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Quasi-phase-matched up- and down-conversion in periodically poled layered semiconductors

Nature Photonics volume 19, pages 291–299 (2025)Cite this article

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Abstract

Nonlinear optics lies at the heart of classical and quantum light generation. The invention of periodic poling revolutionized nonlinear optics and its commercial applications by enabling robust quasi-phase-matching in crystals such as lithium niobate. However, reaching useful frequency conversion efficiencies requires macroscopic dimensions, limiting further technology development and integration. Here we realize a periodically poled van der Waals semiconductor (3R-MoS2). Owing to its large nonlinearity, we achieve a macroscopic frequency conversion efficiency of 0.03% at the relevant telecom wavelength over a microscopic thickness of 3.4 μm (that is, 3 poling periods), 10–100× thinner than current systems with similar performances. Due to intrinsic cavity effects, the thickness-dependent quasi-phase-matched second harmonic signal surpasses the usual quadratic enhancement by 50%. Further, we report the broadband generation of photon pairs at telecom wavelength via quasi-phase-matched spontaneous parametric down-conversion, showing a maximum coincidence-to-accidental ratio of 638 ± 75. This work opens the new and unexplored field of phase-matched nonlinear optics with microscopic van der Waals crystals, unlocking applications that require simple, ultra-compact technologies such as on-chip entangled photon-pair sources for integrated quantum circuitry and sensing.

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Fig. 1: PPTMDs.
Fig. 2: Quasi-phase-matched SHG from PPTMDs.
Fig. 3: Theoretical simulations of QPM in PPTMDs.
Fig. 4: PPTMD second harmonic conversion efficiency.
Fig. 5: Quasi-phase-matched SPDC from PPTMDs.

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Data availability

All data generated or analysed during this study that support the plots within this paper and other findings of this study are available via Zenodo at https://doi.org/10.5281/zenodo.13987619 (ref. 59). Source data are provided with this paper.

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Acknowledgements

We thank B. Ursprung for the useful discussions. This work was supported by Programmable Quantum Materials, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences, under award DE-SC0019443. C.T. acknowledges the European Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie PIONEER HORIZON-MSCA-2021-PF-GF grant agreement no. 101066108. C.T. also acknowledges the Optica Foundation and Coherent Inc. for supporting this research through the Bernard J. Couillaud Prize 2022. G.C. acknowledges support by the Progetti di ricerca di Rilevante Interesse Nazionale (PRIN) of the Italian Ministry of Research 2022HL9PRP Overcoming the Classical limits of ultRafast spEctroSCopy with ENtangleD phOtons (CRESCENDO). C.T. and G.C. acknowledge funding from the European Union–NextGenerationEU under the National Quantum Science and Technology Institute (NQSTI) grant no. PE00000023-q-ANTHEM-CUP H43C22000870001. A.M. acknowledges funding from the European Union–NextGenerationEU under the Italian Ministry of University and Research (MUR) National Innovation Ecosystem grant no. ECS00000041-VITALITY-CUP E13C22001060006, and Progetti di ricerca di Rilevante Interesse Nazionale (PRIN) of the Italian Ministry of Research PHOTO (Photonic Terahertz devices based on topological materials) no. 316 2020RPEPNH. A.Y. acknowledges support from the Department of Defense (DoD) through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program. J.P. acknowledges funding from the Air Force Office of Scientific Research (FA9550-21-1-0323) and the Office of Naval Research (N000142212841). P.W. acknowledges support from the Air Force Office of Scientific Research under award number FA8655-20-1-7030 (PhoQuGraph) and FA8655-23-1-7063 (TIQI). This research was funded in whole or in part by the Austrian Science Fund (FWF) (10.55776/F71). The financial support by the Austrian Federal Ministry of Labour and Economy, the National Foundation for Research, Technology and Development and the Christian Doppler Research Association is gratefully acknowledged. L.A.R. acknowledges support from the Erwin Schrödinger Center for Quantum Science and Technology (ESQ Discovery).

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Authors and Affiliations

  1. Department of Mechanical Engineering, Columbia University, New York, NY, USA

    Chiara Trovatello, Zhi Hao Peng, Xinyi Xu & P. James Schuck

  2. Dipartimento di Fisica, Politecnico di Milano, Milano, Italy

    Chiara Trovatello & Giulio Cerullo

  3. CNR-SPIN, c/o Dipartimento di Scienze Fisiche e Chimiche, L’Aquila, Italy

    Carino Ferrante & Andrea Marini

  4. Department of Physics, Columbia University, New York, NY, USA

    Birui Yang, D. N. Basov & Cory R. Dean

  5. Faculty of Physics, Vienna Center for Quantum Science and Technology (VCQ), University of Vienna, Vienna, Austria

    Josip Bajo, Benjamin Braun, Philipp K. Jenke, Philip Walther & Lee A. Rozema

  6. Faculty of Physics and Vienna Doctoral School in Physics, University of Vienna, Vienna, Austria

    Josip Bajo, Benjamin Braun & Philipp K. Jenke

  7. Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL, USA

    Andrew Ye & Jiwoong Park

  8. Department of Chemistry, Columbia University, New York, NY, USA

    Milan Delor

  9. James Franck Institute, University of Chicago, Chicago, IL, USA

    Jiwoong Park

  10. Department of Chemistry, University of Chicago, Chicago, IL, USA

    Jiwoong Park

  11. Christian Doppler Laboratory for Photonic Quantum Computer, University of Vienna, Vienna, Austria

    Philip Walther

  12. Department of Physical and Chemical Sciences, University of L’Aquila, L’Aquila, Italy

    Andrea Marini

  13. Istituto di Fotonica e Nanotecnologie, Consiglio Nazionale delle Ricerche, Milano, Italy

    Giulio Cerullo

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  1. Chiara Trovatello
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Contributions

C.T., G.C., and P.J.S. conceived the experiment. C.T. also conceived of the design and realization of the samples and performed the measurements. C.F. and A.M. developed the theory model. J.B., B.B., C.T. and P.K.J. performed the spontaneous parametric down-conversion measurements. B.Y., C.T., Z.H.P., X.X. and A.Y. prepared the samples. X.X., C.T. and Z.H.P. built the experimental set-up and performed the morphological characterization of the samples. M.D., D.N.B., J.P., L.A.R., P.W., C.R.D., G.C. and P.J.S. supervised the study. C.T. wrote the paper with input from all authors.

Corresponding authors

Correspondence to Chiara Trovatello, Lee A. Rozema, Giulio Cerullo or P. James Schuck.

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Nature Photonics thanks Maria Chekhova, Christiano de Matos, Qing Zhang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–12, discussion and Table 1.

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Experimental data of Fig. 3.

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Experimental data of Fig. 4.

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Experimental data of Fig. 5.

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Trovatello, C., Ferrante, C., Yang, B. et al. Quasi-phase-matched up- and down-conversion in periodically poled layered semiconductors. Nat. Photon. 19, 291–299 (2025). https://doi.org/10.1038/s41566-024-01602-z

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