Glass-like rare-earth doped fluoride single crystal for high repetition rate high energy lasers

Junyang Liu; Junye Yang; Hao Wu; Yanyan Xue; Zhen Zhang; Qinghui Wu; Dapeng Jiang; Jie Chen; Fengkai Ma; Liangbi Su

doi:10.59717/j.xinn-mater.2026.100217

The Innovation Materials > 2026 Vol. 4 > No. 3 > 100217

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Glass-like rare-earth doped fluoride single crystal for high repetition rate high energy lasers

1.
State Key Laboratory of Functional Crystals and Devices, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China
2.
Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
3.
Spallation Neutron Source Science Center (SNSSC), Dongguan 523803, China
4.
Guangdong Provincial Engineering Research Center of Crystal and Laser Technology, Department of Optoelectronic Engineering, Jinan University, Guangzhou 510632, China
5.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

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These authors contributed equally to this work.
Corresponding authors: chenjie@ihep.ac.cn (J.C.); mafengkai@jnu.edu.cn (F.M.); suliangbi@mail.sic.ac.cn (L.S.)
Received Date: December 11, 2025

Accepted Date: May 06, 2026

Published Online: May 06, 2026

The Innovation Materials 4(3), https://doi.org/10.59717/j.xinn-mater.2026.100217 | Cite this article

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1. The glass-like structure with long-range ordered and short-range disordered is revealed in single crystal.
  
  Crystal with high thermal conductivity and broad bandwidth for high repetition rate ultra-fast laser is grown.
  
  Crystals range from low to high entropy doped with single element are revealed.

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ABSTRACT

Broad spectral bandwidth and high thermal conductivity are prerequisites for achieving high-repetition-rate ultrafast lasers. However, these properties are generally mutually exclusive and pose a persistent challenge in the field of laser materials. In this work, the reported rare-earth fluoride crystal is selected as laser gain materials. Through neutron diffraction, synchrotron radiation X-ray absorption spectroscopy and simulation calculations, a special structure with long-range order and short-range disorder in rare-earth-doped fluoride crystals is revealed for the first time. In the structure, anionic defects are randomly distributed around the activator ions, exhibiting glass-like disordered characteristics. The unique structure enables neodymium-doped fluoride crystals to reconcile the conflicting properties of broad spectrum and high thermal conductivity. Meanwhile, the successful growth of large-size crystals, coupled with the preliminary laser amplification, demonstrates that the developed neodymium-doped fluorites are promising candidates for high-repetition-rate ultrafast lasers.

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[1]	Clark E., Krushelnick K., Zepf M., et al. (2000). Energetic heavy-ion and proton generation from ultraintense laser-plasma interactions with solids. Phys. Rev. Lett. 85:1654. DOI:10.1103/physrevlett.85.1654 View in Article CrossRef Google Scholar
[2]	Huang K., Jin Z., Nakanii N., et al. (2024). Electro-optic 3D snapshot of a laser wakefield accelerated kilo-ampere electron bunch. Light: Sci. Appl. 13:84. DOI:10.1038/s41377-024-01440-2 View in Article CrossRef Google Scholar
[3]	Meron O., Arieli U., Bahar E., et al. (2025). Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses. Light: Sci. Appl. 14:80. DOI:10.1038/s41377-025-01748-7 View in Article CrossRef Google Scholar
[4]	Keller U. (2003). Recent developments in compact ultrafast lasers. Nature 424:831−838. DOI:10.1038/nature01938 View in Article CrossRef Google Scholar
[5]	Fan J. J., Ou Z. Y. and Zhang Z. (2024). Entangled photons enabled ultrafast stimulated Raman spectroscopy for molecular dynamics. Light: Sci. Appl. 13:163. DOI:10.1038/s41377-024-01492-4 View in Article CrossRef Google Scholar
[6]	Südmeyer T., Marchese S., Hashimoto S., et al. (2008). Femtosecond laser oscillators for high-field science. Nat. Photonics 2:599−604. DOI:10.1038/nphoton.2008.194 View in Article CrossRef Google Scholar
[7]	Garanin S. G. and Krokhin O. N. (2011). High-power lasers and laser fusion. Herald Russ. Acad. Sci. 81:204−210. DOI:10.1134/s1019331611030129 View in Article CrossRef Google Scholar
[8]	Temporal M., Canaud B., Garbett W. J., et al. (2014). Irradiation uniformity at the laser megaJoule facility in the context of the shock ignition scheme. High Power Laser Sci. Eng. 2:e8. DOI:10.1017/hpl.2014.12 View in Article CrossRef Google Scholar
[9]	Niu S., Wang W., Liu P., et al. (2024). Recent advances in applications of ultrafast lasers. Photonics 11:857. DOI:10.3390/photonics11090857 View in Article CrossRef Google Scholar
[10]	Li Y., Chen L., Chen M., et al. (2025). High-intensity lasers and research activities in China. High Power Laser Sci. Eng. 13:e12. DOI:10.1017/hpl.2024.69 View in Article CrossRef Google Scholar
[11]	Aus der Au J., Kopf D., Morier-Genoud F., et al. (1997). 60-fs pulses from a diode-pumped Nd: Glass laser. Opt. Lett. 22:307−309. DOI:10.1364/ol.22.000307 View in Article CrossRef Google Scholar
[12]	Gaul E. W., Martinez M., Blakeney J., et al. (2010). Demonstration of a 1.1 petawatt laser based on a hybrid optical parametric chirped pulse amplification/mixed Nd: glass amplifier. Appl. Opt. 49:1676-1681. DOI:10.1364/ao.49.001676. View in Article Google Scholar
[13]	Yang S., Yin D., Gan Z., et al. (2020). Thermal effect of high energy repetition rate Nd:glass laser. Chin. Opt. Lett. 47:0901004. DOI:10.3788/cjl202047.0901004 View in Article CrossRef Google Scholar
[14]	Maker G. and Ferguson A. (1989). Frequency-modulation mode locking of a diode-pumped Nd: YAG laser. Opt. Lett. 14:788−790. DOI:10.1364/ol.14.000788 View in Article CrossRef Google Scholar
[15]	Norvig P., Relman D. A., Goldstein D. B., et al. (2010). 2020 visions. Nature 463:26−32. DOI:10.1038/463026a View in Article CrossRef Google Scholar
[16]	Yu Z., Zhao J., Yang Z., et al. (2024). A novel PiGF@ diamond color converter with a record thermal conductivity for laser-driven projection display. Adv. Mater. 36:e2406147. DOI:10.1002/adma.202406147 View in Article CrossRef Google Scholar
[17]	Penilla E. H., Devia-Cruz L. F., Duarte M. A., et al. (2018). Gain in polycrystalline Nd-doped alumina: Leveraging length scales to create a new class of high-energy, short pulse, tunable laser materials. Light: Sci. Appl. 7:33. DOI:10.1038/s41377-018-0023-z View in Article CrossRef Google Scholar
[18]	Qin Z., Xie G., Ma J., et al. (2014). Generation of 103 fs mode-locked pulses by a gain linewidth-variable Nd, Y: CaF₂ disordered crystal. Opt. Lett. 39:1737−1739. DOI:10.1364/ol.39.001737 View in Article CrossRef Google Scholar
[19]	Chen J., Peng Y., Zhang Z., et al. (2017). Demonstration of a diode pumped Nd, Y co-doped SrF2 crystal based, high energy chirped pulse amplification laser system. Opt. Commun. 382:201−204. DOI:10.1016/j.optcom.2016.07.008 View in Article CrossRef Google Scholar
[20]	Kamat H., Wang F., Barnsley K. E., et al. (2021). Insight into the partitioning and clustering mechanism of rare-earth cations in alkali aluminoborosilicate glasses. Chem. Mater. 33:7944−7963. DOI:10.1021/acs.chemmater.1c01352 View in Article CrossRef Google Scholar
[21]	Zhang Z., Ma F., Jiang D., et al. (2025). Laser crystals from combination paradigm to local structure design: A review on rational design principles, spectroscopic properties and laser applications. Mater. Sci. Eng. R-Rep. 162:100869. DOI:10.1016/j.mser.2024.100869 View in Article CrossRef Google Scholar
[22]	Lu Y., Liu L., Gao R., et al. (2024). Ultrafast near-infrared pyroelectric detector based on inhomogeneous plasmonic metasurface. Light: Sci. Appl. 13:241. DOI:10.1038/s41377-024-01572-5 View in Article CrossRef Google Scholar
[23]	Liu P., Zhao Y., Wang X., et al. (2024). Study on lattice dynamics and thermal conductivity of fluorite AF₂ (A= Ca, Sr, Ba) based on first principles calculations. Phys. Chem. Chem. Phys. 26:10868−10879. DOI:10.1039/d4cp00201f View in Article CrossRef Google Scholar
[24]	Yongzong Z. (1986). Growth of high quality large Nd: YAG crystals by temperature gradient technique (TGT). J. Cryst. Growth 78:31−35. DOI:10.1016/0022-0248(86)90497-5 View in Article CrossRef Google Scholar
[25]	Oishi R., Yonemura M., Nishimaki Y., et al. (2009). Rietveld analysis software for J-PARC. Nucl. Instrum. Methods Phys. Res., Sect. A 600:94−96. DOI:10.1016/j.nima.2008.11.056 View in Article CrossRef Google Scholar
[26]	Ravel B. and Newville M. (2005). ATHENA, ARTEMIS, HEPHAESTUS: Data analysis for X-ray absorption spectroscopy using IFEFFIT. J. Synchrotron Radiat. 12:537−541. DOI:10.1107/s0909049505012719 View in Article CrossRef Google Scholar
[27]	Rehr J. J., Kas J. J., Vila F. D., et al. (2010). Parameter-free calculations of X-ray spectra with FEFF9. Phys. Chem. Chem. Phys. 12:5503−5513. DOI:10.1039/b926434e View in Article CrossRef Google Scholar
[28]	Sato Y. and Taira T. (2025). Augmented spectrum bandwidth of Nd-doped garnet and bixbyite by spectrum tailoring. Opt. Express 33:24050−24059. DOI:10.1364/oe.554538 View in Article CrossRef Google Scholar
[29]	Wang B., Jiang H., Jia X., et al. (2008). Thermal conductivity of doped YAG and GGG laser crystal. Front. Optoelectron. 1:138−141. DOI:10.1007/s12200-008-0049-6 View in Article CrossRef Google Scholar
[30]	Fan Z.-W., Qiu J.-S., Kang Z.-J., et al. (2017). High beam quality 5 J, 200 Hz Nd: YAG laser system. Light: Sci. Appl. 6:e17004−e17004. DOI:10.1038/lsa.2017.4 View in Article CrossRef Google Scholar
[31]	Agnesi A., Greborio A., Pirzio F., et al. (2011). Femtosecond Nd: glass lasers pumped by single-mode laser diodes and mode locked with carbon nanotube or semiconductor saturable absorber mirrors. IEEE J. Sel. Top. Quantum Electron. 18:74−80. DOI:10.1109/jstqe.2011.2104941 View in Article CrossRef Google Scholar
[32]	Naito K., Yamanaka M., Nakatsuka M., et al. (1992). Conceptual design studies of a laser diode pumped solid state laser system for the laser fusion reactor driver. Jpn. J. Appl. Phys. 31:259. DOI:10.1143/jjap.31.259 View in Article CrossRef Google Scholar
[33]	Kuzmin A. A., Khazanov E. A., Kulagin O. V., et al. (2014). Neodymium glass laser with a phase conjugate mirror producing 220 J pulses at 0.02 Hz repetition rate. Opt. Express 22:20842-20855. DOI:10.1364/oe.22.020842 View in Article Google Scholar
[34]	Catlow C. R. A., Chadwick A. V., Greaves G. N., et al. (1984). Direct observations of the dopant environment in fluorites using EXAFS. Nature 312:601−604. DOI:10.1038/312601a0 View in Article CrossRef Google Scholar
[35]	Solari S. F., Poon L. N., Wörle M., et al. (2022). Stabilization of lead-reduced metal halide perovskite nanocrystals by high-entropy alloying. J. Am. Chem. Soc. 144:5864−5870. DOI:10.1021/jacs.1c12294 View in Article CrossRef Google Scholar
[36]	Shannon R. D. (1976). Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr., Sect. A: Found. Crystallogr. 32:751−767. DOI:10.1107/S0567739476001551 View in Article CrossRef Google Scholar
[37]	Cheetham A. K., Fender B. E. F. and Cooper M. J. (1971). Defect structure of calcium fluoride containing excess anions I. Bragg scattering. J. Phys. C: Solid State Phys. 4:3107. DOI:10.1088/0022-3719/4/18/016 View in Article CrossRef Google Scholar
[38]	Hull S. and Wilson C. C. (1992). The defect structure of anion-excess (Ca_1−xY_x)F_2+x with x= 0.06. J. Solid State Chem. 100:101-114. DOI:10.1016/0022-4596(92)90159-s. View in Article Google Scholar
[39]	Dudka A. P., Sobolev B. P. and Simonov V. I. (2013). Discovery of difference in the diffuse scattering from nonstoichiometric Ca_0.87La_0.13F_2.13 and Ca_0.92Er_0.08F_2.08 crystals with different types of clusters of structural defects. Crystallogr. Rep. 58:822-828. DOI:10.1134/s1063774513060084 View in Article Google Scholar
[40]	Lacroix B., Genevois C., Doualan J. L., et al. (2014). Direct imaging of rare-earth ion clusters in Yb:CaF₂. Phys. Rev. B 90:125124. DOI:10.1103/physrevb.90.125124 View in Article CrossRef Google Scholar
[41]	Bevan D. J. M., Greis O. and Strähle J. (1980). A new structural principle in anion-excess fluorite-related superlattices. Acta Crystallogr., Sect. A:Found. Adv. 36:889−890. DOI:10.1107/S0567739480001878 View in Article CrossRef Google Scholar
[42]	Krahl T., Scholz G. and Kemnitz E. (2014). Solid solutions CaF₂–YF₃ with fluorite structure prepared on the Sol–Gel route: investigation by multinuclear MAS NMR spectroscopy. J. Phys. Chem. C 118:21066−21074. DOI:10.1021/jp505616f View in Article CrossRef Google Scholar
[43]	Liu J., Wang Y., Zhang Z., et al. (2023). Insight into neodymium clusters and spectroscopic properties in CaF₂ single crystals. Opt. Mater. Express 13:2288−2301. DOI:10.1364/ome.494068 View in Article CrossRef Google Scholar
[44]	Ma F., Zhou H., Tang Q., et al. (2022). Clusters modification for tunable photoluminescence in Nd³⁺:SrF₂ crystal. J. Alloys Compd. 899:162913. DOI:10.1016/j.jallcom.2021.162913 View in Article CrossRef Google Scholar
[45]	Sulyanova E. A., Karimov D. N. and Sobolev B. P. (2020). Nanostructured crystals of fluorite phases Sr_1–xR_xF_2+x (R are rare-earth elements) and their ordering. 16: Defect structure of the nonstoichiometric phases Sr_1–xR_xF_2+x (R= Pr, Tb–Yb) as grown. Crystallogr. Rep. 65:560-565. DOI:10.1134/s1063774520040215 View in Article Google Scholar
[46]	Danilkin S. A. (2009). Diffuse scattering and lattice dynamics of superionic copper chalcogenides. Solid State Ionics 180:483−487. DOI:10.1016/j.ssi.2008.06.012 View in Article CrossRef Google Scholar
[47]	Liu Z. Y., Liu Y., Xu Y. J., et al. (2023). Novel high-entropy oxides for energy storage and conversion: From fundamentals to practical applications. Green Energy Environ. 8:1341−1357. DOI:10.1016/j.gee.2023.04.007 View in Article CrossRef Google Scholar
[48]	Salian A. and Mandal S. (2022). Entropy stabilized multicomponent oxides with diverse functionality–a review. Crit. Rev. Solid State Mater. Sci. 47:142−193. DOI:10.1080/10408436.2021.1886047 View in Article CrossRef Google Scholar
[49]	Ma X., Ding B., Yang Z., et al. (2024). Sulfur-vacancy-engineered two-dimensional Cu@SnS_2–x nanosheets constructed via heterovalent substitution for high-efficiency piezocatalytic tumor therapy. J. Am. Chem. Soc. 146:21496−21508. DOI:10.1021/jacs.4c04385 View in Article CrossRef Google Scholar
[50]	Mi J., Chen L., Ma J., et al. (2024). Defect strategy in solid‐state lithium batteries. Small Methods 8:2301162. DOI:10.1002/smtd.202301162 View in Article CrossRef Google Scholar
[51]	Popov P., Fedorov P. and Osiko V. (2014). Thermal conductivity of single crystals of the Ca_1−xY_xF_2+x solid solution. Dokl. Phys. 59:199−202. DOI:10.1134/s1028335814050036 View in Article CrossRef Google Scholar
[52]	Kotrbová L., Uhlířová T., Pabst W., et al. (2025). Thermal conductivity of silica refractories and its temperature dependence during thermal cycling, compared to silicite and sandstone. Open Ceram. 21:100735. DOI:10.1016/j.oceram.2025.100735 View in Article CrossRef Google Scholar
[53]	Nolas G. S., Wang D. and Beekman M. (2007). Transport properties of polycrystalline Mg2Si1-ySby (0≤y<0.4). Phys. Rev. B 76:235204. DOI:10.1103/PhysRevB.76.235204 View in Article Google Scholar
[54]	Toberer E. S., Baranowski L. L. and Dames C. (2012). Advances in thermal conductivity. Annu. Rev. Mater. Res. 42:179-209. DOI:10.1146/annurev-matsci-070511-155040 View in Article Google Scholar
[55]	Liu Y., Zhang Z., Yan X., et al. (2025). Highly efficient atomic-scale design of CaF₂ for ultrafast fluoride-ion conduction. J. Mater. Chem. A. 13:24656-24664. DOI:10.1039/D5TA01953B View in Article Google Scholar
[56]	Zhang Z., Tan L., Zhou Y., et al. (2025). Anisotropic plasticity and fracture mechanisms of single-crystal CaF₂ under indentation: Insights from crystal plasticity simulation and experiment. J. Mater. Res. Technol. 39:6435-6447. DOI:10.1016/j.jmrt.2025.11.003 View in Article Google Scholar
[57]	Sato Y. and Taira T. (2005). Comparative study on the spectroscopic properties of Nd:GdVO₄ and Nd:YVO₄ with hybrid process. IEEE J. Sel. Top. Quantum Electron. 11:613−620. DOI:10.1109/jstqe.2005.850569 View in Article CrossRef Google Scholar
[58]	Matthews D. G., Boon J. R., Conroy R. S., et al. (1996). A comparative study of diode pumped microchip laser materials: Nd-doped YVO₄, YOS, SFAP and SVAP. J. Mod. Opt. 43:1079−1087. DOI:10.1080/09500349608233268 View in Article CrossRef Google Scholar
[59]	Wetter N. (2013). Neodymium doped lithium yttrium fluoride (Nd:YLiF₄) lasers. Handbook of solid-state lasers (Elsevier). pp:323-340. DOI:10.1533/9780857097507.2.323 View in Article Google Scholar
[60]	Koechner W. (2013). Solid-state laser engineering (Springer). https://books.google.com/books?hl=en&lr=&id=NtjqCAAAQBAJ&oi=fnd&pg=PA1&dq=Koechner+W.+(2013).+Solid+-+state+laser+engineering&ots=SkB1rEC5Fk&sig=avp79I09uIpXDCE-eYoFnUm0qsI#v=onepage&q=Koechner%20W.%20(2013).%20Solid%20-%20state%20laser%20engineering&f=false View in Article Google Scholar
[61]	Catlow C. R. A., Chadwick A. V., Corish J., et al. (1989). Defect structure of doped CaF₂ at high temperatures. Phys. Rev. B 39:1897. DOI:10.1103/physrevb.39.1897 View in Article CrossRef Google Scholar

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Liu J., Yang J., Wu H., et al. (2026). Glass-like rare-earth doped fluoride single crystal for high repetition rate high energy lasers. The Innovation Materials 4:100217. https://doi.org/10.59717/j.xinn-mater.2026.100217

Liu J., Yang J., Wu H., et al. (2026). Glass-like rare-earth doped fluoride single crystal for high repetition rate high energy lasers. The Innovation Materials 4:100217. https://doi.org/10.59717/j.xinn-mater.2026.100217

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Glass-like rare-earth doped fluoride single crystal for high repetition rate high energy lasers

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