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Register a new userMulti-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase
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Spontaneous C4-symmetry breaking phases are ubiquitous in layered quantum materials and compete with other phases such as superconductivity. Phenomena like light induced superconductivity and metallicity are believed to arise from optical excitations selectively melting the C4-symmetry breaking phase, enabling competing phases to emerge. Phenomenological models suggest that light directly modifies the order parameter or its potential. However, clear evidence for such a process is lacking. Here, we measure the order parameter dynamics of the C4 symmetry breaking transition in the prototypical manganite La0.5Sr1.5MnO4. Despite some degrees of freedom appearing to show a coherent response and critical slowing, consistent with previous measurements, we find the order-parameter is overdamped and incoherent. Concomitant changes in the lattice potential of the entire system in under ~25 fs show rapid energy redistribution and lack of selectivity in photoexcitation, suggesting a disorder-driven transition where the order parameter potential plays a minimal role, in contrast to previous models.
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The conductivity and magnetization of Fe1-xCoxS2 were measured to investigate quantum critical behavior in disordered itinerant magnets. Small x (<0.001) is required to convert insulating iron pyrite into a metal, followed by a paramagnetic-to-ferromagnetic metal transition at x = 0.032+/-0.004. Singular contributions are discovered that are distinct from those at either metal-insulator or magnetic transitions. Our data reveal that disorder and low carrier density associated with proximity to a metal-insulator transition fundamentally modifies the critical behavior of the magnetic transition.
We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales.
The ability to probe symmetry breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-THz response of the model stripe compound La$_{1.75}$Sr$_{0.25}$NiO$_{4}$, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen - as witnessed by time-delayed suppression of zone-folded Ni-O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. The hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry breaking dynamics in solids.
In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced $d^{1}d^{0}$ $xrightarrow{}$ $d^{0}d^{1}$ excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods -- both femtosecond resonant x-ray diffraction and optical reflectivity -- to demonstrate that the orbital response in the layered manganite Nd$_{1-x}$Sr$_{1+x}$MnO$_{4}$ ($it{x}$ = 2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical $d^{1}d^{0}$ $xrightarrow{}$ $d^{0}d^{1}$ transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the $d^{0}$ $ xrightarrow{}$ $d^{1}L$, where $it{L}$ denotes a hole in the oxygen band. This novel finding may pave a new avenue for selectively manipulating specific types of order in complex materials of this class.
The B20 chiral magnets with broken inversion symmetry and C4 rotation symmetry have attracted much attention. The broken inversion symmetry leads to the Dzyaloshinskii-Moriya that gives rise to the helical and Skyrmion states. We report the unusual magnetoresistance (MR) of B20 chiral magnet Fe0.85Co0.15Si that directly reveals the broken C4 rotation symmetry. We present a microscopic theory, a minimal theory with two spin-orbit terms, that satisfies all the symmetry requirements and accounts for the transport experiments.
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