The two-particle problem within a nonequilibrium many-particle system is investigated in the framework of real-time Green's functions. Starting from the nonequilibrium Bethe-Salpeter equation on the Keldysh contour, a Dyson equation is given for two-time two-particle Green's functions. Thereby the well-known Kadanoff-Baym equations are generalized to the case of two-particle functions. The two-time structure of the equations is achieved in an exact way using the semigroup property of the free-particle propagators. The frequently used Shindo approximation is thus avoided. It turns out that results obtained earlier are valid only in limiting cases of a nondegenerate system or a static interaction, respectively. For the case of thermodynamic equilibrium, the differences to former results obtained for the effective two-particle Hamiltonian are discussed.
The nonequilibrium description of quantum systems requires, for more than two or three particles, the use of a reduced description to be numerically tractable. Two possible approaches are based on either reduced density matrices or nonequilibrium Green functions (NEGF). Both concepts are formulated in terms of hierarchies of coupled equations—the Bogoliubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchy for the reduced density operators and the Martin-Schwinger-hierarchy (MS) for the Green functions, respectively. In both cases, similar approximations are introduced to decouple the hierarchy, yet still many questions regarding the correspondence of both approaches remain open. Here we analyze this correspondence by studying the generalized Kadanoff–Baym ansatz (GKBA) that reduces the NEGF to a single-time theory. Starting from the BBGKY-hierarchy we present the approximations that are necessary to recover the GKBA result both, with Hartree-Fock propagators (HF-GKBA) and propagators in second Born approximation. To test the quality of the HF-GKBA, we study the dynamics of a 4-electron Hubbard nanocluster starting from a strong nonequilibrium initial state and compare to exact results and the Wang-Cassing approximation to the BBGKY hierarchy presented recently by Akbari et al. [1].
The method of nonequilibrium Green functions (NEGFs) constitutes a solid framework to describe closed and open quantum systems. It captures situations far from equilibrium including arbitrary perturbations and correlations - effects higher than first order in the binary interactions. On the contrary, in the absence of external fields, it reduces to the imaginary-time Matsubara formalism. The abilities (and successes) of the method originate from its self-consistency and the conserving character of many-body approximations that are introduced by diagram technique. On this account, NEGFs have, now for a long time, brought insight into the dynamics of nuclear matter, non-ideal quantum gases and (semiconductor) plasmas. However, applications to localized, finite and strongly interacting systems have emerged only within the recent decade. The dynamical properties follow from quantum kinetic equations - the two-time Kadanoff-Baym equations for the one-particle NEGF - the numerical solution of which is the central topic of this thesis. The non-Markovian structure of these equations thereby inhibits an unlimited, gradual propagation of the nonequilibrium Green function: Any self-consistent, future dynamics of the system is tightly linked to the (complete) past by non-local self-energies. Further, the success in obtaining solutions is being diminished if the system under investigation is not isotropic or inhomogeneous and, in addition, the spatial topology (e.g., the charge carrier or spin density) needs to be resolved in time. On top of this, small isolated systems are generally not candidates showing fast decoherence which offers little hope for smooth and well-damped integration kernels. Despite these difficulties, the thesis at hand is devoted to the computation of the two-time NEGF for finite, closed systems of which ensembles of electrons bound by nuclei forming atoms or molecules are the most natural representatives. Here, in the spirit of the well-studied one-dimensional helium atom, the electron dynamics in model atoms and molecules is addressed in ab initio fashion. To render calculations possible in the first place, (i) a novel hybrid representation of the NEGF is introduced based on the conception of finite elements (FE) and the discrete variable representation (DVR), and (ii) a parallel algorithm is developed that allows for an efficient, well scalable distributed-memory computation of the full two-time Green function. The first point attributes plenty of flexibility and makes the method readily adjustable to different Hamiltonians avoiding the need to, by hand or in intricate numerical manner, calculate the whole bunch of matrix elements of one- and two-particle operators. Also, in consequence, it drastically simplifies the evaluation of self-energies. The second point makes the NEGF approach ready for large-scale, high-performance computing facilities, the resources (of computer power: mainly memory!) of which are indispensable for (some of) the calculations presented. The applicability of the developed methods is demonstrated inter alia on the basis of helium, beryllium, hydrogen and lithium hydride modeled in one spatial dimension whereby electron-electron correlations are treated in the second(-order) Born approximation. After a thorough discussion on the self-consistent ground states, the thesis focuses on the electron dynamics in the linear response regime as well as in the presence of strong external fields. Overall, to assess the the performance of the second Born approximation, the results are compared to the Hartree-Fock approximation, on the one hand, and to the exact solution of the time-(in)dependent Schrödinger equation, on the other hand. In addition, aiming at the possibility of extended time-dependent calculations, the behavior of the generalized Kadanoff-Baym ansatz is discussed.
The time evolution in quantum many-body systems after external excitations is attracting high interest in many fields, including dense plasmas, correlated solids, laser-excited materials, or fermionic and bosonic atoms in optical lattices. The theoretical modeling of these processes is challenging, and the only rigorous quantum-dynamics approach that can treat correlated fermions in two and three dimensions is nonequilibrium Green functions (NEGF). However, NEGF simulations are computationally expensive due to their
T3 scaling with the simulation duration
T. Recently,
T2 scaling was achieved with the generalized Kadanoff-Baym ansatz (GKBA), for the second-order Born (SOA) self energy, which has substantially extended the scope of NEGF simulations. In a recent Letter [Schl\"unzen et al., Phys. Rev. Lett. 124, 076601 (2020).] we demonstrated that GKBA-NEGF simulations can be efficiently mapped onto coupled time-local equations for the single-particle and two-particle Green functions on the time diagonal, hence the method has been called the G1-G2 scheme. This allows one to perform the same simulations with order
T1 scaling, both for SOA and
GW self energies giving rise to a dramatic speedup. Here we present more details on the G1-G2 scheme, including derivations of the basic equations including results for a general basis, for Hubbard systems, and for jellium. Also, we demonstrate how to incorporate initial correlations into the G1-G2 scheme. Further, the derivations are extended to a broader class of self energies, including the
T matrix in the particle-particle and particle-hole channels and the dynamically-screened-ladder approximation. Finally, we demonstrate that, for all self energies, the CPU-time scaling of the G1-G2 scheme with the basis dimension
Nb can be improved compared to our first report: The overhead compared to the original GKBA is not more than an additional factor
Nb, even for Hubbard systems.
Abstract The two‐particle problem within a nonequilibrium many‐particle system is investigated in the framework of real‐time Green's functions. A nonequilibrium Dyson equation is given for the two‐time two‐particle Green's function. The two‐particle self‐energy in this equation consists of two qualitatively different parts: one part is local in time, whereas the other part is a two‐time quantity having thus a dynamical character. The latter part of the self‐energy can be expressed in terms of multi‐particle Green's functions.
Electron dynamics in a two-sites Hubbard model is studied using the nonequilibrium Green's function approach. The study is motivated by the empirical observation that a full solution of the integro-differential Kadanoff-Baym equation (KBE) is more stable and often accompanied by artificial damping [Marc Puig von Friesen, C. Verdozzi, and C.-O. Almbladh (2009)] than its time-linear reformulations relying on the generalized Kadanoff-Baym ansatz (GKBA). Additionally, for conserving theories, numerical simulations suggest that KBE produces natural occupations bounded by one and zero in agreement with the Pauli exclusion principle, whereas, in some regimes, GKBA-based theories violate this principle. As the first step for understanding these issues, the electron dynamics arising in the adiabatic switching scenario is studied. Many-body approximations are classified according to the channel of the Bethe-Salpeter equation in which electronic correlations are explicitly treated. They give rise to the so-called second Born,
T-matrix and
GW approximations. In each of these cases, the model is reduced to a system of ordinary differential equations, which resemble equations of motion for a driven harmonic oscillator with time-dependent frequencies. A more complete treatment of electronic correlations is achieved by combining different correlation channels, with parquet theory serving as a starting point.