arXiv subjects

Johannes Feist

Publications and source records attributed to Johannes Feist.

At least 37 records · Page 2Linked to original sources

arXiv2024

Taming the Bloch-Redfield equation: Recovering an accurate Lindblad equation for general open quantum systems

Master equations play a pivotal role in investigating open quantum systems. In particular, the Bloch-Redfield equation stands out due to its relation to a concrete physical environment. However, without further approximations it does not lead to a Lindblad master equation that guarantees that the density matrix stays completely positive, which has raised some concerns regarding its use. This study builds on previous efforts to transform the Bloch-Redfield framework into a mathematically robust Lindblad equation, while fully preserving the effects that are lost within the secular approximation that is commonly used to guarantee positivity. These previous approaches introduce two potential deficiencies: the environment-induced energy shift can be non-Hermitian and some decay rates can be negative, violating the assumptions of Lindblad's theorem. Here, we propose and evaluate straightforward solutions to both problems. Our approach offers an effective and general procedure for obtaining a Lindblad equation, derived from a concrete physical environment, while mitigating the unphysical dynamics present in the Bloch-Redfield equation.

quant-ph↗

arXiv2024

Unconventional magnetism mediated by spin-phonon-photon coupling

Magnetic order typically emerges due to the short-range exchange interaction between the constituent electronic spins. Recent discoveries have found a crucial role for spin-phonon coupling in various phenomena from optical ultrafast magnetization switching to dynamical control of the magnetic state. Here, we demonstrate theoretically the emergence of a biquadratic long-range interaction between spins mediated by their coupling to phonons hybridized with vacuum photons into polaritons. The resulting ordered state enabled by the exchange of virtual polaritons between spins is reminiscent of superconductivity mediated by the exchange of virtual phonons. The biquadratic nature of the spin-spin interaction promotes ordering without favoring ferro- or antiferromagnetism. It further makes the phase transition to magnetic order a first-order transition, unlike in conventional magnets. Consequently, a large magnetization develops abruptly on lowering the temperature which \aknew{could} enable magnetic memories admitting ultralow-power thermally-assisted writing while maintaining a high data stability. The role of photons in the phenomenon further enables an in-situ static control over the magnetism. These unique features make our predicted spin-spin interaction and magnetism highly unconventional paving the way for novel scientific and technological opportunities.

cond-mat.mes-hall↗

arXiv2024

Non-Hermitian Anharmonicity Induces Single-Photon Emission

Single-photon sources are in high demand for quantum information applications. A paradigmatic way to achieve single-photon emission is through anharmonicity in the energy levels, such that the absorption of a single photon from a coherent drive shifts the system out of resonance and prevents absorption of a second one. We identify a novel mechanism for single-photon emission through non-Hermitian anharmonicity, i.e., anharmonicity in the losses instead of in the energy levels. We demonstrate the mechanism in two types of systems, including a feasible setup consisting of a hybrid metallodielectric cavity weakly coupled to a two-level emitter, and show that it induces high-purity single-photon emission at high repetition rates.

quant-ph↗

arXiv2024

Coherent multidimensional spectroscopy in polariton systems

The fast dynamics of molecular polaritonics is scrutinized theoretically through the implementation of two-dimensional spectroscopy protocols. We derive conceptually simple and computationally efficient formulas to calculate two-dimensional spectra for molecules, each of them modeled as a system of two electronic states including vibrational relaxation, immersed in an optical cavity, thus coupled to quantized radiation. Cavity photon losses and molecular relaxation are incorporated into the Hamiltonian dynamics to form an open quantum system that is solved through a master equation. In the collective case, the relaxation dynamics into dark states reveals to be the crucial factor to explain the asymmetries in both the diagonal and cross peaks of two-dimensional spectra for long waiting times between excitation and detection, a feature shown by recent experiments. Our theoretical method provides a deeper insight in those processes that yield relevant signals in multidimensional molecular spectroscopy.

quant-ph↗

arXiv2024

A mixed perturbative-nonperturbative treatment for strong light-matter interactions

The full information about the interaction between a quantum emitter and an arbitrary electromagnetic environment is encoded in the so-called spectral density. We present an approach for describing such interaction in any coupling regime, providing a Lindblad-like master equation for the emitter dynamics when coupled to a general nanophotonic structure. Our framework is based on the splitting of the spectral density into two terms. On the one hand, a spectral density responsible for the non-Markovian and strong-coupling-based dynamics of the quantum emitter. On the other hand, a residual spectral density including the remaining weak-coupling terms. The former is treated nonperturbatively with a collection of lossy interacting discrete modes whose parameters are determined by a fit to the original spectral density in a frequency region encompassing the quantum emitter transition frequencies. The latter is treated perturbatively under a Markovian approximation. We illustrate the power and validity of our approach through numerical simulations in three different setups, thus offering a variety of scenarios for a full test, including the ultra-strong coupling regime.

quant-ph↗

arXiv2023

Vacuum-field-induced state mixing

By engineering the electromagnetic vacuum field, the induced Casimir-Polder shift (also known as Lamb shift) and spontaneous emission rates of individual atomic levels can be controlled. When the strength of these effects becomes comparable to the energy difference between two previously uncoupled atomic states, an environment-induced interaction between these states appears after tracing over the environment. This interaction has been previously studied for degenerate levels and simple geometries involving infinite, perfectly conducting half-spaces or free space. Here, we generalize these studies by developing a convenient description that permits the analysis of these non-diagonal perturbations to the atomic Hamiltonian in terms of an accurate non-Hermitian Hamiltonian. Applying this theory to a hydrogen atom close to a dielectric nanoparticle, we show strong vacuum-field-induced state mixing that leads to drastic modifications in both the energies and decay rates compared to conventional diagonal perturbation theory. In particular, contrary to the expected Purcell enhancement, we find a surprising decrease of decay rates within a considerable range of atom-nanoparticle separations. Furthermore, we quantify the large degree of mixing of the unperturbed eigenstates due to the non-diagonal perturbation. Our work opens new quantum state manipulation possibilities in emitters with closely spaced energy levels.

quant-ph↗

arXiv2023

Electrostatic nature of cavity-mediated interactions between low-energy matter excitations

The use of cavity quantum electrodynamical effects, i.e., of vacuum electromagnetic fields, to modify material properties in cavities has rapidly gained popularity and interest in the last few years. However, there is still a scarcity of general results that provide guidelines for intuitive understanding and limitations of what kind of effects can be achieved. We provide such a result for the effective interactions between low-energy matter excitations induced either directly by their mutual coupling to the cavity electromagnetic (EM) field or indirectly through coupling to mediator modes that couple to the EM field. We demonstrate that the induced interactions are purely electrostatic in nature and are thus fully described by the EM Green's function evaluated at zero frequency. Our findings imply that reduced models with one or a few cavity modes can easily give misleading results.

quant-ph↗

arXiv2023

Enhanced Excitation Energy Transfer under Strong Light-Matter Coupling: Insights from Multi-Scale Molecular Dynamics Simulations

Exciton transport can be enhanced in the strong coupling regime where excitons hybridise with confined light modes to form polaritons. Because polaritons have group velocity, their propagation should be ballistic and long-ranged. However, experiments indicate that organic polaritons propagate in a diffusive manner and more slowly than their group velocity. Here, we resolve this controversy by means of molecular dynamics simulations of Rhodamine molecules in a Fabry-Pérot cavity. Our results suggest that polariton propagation is limited by the cavity lifetime and appears diffusive due to reversible population transfers between polaritonic states that propagate ballistically at their group velocity, and dark states that are stationary. Furthermore, because long-lived dark states transiently trap the excitation, propagation is observed on timescales beyond the intrinsic polariton lifetime. These insights not only help to better understand and interpret experimental observations, but also pave the way towards rational design of molecule-cavity systems for coherent exciton transport.

physics.chem-ph↗

arXiv2023

Strong light-matter coupling in lead halide perovskite quantum dot solids

Strong coupling between lead halide perovskite materials and optical resonators enables both the polaritonic control of the photophysical properties of these emerging semiconductors and the observation of novel fundamental physical phenomena. However, the difficulty to achieve optical-quality perovskite quantum dot (PQD) films showing well-defined excitonic transitions has prevented the study of strong light-matter coupling in these materials, central to the field of optoelectronics. Herein we demonstrate the formation at room temperature of multiple cavity exciton-polaritons in metallic resonators embedding highly transparent Cesium Lead Bromide quantum dot (CsPbBr3-QD) solids, revealed by a significant reconfiguration of the absorption and emission properties of the system. Our results indicate that the effects of biexciton interaction or large polaron formation, frequently invoked to explain the properties of PQDs, are seemingly absent or compensated by other more conspicuous effects in the CsPbBr3-QD optical cavity. We observe that strong coupling enables a significant reduction of the photoemission linewidth, as well as the ultrafast switching of the optical absorption, controllable by means of the excitation fluence. We find that the interplay of the polariton states with the large dark state reservoir play a decisive role in determining the dynamics of the emission and transient absorption properties of the hybridized light-quantum dot solid system. Our results open the route for the investigation of PQD solids as polaritonic optoelectronic materials.

cond-mat.mtrl-sci↗

arXiv2023

A Lindblad master equation capable of describing hybrid quantum systems in the ultra-strong coupling regime

Despite significant theoretical efforts devoted to studying the interaction between quantized light modes and matter, the so-called ultra-strong coupling regime still presents significant challenges for theoretical treatments and prevents the use of many common approximations. Here we demonstrate an approach that can describe the dynamics of hybrid quantum systems in any regime of interaction for an arbitrary electromagnetic (EM) environment. We extend a previous method developed for few-mode quantization of arbitrary systems to the case of ultrastrong light-matter coupling, and show that even such systems can be treated using a Lindblad master equation where decay operators act only on the photonic modes by ensuring that the effective spectral density of the EM environment is sufficiently suppressed at negative frequencies. We demonstrate the validity of our framework and show that it outperforms current state-of-the-art master equations for a simple model system, and then study a realistic nanoplasmonic setup where existing approaches cannot be applied.

quant-ph↗

arXiv2022

Can we observe non-perturbative vacuum shifts in cavity QED?

We address the fundamental question whether or not it is possible to achieve conditions under which the coupling of a single dipole to a strongly confined electromagnetic vacuum can result in non-perturbative corrections to the dipole's ground state. To do so we consider two simplified, but otherwise rather generic cavity QED setups, which allow us to derive analytic expressions for the total ground state energy and to distinguish explicitly between purely electrostatic and genuine vacuum-induced contributions. Importantly, this derivation takes the full electromagnetic spectrum into account while avoiding any ambiguities arising from an ad-hoc mode truncation. Our findings show that while the effect of confinement per se is not enough to result in substantial vacuum-induced corrections, the presence of high-impedance modes, such as plasmons or engineered LC resonances, can drastically increase these effects. Therefore, we conclude that with appropriately designed experiments it is at least in principle possible to access a regime where light-matter interactions become non-perturbative.

quant-ph↗

arXiv2022

Exact time-dependent density functional theory for non-perturbative dynamics of helium atom

By inverting the time-dependent Kohn-Sham equation for a numerically exact dynamics of the helium atom, we show that the dynamical step and peak features of the exact correlation potential found previously in one-dimensional models persist for real three-dimensional systems. We demonstrate that the Kohn-Sham and true current-densities differ by a rotational component. The results have direct implications for approximate TDDFT calculations of atoms and molecules in strong fields, emphasizing the need to go beyond the adiabatic approximation, and highlighting caution in quantitative use of the Kohn-Sham current.

physics.chem-ph↗

arXiv2022

Permutational symmetry for identical multi-level systems: a second quantized approach

We develop a framework that provides a straightforward approach to fully exploit the permutational symmetry of identical multi-level systems. By taking into account the permutational symmetry, we outline a simple scheme that allows to map the dynamics of $N$ identical $d$-level systems to the dynamics of $d$ bosonic modes with $N$ particles, achieving an exponential reduction on the dimensionality of the problem in a simple and straightforward way. In particular, we consider the Lindblad dynamics of several identical multi-level systems interacting with a common subsystem under the action of collective dissipation terms.

quant-ph↗

arXiv2022

A theoretical perspective on molecular polaritonics

In the last decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction of polaritonic phenomena emerging in this light-matter interaction regime have proven to be difficult tasks. The challenge originates from the enormous number of degrees of freedom that need to be taken into account, both in the organic molecules and in their photonic environment. On the one hand, the accurate treatment of the vibrational spectrum of the former is key, and simplified quantum models are not valid in many cases. On the other hand, most photonic setups have complex geometric and material characteristics, with the result that photon fields corresponding to more than just a single electromagnetic mode contribute to the light-matter interaction in these platforms. Moreover, loss and dissipation, in the form of absorption or radiation, must also be included in the theoretical description of polaritons. Here, we review and offer our own perspective on some of the work recently done in the modelling of interacting molecular and optical states with increasing complexity.

quant-ph↗

arXiv2021

Few-mode Field Quantization for Multiple Emitters

The control of the interaction between several quantum emitters using nanophotonic structures holds great promise for quantum technology applications. However, the theoretical description of such processes for complex nanostructures is a highly demanding task as the electromagnetic (EM) modes are in principle described by a high-dimensional continuum. We here introduce an approach that permits a quantized description of the full EM field through a "minimal" number of discrete modes. This extends the previous work in [Medina et al., Phys. Rev. Lett. 126, 093601 (2021)] to the case of an arbitrary number of emitters with arbitrary orientations, without any restrictions on the emitter level structure or dipole operators. We illustrate the power of our approach for a model system formed by three emitters placed in different positions within a metallodielectric photonic structure consisting of a metallic dimer embedded in a dielectric nanosphere. The low computational demand of this method makes it suitable for studying dynamics for a wide range of parameters. We show that excitation transfer between the emitters is highly sensitive to the properties of the hybrid photonic-plasmonic modes, demonstrating the potential of such structures for achieving control over emitter interactions.

physics.optics↗

arXiv2021

Theoretical Challenges in Polaritonic Chemistry

Polaritonic chemistry exploits strong light-matter coupling between molecules and confined electromagnetic field modes to enable new chemical reactivities. In systems displaying this functionality, the choice of the cavity determines both the confinement of the electromagnetic field and the number of molecules that are involved in the process, whereas in wavelength-scale optical cavities light-matter interaction is ruled by collective effects, plasmonic subwavelength nanocavities allow even single molecules to reach strong coupling. Due to these very distinct situations, a multiscale theoretical toolbox is then required to explore the rich phenomenology of polaritonic chemistry. Within this framework, each component of the system (molecules and electromagnetic modes) needs to be treated in sufficient detail to obtain reliable results. Starting from the very general aspects of light-molecule interactions in typical experimental setups, we underline the basic concepts that should be taken into account when operating in this new area of research. Building on these considerations, we then provide a map of the theoretical tools already available to tackle chemical applications of molecular polaritons at different scales. Throughout the discussion, we draw attention to both the successes and the challenges still ahead in the theoretical description of polaritonic chemistry.

physics.optics↗

arXiv2021

Not dark yet: strong light-matter coupling can accelerate singlet fission dynamics

Polaritons are unique hybrid light-matter states that offer an alternative way to manipulate chemical processes and change material properties. In this work we theoretically demonstrate that singlet fission dynamics can be accelerated under strong light-matter coupling. For superexchange-mediated singlet fission, state mixing speeds up the dynamics in cavities when the lower polariton is close in energy to the multiexcitonic triplet-pair state. We show that this effect is more pronounced in non-conventional singlet fission materials in which the energy gap between the bright singlet exciton and the multiexcitonic state is large (> 0.1 eV). In this case, the dynamics is dominated by the polaritonic modes and not by the bare-molecule-like dark states, and additionally, the resonant enhancement due to strong coupling is very robust even for energetically broad molecular states. The present results provide a new strategy to expand the range of suitable materials for efficient singlet fission by making use of strong light-matter coupling.

physics.chem-ph↗

arXiv2020

Molecular photodissociation enabled by ultrafast plasmon decay

We propose a strategy for enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon. The large possible coupling on the single-molecule level combined with the highly lossy nature of plasmonic modes, with lifetimes on the order of femtoseconds, opens an ultrafast decay channel for the molecule. For plasmon mode frequencies below the vertical photoexcitation energy of the molecule, the difference between excitation and emission energy is converted into vibrational energy on the molecular ground state in a Raman-like process. Under the correct conditions, this energy can be high enough to enable efficient photodissociation on the electronic ground state. We demonstrate the concept using numerical simulations of the Lindblad master equation for the hydrogen molecule in the vicinity of an aluminum nanoparticle, and explore the photodissociation efficiency as a function of various system parameters.

quant-ph↗