A major challenge in condensed-matter physics is active control of quantum phases1,2. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible3,4,5. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility, where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic–lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.
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Nasu, K. Photoinduced Phase Transitions (World Scientific, 2004).
Zhang, J. & Averitt, R. D. Dynamics and control in complex transition metal oxides. Annu. Rev. Mater. Res. 44, 19–43 (2014).
Fausti, D. et al. Light-induced superconductivity in a stripe-ordered cuprate. Science 331, 189–191 (2011).
Stojchevska, L. et al. Ultrafast switching to a stable hidden quantum state in an electronic crystal. Science 344, 177–180 (2014).
Wang, Y. H., Steinberg, H., Jarillo-Herrero, P. & Gedik, N. Observation of Floquet–Bloch states on the surface of a topological insulator. Science 342, 453–457 (2013).
Rondinelli, J. M., May, S. J. & Freeland, J. W. Control of octahedral connectivity in perovskite oxide heterostructures: an emerging route to multifunctional materials discovery. MRS Bull. 37, 261–270 (2012).
Imada, M., Fujimori, A. & Tokura, Y. Metal–insulator transitions. Rev. Mod. Phys. 70, 1039–1263 (1998).
May, S. J. et al. Quantifying octahedral rotations in strained perovskite oxide films. Phys. Rev. B 82, 14110 (2010).
Liu, M. et al. Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial. Nature 487, 345–348 (2012).
Rini, M. et al. Control of the electronic phase of a manganite by mode-selective vibrational excitation. Nature 449, 72–74 (2007).
Miyano, K., Tanaka, T., Tomioka, Y. & Tokura, Y. Photoinduced insulator-to-metal transition in a perovskite manganite. Phys. Rev. Lett. 78, 4257–4260 (1997).
Takubo, N. et al. Persistent and reversible all-optical phase control in a manganite thin film. Phys. Rev. Lett. 95, 017404 (2005).
Ichikawa, H. et al. Transient photoinduced ‘hidden’ phase in a manganite. Nature Mater. 10, 101–105 (2011).
Asamitsu, A., Tomioka, Y., Kuwahara, H. & Tokura, Y. Current switching of resistive states in magnetoresistive manganites. Nature 388, 50–52 (1997).
Li, T. et al. Femtosecond switching of magnetism via strongly correlated spin-charge quantum excitations. Nature 496, 69–73 (2013).
Hwang, H. Y., Cheong, S.-W., Radaelli, P. G., Marezio, M. & Batlogg, B. Lattice effects on the magnetoresistance in doped LaMnO3 . Phys. Rev. Lett. 75, 914–917 (1995).
Ahn, K., Lookman, T. & Bishop, A. Strain-induced metal–insulator phase coexistence in perovskite manganites. Nature 804, 401–404 (2004).
Burgy, J., Moreo, A. & Dagotto, E. Relevance of cooperative lattice effects and stress fields in phase-separation theories for CMR manganites. Phys. Rev. Lett. 92, 097202 (2004).
Kiryukhin, V. et al. An X-ray-induced insulator–metal transition in a magnetoresistive manganite. Nature 386, 813–815 (1997).
Chakhalian, J., Millis, A. J. & Rondinelli, J. Whither the oxide interface. Nature Mater. 11, 92–94 (2012).
Nakamura, M., Ogimoto, Y., Tamaru, H., Izumi, M. & Miyano, K. Phase control through anisotropic strain in Nd0.5Sr0.5MnO3 thin films. Appl. Phys. Lett. 86, 182504 (2005).
Huang, Z. et al. Tuning the ground state of La0.67Ca0.33MnO3 films via coherent growth on orthorhombic NdGaO3 substrates with different orientations. Phys. Rev. B 86, 014410 (2012).
Wang, L. F. et al. Annealing assisted substrate coherency and high-temperature antiferromagnetic insulating transition in epitaxial La0.67Ca0.33MnO3/NdGaO3 (001) films. AIP Adv. 3, 52106 (2013).
Basov, D. N., Averitt, R. D., van der Marel, D., Dressel, M. & Haule, K. Electrodynamics of correlated electron materials. Rev. Mod. Phys. 83, 471–541 (2011).
Kovaleva, N. et al. Spin-controlled Mott–Hubbard bands in LaMnO3 probed by optical ellipsometry. Phys. Rev. Lett. 93, 147204 (2004).
Quijada, M., Černe, J., Simpson, J. & Drew, H. Optical conductivity of manganites: crossover from Jahn–Teller small polaron to coherent transport in the ferromagnetic state. Phys. Rev. B 58, 16093–16102 (1998).
Kim, K., Lee, S., Noh, T. & Cheong, S.-W. Charge ordering fluctuation and optical pseudogap in La1−xCaxMnO3 . Phys. Rev. Lett. 88, 167204 (2002).
Shin, T., Wolfson, J. W., Teitelbaum, S. W., Kandyla, M. & Nelson, K. A. Dual echelon femtosecond single-shot spectroscopy. Rev. Sci. Inst. 85, 83115 (2014).
Wall, S., Prabhakaran, D., Boothroyd, A. & Cavalleri, A. Ultrafast coupling between light, coherent lattice vibrations, and the magnetic structure of semicovalent LaMnO3 . Phys. Rev. Lett. 103, 097402 (2009).
Chatterji, T., Henry, P. & Ouladdiaf, B. Neutron diffraction investigation of the magneto-elastic effect in LaMnO3 . Phys. Rev. B 77, 212403 (2008).
R.D.A. and J.Z. acknowledge support from DOE—Basic Energy Sciences under Grant No. DE-FG02-09ER46643. X.T., F.J. and W.W. acknowledge support from the NSF of China (Grant No. 11274287), the National Basic Research Program of China (Grant Nos. 2012CB927402 and 2015CB921201) and from NSF of China (Grant Nos. 11474263 and U1432251). S.W.T. and K.A.N. acknowledge support from Office of Naval Research (N00014-12-1-0530) and the National Science Foundation (CHE-1111557). M.L., K.W.P. and D.N.B. are supported by DE-SC0012375 and DE-SC0012592. D.N.B. is the Moore Foundation Investigator in Quantum Materials, EPiQS Initiative GBMF4533.
The authors declare no competing financial interests.
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Zhang, J., Tan, X., Liu, M. et al. Cooperative photoinduced metastable phase control in strained manganite films. Nature Mater 15, 956–960 (2016). https://doi.org/10.1038/nmat4695
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