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Jonas Grumm

Publications and source records attributed to Jonas Grumm.

5 recordsLinked to original sources

Nonlinear Diamagnetic Interactions in Ultrastrongly Coupled 2D Electrons

The quantum Hopfield model is widely used to describe ultrastrong light--matter coupling between cavity photons and collective bosonic excitations in solids, where the diamagnetic interaction is conventionally assumed to be a constant. We experimentally demonstrate that the diamagnetic response of Landau polaritons is reduced under strong terahertz field excitation. We show that this behavior originates from field-driven redistribution of electrons into the nonparabolic regime of the conduction band of GaAs, which reduces the plasma frequency and consequently the diamagnetic interaction strength. A microscopic hot-electron model reproduces the observed nonlinear response. Motivated by this microscopic picture, we propose a nonlinear extension of the Hopfield model with a Kerr-like interaction. Our results establish a route toward nonlinear cavity quantum electrodynamics and driven ultrastrong light--matter coupling beyond the conventional linear Hopfield description, which is capable of creating uniquely quantum optical effects such as squeezed light generation.

quant-ph

Electron- and Lattice-Temperature Dependence of the Optical Response of Gold Nanoparticles

Transient absorption spectroscopy is routinely used to study the electron dynamics in plasmonic gold nanoparticles. Typically, the transient absorption bleach is analyzed as measure for the electron temperature. However, the implicitly assumed linear dependence between bleach intensity and temperature has not been systematically studied. Similarly, the influence of lattice heating also lacks a detailed analysis. Here, we solve momentum-resolved metal Boltzmann-Bloch equations for a semi-analytic access to the temperature-dependent gold nanoparticle absorption. We confirm the theory with steady state and transient absorption experiments, define regions of linear correlation between transient absorption bleach intensity and electron temperature and reveal a strong impact of the lattice temperature on the TA bleach intensity.

cond-mat.mes-hall

Boltzmann-Bloch Equation Approach to the Theory of the Optical Inter- and Intraband Response in Noble Metals

In this paper we introduce momentum-resolved metal Boltzmann-Bloch equations (MBBE) for the combined description of electronic intra- and interband processes in noble metals. This microscopic framework incorporates a full treatment of many-body electron-electron and electron-phonon interactions, relevant for relaxation and dephasing processes after optical excitation. For the example of gold, we calculate the linear optical response for near-infrared and visible energies. This provides insight into the interplay of microscopic processes hidden in phenomenological Drude-Lorentz models. The complex geometry of the Fermi surface is treated by an anisotropic electronic dispersion model, which is necessary to explain the temperature dependent spectrum over the whole frequency range of intra- and interband transitions.

cond-mat.mes-hall

Theory of Non-Linear Electron Relaxation in Thin Gold Films and Their Signatures in Optical Observables

Based on the momentum-resolved Boltzmann equation, we provide self-consistent numerical calculations of the dynamics of conduction electrons in thin noble metal films after linear and non-linear optical excitations with infrared and terahertz frequencies. Focusing exclusively on electron-phonon interaction, orientational relaxation is introduced and acts as dephasing of the optical excitation on a scale of tens of fs. In the linear regime, our numerical results agree with the experimental fits to a Drude model and predicts for non-linear excitations a field strength dependency of the orientational relaxation rate. In the THz regime, where the orientational relaxation proceeds faster than the oscillation cycle of the excitation THz field, a new high order dissipative Kerr-type non-linearity is predicted. This non-linearity originates from the Pauli blocking included in the electron-phonon scattering and results in a non-linearly increasing transmission of the film, detectable in experiments.

cond-mat.mes-hall

Ultrafast Electrons in Noble Metals: Orientational Relaxation, Thermalization and Cooling in Terms of Electron-Phonon Interaction

We investigate the momentum-resolved dynamics of conduction electrons in noble metals following ultrashort optical excitation with linearly polarized light. Using a momentum-resolved Boltzmann equation approach for electron-phonon interaction, we solve for the combined effects of orientational relaxation, thermalization, and cooling. We introduce momentum orientational relaxation as the initial step in the equilibration of an optically excited non-equilibrium electron gas by highlighting its importance for the optical response of noble metals and the dephasing of plasmonic excitations. Our numerical results for gold reveal that orientational relaxation exists independently of the absorbed optical energy and dominates on time scales on the first tens of fs after excitation. Incorporating also thermalization and cooling on times up to a few ps, our approach provides a simultaneous description of optical and thermal properties of noble metals under initial non-equilibrium conditions.

cond-mat.mes-hall