PHYSICAL REVIEW B 103, L041106 (2021) Letter Kinetic pathway facilitated by a phase competition to achieve a metastable electronic phase Keisuke Matsuura, 1 , * Hiroshi Oike , 1, 2 Vilmos Kocsis, 1 Takuro Sato, 1 Yasuhide Tomioka, 3 Yoshio Kaneko, 1 Masao Nakamura , 1 Yasujiro Taguchi , 1 Masashi Kawasaki, 1, 2 Yoshinori Tokura , 1, 2, 4 and Fumitaka Kagawa 1, 2 , † 1 RIKEN Center for Emergent Matter Science, Wako 351-0198, Japan 2 Department of Applied Physics and Quantum-Phase Electronics Center (QPEC), University of Tokyo, Tokyo 113-8656, Japan 3 National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba 305-8560, Japan 4 Tokyo College, University of Tokyo, Tokyo 113-8656, Japan (Received 7 October 2020; accepted 5 January 2021; published 14 January 2021) We show that ground state phase competition significantly decreases the critical cooling rate required for the kinetic avoidance of a first-order phase transition and thus facilitates the creation of metastable electronic states. This principle is revealed for the phase transition between antiferromagnetic charge-orbital-ordered insulating and ferromagnetic metallic states in the so-called colossal magnetoresistive manganite Nd 0.5 Sr 0.5 MnO 3 . In a phase competition situation, we achieve reversible and nonvolatile control of bulk magnetization by 1μ B /f .u. and resistivity by ∼1000% by applying electric pulses to exploit electric heating and subsequent rapid cooling. DOI: 10.1103/PhysRevB.103.L041106 The control of crystallization and vitrification from a liquid is significant [1], for instance, in metal alloys [2] and phase change materials [3–5], as these systems are used in both crystalline and glassy forms. When obtaining a metastable glassy form, a liquid should be rapidly cooled beyond a threshold rate, which is called the critical cooling rate. Thus, the constituent particles lack time to rearrange their ran- dom configuration to form crystal nuclei, and consequently, the first-order crystallization transition is kinetically avoided. These types of kinetic processes, which also involve thermally activated diffusion, are under nonequilibrium conditions, and therefore are seemingly an issue beyond the framework of thermodynamics. Extensive studies on glass-forming liquids and metal alloys, however, have revealed that the critical cool- ing rate for the crystallization transition is also related to the thermodynamic phase diagram, and this rate often becomes lowest near the eutectic point [6] and the triple point where two different crystalline forms coexist with a liquid [7–9]. Recently, there has been growing evidence that the ap- plication of rapid cooling beyond a critical cooling rate can have a remarkable impact on the electronic system with a first-order phase transition, resulting in a quenched high- temperature state at the lowest temperature [10–15]. Thus, the relationship between the critical cooling rate and the thermodynamic phase diagram is a current research topic in terms of the phase transition in the electronic degrees of freedom, which is usually irrelevant to the diffusion of atoms. In this study, we focus on perovskite-type manganese ox- ides [16–22], Nd 1−x Sr x MnO 3 , which have a phase diagram [Fig. 1(a)] consisting of paramagnetic metallic (PM-M), anti- ferromagnetic charge-orbital-ordered insulating (AFM-COI) and “charge-orbital-liquid” ferromagnetic metallic (FM-M) * keisuke.matsuura@riken.jp † kagawa@ap.t.u-tokyo.ac.jp phases. In particular, Nd 0.5 Sr 0.5 MnO 3 deserves special con- sideration in that the first-order transition can be induced by applying a magnetic field [23,24] [Fig. 1(b)], which is isother- mally variable even at low temperatures. Accordingly, in Nd 0.5 Sr 0.5 MnO 3 , the first-order phase transition is reversibly controllable with respect to the phase-control parameter (see Fig. S1 in Ref. [25]). Note that this is not the case for a first-order phase transition whose phase-control parameter is the chemical composition or pressure. To determine the critical cooling rate, whether the high- temperature FM-M phase can be quenched by rapid cooling at an experimentally feasible rate must first be determined. In this study, we used current-pulse-based rapid cooling, which utilizes a transient large thermal gradient between the pulse- heated sample and the low-temperature heat bath and thus enables rapid cooling of the sample on the order of 10 2 Ks −1 for bulk crystals. We performed simultaneous measurements of resistivity and bulk magnetization to detect a pulse-induced bulk phase transformation between the FM-M and AFM-COI phases. Figures 1(c) and 1(d) show the resistance- and magnetization-temperature profiles under a magnetic field of 5.5 T, respectively. Upon slow thermal cycling at ∼0.08 K s −1 , both quantities unambiguously indicate a first-order phase transition at ∼85 K upon cooling and 110 K upon heating [Figs. 1(c) and 1(d), dotted lines] between the high-temperature FM-M and low-temperature AFM-COI phases [24]. To perform rapid cooling from the high-temperature FM-M phase, we applied a current pulse of 7.0 × 10 5 Am −2 with a duration of 1 s to the sample at 5 K. Note that the energy supplied by the pulse is sufficiently large to heat the sample temperature above 110 K, and thus, rapid cooling from the high-temperature FM-M phase to 5 K is achieved, in the present case, at ∼150 K s −1 (see Fig. S2 in Ref. [25]). We then found that after the pulse application, the resistance is decreased by more than one order of magnitude, 2469-9950/2021/103(4)/L041106(5) L041106-1 ©2021 American Physical Society