Exploring nonequilibrium phases of photo-doped Mott insulators with generalized Gibbs ensembles

Many experiments show that strong excitations of correlated quantum materials can cause non-thermal phases without equilibrium analogues. Understanding the origin and properties of these nonequilibrium states has been challenging due to the limitations of theoretical methods for nonequilibrium strongly correlated systems. In this work, we introduce a generalized Gibbs ensemble description that enables a systematic analysis of the long-time behavior of photo-doped states in Mott insulators based on equilibrium methods. We demonstrate the power of the method by mapping out the nonequilibrium phase diagram of the one-dimensional extended Hubbard model, which features η-pairing and charge density wave phases in a wide photo-doping range. We furthermore clarify that the peculiar kinematics of photo-doped carriers, and the interaction between them, play an essential role in the formation of these non-thermal phases. Our results establish a new path for the systematic analysis of nonequilibrium strongly correlated systems.

Localized time accurate sampling of nonequilibrium and unsteady hypersonic flows: methods and horizons

Modern “non-intrusive” optical methods are providing revolutionary capabilities for diagnostics of hypersonic flow fields. They generate accurate information on the performance of ground test facilities and provide local time accurate measurements of near-wall and off-body flow fields surrounding hypersonic test articles. They can follow the true molecular motion of the flow and detect nonequilibrium states and gas mixtures. They can be used to capture a wide range of turbulent scales and can produce highly accurate velocity, temperature and density measurements as well as time-frozen images that provide intuitive understanding of flow phenomena. Recent review articles address many of these methods and their applications. The methods highlighted in this review are those that have been enabled or greatly improved by new, versatile laser systems, particularly including kHz rate femtosecond lasers and MHz rate pulse burst lasers. Although these methods can be applied to combusting environments, the focus of this review is on external high Mach number flows surrounding test articles and wind tunnel core flow properties. The high repetition rates enable rapid time evolving flows to be analyzed and enable the collection of large data sets necessary for statistical analysis. Future capabilities based on the use of atomic vapor filters and on frequency tunable, injection locked MHz rate lasers are promising.

Atom Probe Study of the Miscibility Gap in CuNi Thin Films and Microstructure Development

The unclear miscibility of CuNi alloys was investigated with atom probe tomography (APT). Multilayered thin film samples were prepared by ion beam sputtering (IBS) and focused ion beam (FIB) shaping. Long-term isothermal annealing treatments in a UHV furnace were conducted at temperatures of 573, 623, and 673 K to investigate the mixing process. The effective interdiffusion coefficient of the nanocrystalline microstructure (including defect diffusion) was determined to be Deff = 1.86 × 10−10 m2/s × exp(−164 kJ/mol/RT) by fitting periodic composition profiles through a Fourier series. In nonequilibrium states, microstructural defects like grain boundaries and precipitates were observed. While at the two higher temperatures total mixing is observed, a clear experimental evidence is found for a miscibility gap at 573 K with the boundary concentrations of 26 and 66 at%. These two compositions are used in a subregular solution model to reconstruct the phase miscibility gap. So, the critical temperature TC of the miscibility gap is found to be 608 K at a concentration of 45 at% Ni.

Origin of electroneutrality in living system

Identifying the first chemical transformations, from which life emerged is a central problem in the theories of life’s origins. These reactions would likely have been self-sustaining and self-reproductive before the advent of complex biochemical pathways found in modern organisms to synthesize lipid membranes, enzymes, or nucleic acids. Without lipid membranes and enzymes, exceedingly low concentrations of the organic intermediates of early metabolic cycles in protocells would have significantly hindered evolvability. To address this problem, we propose a mechanism, where a positive membrane potential elevates the concentration of the organic intermediates. In this mechanism, positively charged surfaces of protocell membranes due to accumulation of transition metals generate positive membrane potentials. We compute steady-state ion distributions and determine their stability in a protocell model to identify the key factors constraining achievable membrane potentials. We find that (i) violation of electroneutrality is necessary to induce nonzero membrane potentials; (ii) strategies that generate larger membrane potentials can destabilize ion distributions; and (iii) violation of electroneutrality enhances osmotic pressure and diminishes reaction efficiency, thereby driving the evolution of lipid membranes, specialized ion channels, and active transport systems.SignificanceThe building blocks of life are constantly synthesized and broken down through concurrent cycles of chemical transformations. Tracing these reactions back 4 billion years to their origins has been a long-standing goal of evolutionary biology. The first metabolic cycles at the origin of life must have overcome several obstacles to spontaneously start and sustain their nonequilibrium states. Notably, maintaining the concentration of organic intermediates at high levels needed to support their continued operation and subsequent evolution would have been particularly challenging in primitive cells lacking evolutionarily tuned lipid membranes and enzymes. Here, we propose a mechanism, in which the concentration of organic intermediates could have been elevated to drive early metabolic cycles forward in primitive cells with ion-permeable porous membranes under prebiotic conditions and demonstrate its feasibility in a protocell model from first principles.

Pushing the Limits of Luminescence Thermometry: Probing the Temperature of Proteins in Cells

Proteins are involved in numerous cellular activities such as transport and catalysis. Misfolding during biosynthesis and malfunctioning as a molecular machine may lead to physiological disorders and metabolic problems. Protein folding and mechanical work may be viewed as thermodynamic energetically favorable processes in which stochastic nonequilibrium intermediate states may be present with conditions such as thermal fluctuations. In my opinion, measuring those thermal fluctuations may be a way to access the energy exchange between the protein and the physiological environment and to better understand how those nonequilibrium states may influence the misfolding/folding process and the efficiency of the molecular engine cycle. Here, I discuss luminescence thermometry as a possible way to measure those temperature fluctuations from a single molecule experimental perspective with its current technical limitations and challenges.

Molecular Insight into the Possible Mechanism of Drag Reduction of Surfactant Aqueous Solution in Pipe Flow

The phenomenon of drag reduction (known as the “Toms effect”) has many industrial and engineering applications, but a definitive molecular-level theory has not yet been constructed. This is due both to the multiscale nature of complex fluids and to the difficulty of directly observing self-assembled structures in nonequilibrium states. On the basis of a large-scale coarse-grained molecular simulation that we conducted, we propose a possible mechanism of turbulence suppression in surfactant aqueous solution. We demonstrate that maintaining sufficiently large micellar structures and a homogeneous radial distribution of surfactant molecules is necessary to obtain the drag-reduction effect. This is the first molecular-simulation evidence that a micellar structure is responsible for drag reduction in pipe flow, and should help in understanding the mechanisms underlying drag reduction by surfactant molecules under nonequilibrium conditions.

Dynamically overridden systems for modeling of the two population processes with threshold effects

We have proposed a method for constructing dynamically redefined structures for the purpose of modeling abrupt changes in biological processes. The method provides for the analysis of scenarios with a control action, which is aimed at optimizing the profit from the exploitation of biological resources. The situations are described by three differential equations, which are numerically solved on adjacent time intervals. The state of the predicate set controls the selection of dynamically overridden coefficients. We carry out comparisons of all predicates on the basis of averaged individual indicators of generations. Threshold states in the dynamics of population size are a consequence of the selection of events as special nonequilibrium states that change the regulation algorithm. Our method makes it possible to implement dangerous qualitative changes in the scenarios of biological resource management, when the stable modes of their existence are suddenly lost. For practical problems, we have algorithmically implemented computational scenarios for two different processes such as the collapse of fish stocks under expert control of the fishery and a rapid outbreak of pests. The situation of the collapse of the fish population in the scenario with control develops in two stages and is a consequence of the experts 'desire to optimize the operation with uncertainty in an expert’s assessment of a state of a fishery. To confirm the relevance of our models, comparisons are made with the graphs of the development of the two real processes, as the spontaneous population explosion and the stock crisis during optimization of the sea cod fishery.