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Marten Richter

Publications and source records attributed to Marten Richter.

33 records · Page 2Linked to original sources

Combined tensor network/cluster expansion method using logic gates: Illustrated for (bi-)excitons by a single layer MoS$_2$ model system

Carriers such as electrons and holes inside the Brillouin zone of complex semiconducting materials can form bound states (excitons, biexcitons etc.). For obtaining the corresponding eigenstates (e.g. through Wannier or Bethe Salpeter equation) and dynamics (e.g. cluster expansion) the number of involved electrons and holes as well as the accuracy is limited by the appearing high dimensional tensors (i.e. wavefunctions or correlations). These tensors can be efficiently represented and manipulated via tensor network methods. We show how tensor networks formulated via classic logic gates can be used to treat electron-hole complexes inside the Brillouin zone. The method is illustrated for the exciton and biexciton states of a single layer transition metal dichalcogenide MoS$_2$ like model system.

cond-mat.mes-hall↗

Theory and limits of on-demand single photon sources using plasmonic resonators: a quantized quasinormal mode approach

Quantum emitters coupled to plasmonic resonators are known to allow enhanced broadband Purcell factors, and such systems have been recently suggested as possible candidates for on-demand single photon sources, with fast operation speeds. However, a true single photon source has strict requirements of high efficiency (brightness) and quantum indistinguishability of the emitted photons, which can be quantified through two-photon interference experiments. To help address this problem, we employ and extend a recently developed quantized quasinormal mode approach, which rigorously quantizes arbitrarily lossy open system modes, to compute the key parameters that accurately quantify the figures of merit for plasmon-based single photon sources. We also present a quantized input-output theory to quantify the radiative and nonradiative quantum efficiencies. We exemplify the theory using a nanoplasmonic dimer resonator made up of two gold nanorods, which yields large Purcell factors and good radiative output beta factors. Considering an optically pulsed excitation scheme, we explore the key roles of pulse duration and pure dephasing on the single photon properties, and show that ultrashort pulses (sub-ps) are generally required for such structures, even for low temperature operation. We also quantify the role of the nonradiative beta factor both for single photon and two-photon emission processes. Our general approach can be applied to a wide variety of plasmon systems, including metal-dielectrics, and cavity-waveguide systems, without recourse to phenomenological quantization schemes.

quant-ph↗

Quantization of quasinormal modes for open cavities and plasmonic cavity-QED

We introduce a second quantization scheme based on quasinormal modes, which are the dissipative modes of leaky optical cavities and plasmonic resonators with complex eigenfrequencies. The theory enables the construction of multi-plasmon/photon Fock states for arbitrary three-dimensional dissipative resonators and gives a solid understanding to the limits of phenomenological dissipative Jaynes-Cummings models. In the general case, we show how different quasinormal modes interfere through an off-diagonal mode coupling and demonstrate how these results affect cavity-modified spontaneous emission. To illustrate the practical application of the theory, we show examples using a gold nanorod dimer and a hybrid dielectric-metal cavity structure.

cond-mat.mes-hall↗

Theory of excitation transfer between two-dimensional semiconductor and molecular layers

The geometry-dependent energy transfer rate from an electrically pumped inorganic semiconductor quantum well into an organic molecular layer is studied theoretically. We focus on Förster-type nonradiative excitation transfer between the organic and inorganic layer and include quasi-momentum conservation and intermolecular coupling between the molecules in the organic film. (Transition) partial charges calculated from density-functional theory are used to calculate the coupling elements. The partial charges describe the spatial charge distribution and go beyond the common dipole-dipole interaction. We find that the transfer rates are highly sensitive to variations in the geometry of the hybrid inorganic/organic system. For instance, the transfer efficiency is improved by orders of magnitude by tuning the relative orientation and positioning of the molecules. Also, the operating regime is identified where in-scattering dominates over unwanted back-scattering from the molecular layer into the substrate.

cond-mat.mes-hall↗

Superradiant to subradiant phase transition in the open system Dicke model: Dark state cascades

Collectivity in ensembles of atoms gives rise to effects like super- and subradiance. While superradiance is well studied and experimentally accessible, subradiance remains elusive since it is difficult to track experimentally as well as theoretically. Here we present a new type of phase transition in the resonantly driven, open Dicke model that leads to a deterministic generation of subradiant states. At the transition the system switches from a predominantly superradiant to a predominantly subradiant state. Clear experimental signatures for the effect are presented and entanglement properties are discussed. Letting the system relax into the ground state generates a cascade of dark Dicke states, with dark state populations up to unity. Furthermore we introduce a collectivity measure that allows to quantify collective behavior.

quant-ph↗

PsiQuaSP -- A library for efficient computation of symmetric open quantum systems

In a recent publication we showed that permutation symmetry reduces the numerical complexity of Lindblad quantum master equations for identical multi-level systems from exponential to polynomial scaling. This is important for open system dynamics including realistic system bath interactions and dephasing in, for instance, the Dicke model, multi-$Λ$ system setups etc. Here we present an object-oriented C++ library that allows to setup and solve arbitrary quantum optical Lindblad master equations, especially those that are permutationally symmetric in the multi-level systems. PsiQuaSP (Permutation symmetry for identical Quantum Systems Package) uses the PETSc package for sparse linear algebra methods and differential equations as basis. The aim of PsiQuaSP is to provide flexible, storage efficient and scalable code while being as user friendly as possible. It is easily applied to many quantum optical or quantum information systems with more than one multi-level system. We first review the basics of the permutation symmetry for multi-level systems in quantum master equations. The application of PsiQuaSP to quantum dynamical problems is illustrated with several typical, simple examples of open quantum optical systems.

quant-ph↗

Nanoplatelets as material system between strong confinement and weak confinement

Recently, the fabrication of CdSe nanoplatelets became an important research topic. Nanoplatelets are often described as having a similar electronic structure as 2D dimensional quantum wells and are promoted as colloidal quantum wells with monolayer precision width. In this paper, we show, that nanoplatelets are not ideal quantum wells, but cover depending on the size: the strong confinement regime, an intermediate regime and a Coulomb dominated regime. Thus, nanoplatelets are an ideal platform to study the physics in these regimes. Therefore, the exciton states of the nanoplatelets are numerically calculated by solving the full four dimensional Schrödinger equation. We compare the results with approximate solutions from semiconductor quantum well and quantum dot theory. The paper can also act as review of these concepts for the colloidal nanoparticle community.

cond-mat.mes-hall↗

Coherent coupling of individual quantum dots measured with phase-referenced two-dimensional spectroscopy: photon echo versus double quantum coherence

We employ two-dimensional (2D) coherent, nonlinear spectroscopy to investigate couplings within individual InAs quantum dots (QD) and QD molecules. Swapping pulse ordering in a two-beam sequence permits to distinguish between rephasing and non-rephasing four-wave mixing (FWM) configurations. We emphasize the non-rephasing case, allowing to monitor two-photon coherence dynamics. Respective Fourier transform yields a double quantum 2D FWM map, which is corroborated with its single quantum counterpart, originating from the rephasing sequence. We introduce referencing of the FWM phase with the one carried by the driving pulses, overcoming the necessity of its active-stabilization, as required in 2D spectroscopy. Combining single and double quantum 2D FWM, provides a pertinent tool in detecting and ascertaining coherent coupling mechanisms between individual quantum systems, as exemplified experimentally.

cond-mat.mes-hall↗

Dark and bright exciton formation, thermalization, and photoluminescence in monolayer transition metal dichalcogenides

The remarkably strong Coulomb interaction in atomically thin transition metal dichalcogenides (TMDs) results in an extraordinarily rich many-particle physics including the formation of tightly bound excitons. Besides optically accessible bright excitonic states, these materials also exhibit a variety of dark excitons. Since they can even lie below the bright states, they have a strong influence on the exciton dynamics, lifetimes, and photoluminescence. While very recently, the presence of dark excitonic states has been experimentally demonstrated, the origin of these states, their formation, and dynamics have not been revealed yet. Here, we present a microscopic study shedding light on time- and energy-resolved formation and thermalization of bright and dark intra- and intervalley excitons as well as their impact on the photoluminescence in different TMD materials. We demonstrate that intervalley dark excitons, so far widely overlooked in current literature, play a crucial role in tungsten-based TMDs giving rise to an enhanced photoluminescence and reduced exciton lifetimes at elevated temperatures.

cond-mat.mes-hall↗

Neutral and Charged Inter-Valley Biexcitons in Monolayer MoSe$_2$

In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods alone. Here, we implement polarization-resolved two-dimensional coherent spectroscopy to unravel the complex optical response of monolayer MoSe$_2$ and identify multiple higher-order correlated states. Decisive signatures of neutral and charged inter-valley biexcitons appear in cross-polarized two-dimensional spectra as distinct resonances with respective ~20 meV and ~5 meV binding energies--similar to recent calculations using variational and Monte Carlo methods. A theoretical model taking into account the valley-dependent optical selection rules reveals the specific quantum pathways that give rise to these states. Inter-valley biexcitons identified here, comprised of neutral and charged excitons from different valleys, offer new opportunities for creating exotic exciton-polariton condensates and for developing ultrathin biexciton lasers and polarization-entangled photon sources.

cond-mat.mes-hall↗

Trion Formation Dynamics in Monolayer Transition Metal Dichalcogenides

We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in TMDs. The quasiparticle formation and conversion processes are important for interpreting photoluminescence and photoconductivity in TMDs.

cond-mat.mes-hall↗

Numerically exact solution of the many emitter -- cavity laser problem: application to the fully quantized spaser emission

A numerically exact solution to the many emitter -- cavity problem as an open many body system is presented. The solution gives access to the full, nonperturbative density matrix and thus the full quantum statistics and quantum correlations. The numerical effort scales with the third power in the number of emitters. Notably the solution requires none of the common approximations like good/bad cavity limit. As a first application the recently discussed concept of coherent surface plasmon amplification -- spaser -- is addressed: A spaser consists of a plasmonic nanostructure that is driven by a set of quantum emitters. In the context of laser theory it is a laser in the (very) bad cavity limit with an extremely high light matter interaction strength. The method allows us to answer the question of spasing with a fully quantized theory.

cond-mat.mes-hall↗

Two-dimensional double-quantum spectra reveal collective resonances in an atomic vapor

We report the observation of double-quantum coherence signals in a gas of potassium atoms at twice the frequency of the one-quantum coherences. Since a single atom does not have a state at the corresponding energy, this observation must be attributed to a collective resonance involving multiple atoms. These resonances are induced by weak inter-atomic dipole-dipole interactions, which means that the atoms cannot be treated in isolation, even at a low density of $10^{12}$ cm$^{-3}$.

physics.atom-ph↗

Influence of Coulomb correlations on the quantum well intersubband absorption at low temperatures

We present a theory for the intersubband absorption including electronic ground state correlations in a doped GaAs/Al_{35}Ga_{65}As quantum well system. Focusing on the influence of the Coulomb interaction among the carriers at low temperatures, we find that the ground state correlations lead to an increased renormalization and spectral broadening of the absorption spectrum. At T = 1 K, its full width at half maximum is increased by up to a factor 3. The inclusion of electron-phonon scattering strongly reduces the relative impact of the electronic correlations.

cond-mat.mes-hall↗

Few-photons model of the optical emission of semiconductor quantum dots

The Jaynes-Cummings model provides a well established theoretical framework for single electron two level systems in a radiation field. Similar exactly solvable models for semiconductor light emitters such as quantum dots dominated by many particle interactions are not known. We access these systems by a generalized cluster expansion, the photon-probability-cluster-expansion: a reliable approach for few photon dynamics in many body electron systems. As a first application, we discuss vacuum Rabi flopping and show that their amplitude determines the number of electrons in the quantum dot.

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