When electrons in a solid are excited with light, they can alter the free energy landscape and access phases of matter that are beyond reach in thermal equilibrium. This accessibility becomes of vast importance in the presence of phase competition, when one state of matter is preferred over another by only a small energy scale that, in principle, is surmountable by light. Here, we study a layered compound, LaTe3, where a small in-plane (a-c plane) lattice anisotropy results in a unidirectional charge density wave (CDW) along the c-axis. Using ultrafast electron diffraction, we find that after photoexcitation, the CDW along the c-axis is weakened and subsequently, a different competing CDW along the a-axis emerges. The timescales characterizing the relaxation of this new CDW and the reestablishment of the original CDW are nearly identical, which points towards a strong competition between the two orders. The new density wave represents a transient non-equilibrium phase of matter with no equilibrium counterpart, and this study thus provides a framework for unleashing similar states of matter that are "trapped" under equilibrium conditions.
Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photo-induced transition of a model charge-densitywave (CDW) compound, LaTe3. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be quantitatively captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.In a second-order symmetry-breaking phase transition, the spatial extent of fluctuating regions diverges close to the critical temperature, T c . Correspondingly, the relaxation time of these fluctuations tends to infinity, a phenomenon known as critical slowing down [1,2]. The phenomenology of slowing dynamics near a critical point is much more general: it has been observed in first-order transitions [3,4], glasses [5,6], dynamical systems [7], and even microbial communities [8]. Its common occurrence makes it a robust signature of phase transitions in a vast array of complex systems [9].Close to equilibrium, critical slowing down has been well characterized in condensed matter systems. Theoretically, it is described by a dynamical critical exponent, whose value depends on the dynamic universality class [2]. Experimentally, the evidence comes from a vanishing rate of change in the order parameter close to T c , with early reports in refs. [3,10,11]. While these measurements probe the slowing dynamics in the time domain, it can be observed in the frequency domain as well. For example, inelastic neutron scattering has revealed a narrowing quasi-elastic peak along the energy axis as T c is approached, indicating a suppressed relaxation rate of critical fluctuations [12][13][14]. Moreover, if there is a collective mode associated with the phase transition, the mode softening in the vicinity of T c is also taken as a signature of critical slowing down [15].For symmetry-breaking phase transitions in a highly nonequilibrium setting, the dynamics are much less understood. Recent studies have found important features in nonequilibrium transitions, such as topological defects, which are absent in their equilibrium counterparts [16][17][18]. Despite the differences, a slowdown in dynamics is thought to carry over to systems far from equilibrium. For example, in a rapid...
We present a new method for a fast, unbiased and accurate representation of interatomic interactions. It is a combination of an artificial neural network and our new approach for pair potential reconstruction. The potential reconstruction method is simple and computationally cheap and gives rich information about interactions in crystals. This method can be combined with structure prediction and molecular dynamics simulations, providing accuracy similar to ab initio methods, but at a small fraction of the cost. We present applications to real systems and discuss the insight provided by our method.
Upon excitation by a laser pulse, broken-symmetry phases of a wide variety of solids demonstrate similar order parameter dynamics characterized by a dramatic slowing down of relaxation for stronger pump fluences. Motivated by this recurrent phenomenology, we develop a simple nonperturbative effective model for photoinduced dynamics of collective bosonic excitations. We find that as the system recovers after photoexcitation, it shows universal prethermalized dynamics manifesting a power-law, as opposed to exponential, relaxation, explaining the slowing down of the recovery process. For strong quenches, long-wavelength overpopulated transverse modes dominate the long-time dynamics; their distribution function exhibits universal scaling in time and space, whose universal exponents can be computed analytically. Our model offers a unifying description of order parameter fluctuations in a regime far from equilibrium, and our predictions can be tested with available time-resolved techniques.
We demonstrate that thermoelectric signal as well as dc Josephson current may be severely enhanced in multi-terminal superconducting hybrid nanostructures exposed to a temperature gradient. At temperatures T strongly exceeding the Thouless energy of our device both the supercurrent and the thermo-induced voltage are dominated by the contribution from non-equilibrium low energy quasiparticles and are predicted to decay slowly (algebraically rather than exponentially) with increasing T . We also predict a non-trivial current-phase relation and a transition to a π-junction state controlled by both the temperature gradient and the system topology. All these features are simultaneously observable in the same experiment.
We formulate a dynamical model to describe a photo-induced charge density wave (CDW) quench transition and apply it to recent multi-probe experiments on LaTe3 [A. Zong et al., Nat. Phys. 15, 27 (2019)]. Our approach relies on coupled time-dependent Ginzburg-Landau equations tracking two order parameters that represent the modulations of the electronic density and the ionic positions. We aim at describing the amplitude of the order parameters under the assumption that they are homogeneous in space. This description is supplemented by a three-temperature model, which treats separately the electronic temperature, temperature of the lattice phonons with stronger couplings to the electronic subsystem, and temperature of all other phonons. The broad scope of available data for LaTe3 and similar materials as well as the synergy between different time-resolved spectroscopies allow us to extract model parameters. The resulting calculations are in good agreement with ultrafast electron diffraction experiments, reproducing qualitative and quantitative features of the CDW amplitude evolution during the initial few picoseconds after photoexcitation.
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