Relationship between Population Dynamics and the Self-Energy in Driven Non-Equilibrium Systems

We compare the decay rates of excited populations directly calculated within a Keldysh formalism to the equation of motion of the population itself for a Hubbard-Holstein model in two dimensions. While it is true that these two approaches must give the same answer, it is common to make a number of simplifying assumptions within the differential equation for the populations that allows one to interpret the decay in terms of hot electrons interacting with a phonon bath. Here we show how care must be taken to ensure an accurate treatment of the equation of motion for the populations due to the fact that there are identities that require cancellations of terms that naively look like they contribute to the decay rates. In particular, the average time dependence of the Green's functions and self-energies plays a pivotal role in determining these decay rates.Comment: Submitted to Entrop

Quantum Eigenvector Continuation for Chemistry Applications

A typical task for classical and quantum computing in chemistry is finding a potential energy surface (PES) along a reaction coordinate, which involves solving the quantum chemistry problem for many points along the reaction path. Developing algorithms to accomplish this task on quantum computers has been an active area of development, yet finding all the relevant eigenstates along the reaction coordinate remains a difficult problem, and determining PESs is thus a costly proposal. In this paper, we demonstrate the use of a eigenvector continuation -- a subspace expansion that uses a few eigenstates as a basis -- as a tool for rapidly exploring potential energy surfaces. We apply this to determining the binding PES or torsion PES for several molecules of varying complexity. In all cases, we show that the PES can be captured using relatively few basis states; suggesting that a significant amount of (quantum) computational effort can be saved by making use of already calculated ground states in this manner.Comment: 13 pages, 8 figures, 3 pages of appendi

Creating stable Floquet-Weyl semimetals by laser-driving of 3D Dirac materials

Tuning and stabilising topological states, such as Weyl semimetals, Dirac semimetals, or topological insulators, is emerging as one of the major topics in materials science. Periodic driving of many-body systems offers a platform to design Floquet states of matter with tunable electronic properties on ultrafast time scales. Here we show by first principles calculations how femtosecond laser pulses with circularly polarised light can be used to switch between Weyl semimetal, Dirac semimetal, and topological insulator states in a prototypical 3D Dirac material, Na$_3$Bi. Our findings are general and apply to any 3D Dirac semimetal. We discuss the concept of time-dependent bands and steering of Floquet-Weyl points (Floquet-WPs), and demonstrate how light can enhance topological protection against lattice perturbations. Our work has potential practical implications for the ultrafast switching of materials properties, like optical band gaps or anomalous magnetoresistance. Moreover, we introduce Floquet time-dependent density functional theory (Floquet-TDDFT) as a general and robust first principles method for predictive Floquet engineering of topological states of matter.Comment: 21 pages, 4 figure

All-optical nonequilibrium pathway to stabilizing magnetic Weyl semimetals in pyrochlore iridates

Nonequilibrium many-body dynamics is becoming one of the central topics of modern condensed matter physics. Floquet topological states were suggested to emerge in photodressed band structures in the presence of periodic laser driving. Here we propose a viable nonequilibrium route without requiring coherent Floquet states to reach the elusive magnetic Weyl semimetallic phase in pyrochlore iridates by ultrafast modification of the effective electron-electron interaction with short laser pulses. Combining \textit{ab initio} calculations for a time-dependent self-consistent reduced Hubbard $U$ controlled by laser intensity and nonequilibrium magnetism simulations for quantum quenches, we find dynamically modified magnetic order giving rise to transiently emerging Weyl cones that are probed by time- and angle-resolved photoemission spectroscopy. Our work offers a unique and realistic pathway for nonequilibrium materials engineering beyond Floquet physics to create and sustain Weyl semimetals. This may lead to ultrafast, tens-of-femtoseconds switching protocols for light-engineered Berry curvature in combination with ultrafast magnetism.Comment: 27 pages including methods and supplementary information, 4 figures, 4 supplementary figure

On the Positive Definiteness of Response Functions in the Time Domain

Response functions of quantum systems, such as electron Green's functions, magnetic, or charge susceptibilities, describe the response of a system to an external perturbation. They are the central objects of interest in field theories and quantum computing and measured directly in experiment. Response functions are intrinsically causal. In equilibrium and steady-state systems, they correspond to a positive spectral function in the frequency domain. This article shows that response functions define an inner product on a Hilbert space and thereby induce a positive definite function. The properties of this function can be used to reduce noise in measured data and, in equilibrium and steady state, to construct positive definite extensions for data known on finite time intervals, which are then guaranteed to correspond to positive spectra