary band structures. Here we report an extreme THz nonlinear-phononics mechanism in $\text{Ta}_\text{2}\text{NiSe}_\text{5}$, where a highly susceptible non-equilibrium electronic correlation bath dramatically amplifies lattice nonlinearities under coherent driving. Utilizing THz two-dimensional spectroscopy as a coherence-tomography tool, we resolve an exceptionally rich landscape of approximately 30 distinct multi-order quantum pathways, including high-harmonic phonon generation, multi-quantum coherences, and multi-wave anharmonic cross-mode mixing. The density and complexity of this extreme manifold establishes a new benchmark for THz nonlinear phononics, as the multi-order quantum pathways surpass the limits of conventional lattice responses. These high-order signals collapse above ~100~K, defining an electronic correlation scale of a coherence-imprinted hybrid electronic-phonon order that governs the sustainability of high-order quantum correlations and nonlinear pathways beyond linear and equilibrium responses. Our results establish a route for correlation-boosted, phonon-anchored periodic Hamiltonian engineering and for certifying such periodically-driven states via multi-correlation coherence tomography. |
| title | Extreme Terahertz Nonlinear Phononics by Coherence-Imprinted Control of Hybrid Order |
| topic | Strongly Correlated Electrons Materials Science Optics |
| url | https://arxiv.org/abs/2604.13429 |