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Physical Review A

Single-particle approach to many-body relaxation dynamics

M. Pelc, David Dams, Abhishek Ghosh, Miriam Kosik, Marvin M. Müller, Garnett W. Bryant, Carsten Rockstuhl, Andrés Ayuela, Karolina Słowik

Published Feb 26, 2024• 3 citations
Publisher

Abstract

This paper addresses the challenge of modeling relaxation dynamics in quantum many-body systems, specifically focusing on electrons in graphene nanoflakes. While quantum many-body techniques effectively describe dynamics up to a few particles, these approaches become computationally intractable for large systems. Larger systems may be tackled with a single-particle approach that, however, struggles to incorporate relaxation effects. Existing relaxation models encounter issues such as an inability to capture system complexity and violation of the Pauli principle. In this paper, we propose a single-particle model that accounts for various relaxation effects at the crossroads of quantum optics and solid-state photonics, that overcomes the limitations of previous models. Our approach is rooted in the quantum-optical Lindblad model, where relaxation rates are deactivated once the target levels saturate due to the Pauli principle. This approach is referred to as the saturated-Lindblad model. To validate the predictions of the saturated-Lindblad model, we confront them against phenomenological and many-body physics models in low-dimensional systems, including atomic chains and graphene nanoflakes. Remarkably, the saturated-Lindblad model exhibits excellent agreement with few-body calculations, distinguishing itself from other existing approaches. Moreover, by assigning different relaxation rates to different transitions, we successfully reproduce cascade deexcitation dynamics and predict emission spectra. The saturated-Lindblad model offers the ability to describe dynamics in systems of practical sizes, encompassing a wide range of structures that can be effectively captured within the single-particle description.

DOI
10.1103/physreva.109.022237

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This paper addresses the challenge of modeling relaxation dynamics in quantum many-body systems, specifically focusing on electrons in graphene nanoflakes. While quantum many-body techniques effectively describe dynamics up to a few particles, these approaches become computationally intractable for large systems. Larger systems may be tackled with a single-particle approach that, however, struggles to incorporate relaxation effects. Existing relaxation models encounter issues such as an inability to capture system complexity and violation of the Pauli principle. In this paper, we propose a single-particle model that accounts for various relaxation effects at the crossroads of quantum optics and solid-state photonics, that overcomes the limitations of previous models. Our approach is rooted in the quantum-optical Lindblad model, where relaxation rates are deactivated once the target levels saturate due to the Pauli principle. This approach is referred to as the saturated-Lindblad model. To validate the predictions of the saturated-Lindblad model, we confront them against phenomenological and many-body physics models in low-dimensional systems, including atomic chains and graphene nanoflakes. Remarkably, the saturated-Lindblad model exhibits excellent agreement with few-body calculations, distinguishing itself from other existing approaches. Moreover, by assigning different relaxation rates to different transitions, we successfully reproduce cascade deexcitation dynamics and predict emission spectra. The saturated-Lindblad model offers the ability to describe dynamics in systems of practical sizes, encompassing a wide range of structures that can be effectively captured within the single-particle description.
We report a linear-scaling numerical method for exploring nonequilibrium electron dynamics in systems of arbitrary complexity. Based on the Chebyshev expansion of the time evolution of the single-particle density matrix, the method gives access to nonperturbative excitation and relaxation phenomena in models of disordered materials with sizes on the experimental scale. After validating the method by applying it to saturable optical absorption in clean graphene, we uncover that disorder can enhance absorption in graphene and that the interplay between light, anisotropy, and disorder in nanoporous graphene might be appealing for sensing applications. Beyond the optical properties of graphenelike materials, the method can be applied to a wide range of large-area materials and systems with arbitrary descriptions of defects and disorder.
The exact nonequilibrium time evolution of the momentum distribution for a finite many-particle system in one dimension with a linear energy dispersion coupled to optical phonons is presented. For distinguishable particles the influence function of the phonon bath can be evaluated also for a finite particle density in the thermodynamic limit. In the case of fermions the exact fulfillment of the Pauli principle involves a sum over permutations of the electrons and the numerical evaluation is restricted to a finite number of electrons. In the dynamics the antisymmetry of the wave function shows up in the obvious Pauli blocking of momentum states as well as more subtle interference effects. The model shows the expected physical features known from approximate treatments of more realistic models for the relaxation in the energy regime far from the bottom of the conduction band and provides an excellent testing ground for quantum kinetic equations.
The exact nonequilibrium time evolution of the momentum distribution for a finite many particle system in one dimension with a linear energy dispersion coupled to optical phonons is presented. For distinguishable particles the influence function of the phonon bath can be evaluated also for a finite particle density in the thermodynamic limit. In the case of fermions the exact fulfillment of the Pauli principle involves a sum over permutations of the electrons and the numerical evaluation is restricted to a finite number of electrons. In the dynamics the antisymmetry of the wavefunction shows up in the obvious Pauli blocking of momentum states as well as more subtle interference effects. The model shows the expected physical features known from approximate treatments of more realistic models for the relaxation in the energy regime far from the bottom of the conduction band and provides an excellent testing ground for quantum kinetic equations.
We study interaction-driven ultrafast dynamics in finite graphene flakes following an optical pump quench in an interacting tight-binding model. By comparing exact real-time evolution with simulations restricted to particle-hole excitation subspaces, we assess when relaxation can be captured by low-order many-body processes and when this is not sufficient. The single-particle orbital entropy provides a compact diagnostic for dynamic correlation growth. For the systems studied here, periodic graphene flakes are well described by low-order excitations, whereas confined geometries require substantial higher-order contributions even for relatively small interaction strengths. The quench protocol combines simple initial-state preparation with strongly correlated dynamics, identifying a promising benchmark problem for future quantum-computing simulations.
Quantum master equations are common tools to describe the dynamics of many-body systems open to an environment. Due to the interaction with the latter, even for the case of noninteracting electrons, the computational cost to solve these equations increases exponentially with the particle number. We propose a simple scheme, which allows to study the dynamics of NNN noninteracting electrons taking into account both dissipation effects and Fermi statistics, with a computational cost that scales linearly with NNN. Our method is based on a mapping of the many-body system to a specific set of effective single-particle systems. We provide detailed numerical results showing excellent agreement between the effective single-particle scheme and the exact many-body one, as obtained from studying the dynamics of two different systems. In the first, we study optically-induced currents in quantum rings at zero temperature, and in the second we study a linear chain coupled at its ends to two thermal baths with different (finite) temperatures. In addition, we give an analytical justification for our method, based on an exact averaging over the many-body states of the original master equations.
Spontaneous light emission is central to a vast range of physical systems and is a founding pillar for the theory of light–matter interactions. In the presence of complex photonic media, the description of spontaneous light emission usually requires advanced theoretical quantum optics tools such as macroscopic quantum electrodynamics, involving quantized electromagnetic fields. Although rigorous and comprehensive, the complexity of such models can obscure the intuitive understanding of many quantum-optical phenomena. Here, we review a method for calculating spontaneous emission and other quantum-optical processes without making explicit use of quantized electromagnetic fields. Instead, we introduce the concept of transition currents, comprising charges in matter that undergo transitions between initial and final quantum states. We show how predictions that usually demand advanced methods in quantum electrodynamics or quantum optics can be reproduced by feeding these transition currents as sources to the classical Maxwell equations. One then obtains the relevant quantum observables from the resulting classical field amplitudes, without washing out quantum optical effects. We show that this procedure allows for a straightforward description of quantum phenomena, even when going beyond the dipole approximation and single emitters. As illustrative examples, we calculate emission patterns and Purcell-enhanced emission rates in both bound-electron and free-electron systems. For the latter, we derive cathodoluminescence emission and energy-loss probabilities of free electrons interacting with nanostructured samples. In addition, we calculate quantum-beat phenomena in bound-electron systems and wave function-dependent optical coherence in free-electron systems. Remarkably, the transition-current formalism captures more complex phenomena, such as many-body interference effects and super-radiance of both bound- and free-electron systems, second-order processes such as two-photon emission, and quantum recoil corrections to free-electron radiation. We review a variety of light–matter interactions in fields ranging from electron microscopy to nanophotonics and quantum optics, for which the transition-current theoretical formalism facilitates practical simulations and a deeper understanding of novel applications.