arXiv subjects

Stephan Götzinger

Publications and source records attributed to Stephan Götzinger.

At least 19 recordsLinked to original sources

arXiv2026

Designing metallo-dielectric antennas for cryogenic applications

We present the design of cryogenic metallo-dielectric antennas tailored to single organic emitters, where the choice of host material imposes specific constraints on the antenna geometry. Using dibenzoterrylene (DBT) in para-dichlorobenzene (p-DCB}) as a model system, we show that photon collection efficiencies exceeding 90% can be achieved for arbitrary dipole orientations of the fluorescent molecule. The antenna design is intrinsically broadband and tolerant to emitter positioning within the structure. We further provide concrete fabrication guidelines for the full antenna architecture, and experimentally demonstrate its operating principle by recording a back-focal-plane image (BFP) of a single molecule inside a fabricated antenna.

physics.optics↗

arXiv2026

Design of monolithic microcavities for enhancing organic quantum emitters

Single organic molecules are a well-established platform for high-quality single-photon generation: they can emit lifetime-limited photons with high purity and indistinguishability. However, their emission is accompanied by a pronounced red-shifted phonon sideband and higher-order vibrational peaks, which reduce the fraction of photons emitted into the desired narrowband zero-phonon line. The standard approach to suppressing this unwanted emission is to integrate the emitter into a monolithic photonic nanostructure that provides Purcell enhancement. However, incorporating organic materials using clean-room techniques has proven challenging, and has in fact so far prevented their integration into monolithic microcavities altogether. As a result, efficient, narrowband organic single-photon sources for applications in quantum information processing have remained elusive despite their considerable promise. Here, we propose three monolithic microcavity designs tailored to provide sufficient Purcell enhancement for organic quantum emitters. The Purcell effect induced by these cavities preferentially enhances emission into the 0-0 zero-phonon line, increasing spectral purity, photon extraction, and shortening the excited-state lifetime, which in turn relaxes the requirements for generating indistinguishable photons. The cavities have been optimized using Bayesian optimization and the adaptive Antoulas-Anderson (AAA) algorithm for rational approximation, which offer global optimization and the efficient reconstruction of spectra from scattering simulations, respectively. These structures are compatible with both standard clean-room processing and single-molecule preparation techniques. Therefore, they offer a clear route to realize high-quality, practically monochromatic organic single-photon light sources.

quant-ph↗

arXiv2026

Organic molecules as single-photon sources

The development of single-photon sources has been nothing but rapid in recent years, with quantum emitter-based systems showing especially impressive progress. In this article, we give an overview of the developments in single-photon sources based on single molecules. We will introduce polycyclic hydrocarbons as the most commonly used emitter systems for the realization of an organic solid-state single-photon source. At cryogenic temperatures this special class of fluorescent molecules demonstrates remarkable optical properties such as negligible dephasing, indefinite photostability, and high photon rates, which make them attractive as fundamental building blocks in emerging quantum technologies. To better understand the general properties and limitations of these molecules, we discuss sample preparation and relevant emitter parameters such as absorption and emission spectra, lifetime, and dephasing. We will also give an overview of light extraction strategies as a crucial part of a single-photon source. Finally, we conclude with a look into the future, displaying current challenges and possible solutions.

quant-ph↗

arXiv2025

Nano-electronvolt Fourier-limited transition of a single surface-adsorbed molecule

High-resolution spectroscopy allows one to probe weak interactions and to detect subtle phenomena. While such measurements are routinely performed on atoms and molecules in the gas phase, spectroscopy of adsorbed species on surfaces is faced with challenges. As a result, previous studies of surface-adsorbed molecules have fallen short of the ultimate resolution, where the transition linewidth is determined by the lifetime of the excited state. In this work, we conceive a new approach to surface deposition and report on Fourier-limited electronic transitions in single dibenzoterrylenes adsorbed onto the surface of an anthracene crystal. By performing spectroscopy and super-resolution microscopy at liquid helium temperature, we shed light on various properties of the adsorbed molecules. Our experimental results pave the way for a new class of experiments in surface science, where high spatial and spectral resolution can be combined.

physics.chem-ph↗

arXiv2024

Cavity-mediated hybridization of several molecules in the strong coupling regime

Molecular complexes are held together via a variety of bonds, but they all share the common feature that their individual entities are in contact. In this work, we introduce and demonstrate the concept of a \textit{molecular optical bond}, resulting from the far-field electromagnetic coupling of several molecules via a shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and sub-radiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.

cond-mat.mes-hall↗

arXiv2024

High-resolution Cryogenic Spectroscopy of Single Molecules in Nanoprinted Crystals

We perform laser spectroscopy at liquid helium temperatures (T=2 K) to investigate single dibenzoterrylene (DBT) molecules doped in anthracene crystals of nanoscopic height fabricated by electrohydrodynamic dripping. Using high-resolution fluorescence excitation spectroscopy, we show that zero-phonon lines of single molecules in printed nanocrystals are nearly as narrow as the Fourier-limited transitions observed for the same guest-host system in the bulk. Moreover, the spectral instabilities are comparable to or less than one linewidth. By recording super-resolution images of DBT molecules and varying the polarization of the excitation beam, we determine the dimensions of the printed crystals and the orientation of the crystals' axes. Electrohydrodynamic printing of organic nano and microcrystals paves the way for a series of applications, where controlled positioning of quantum emitters with narrow optical transitions is desirable.

quant-ph↗

arXiv2023

Spectral splitting of a stimulated Raman transition in a single molecule

The small cross section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operation at T < 2K, we succeed at driving a coherent stimulated Raman transition in individual molecules. We observe and model a spectral splitting that serves as a characteristic signature of the phenomenon at hand. Our study sets the ground for exploiting the intrinsic optomechanical degrees of freedom of molecules for applications in solid-state quantum optics and information processing.

quant-ph↗

arXiv2023

Organic molecules as origin of visible-range single photon emission from hexagonal boron nitride and mica

The discovery of room-temperature single-photon emitters (SPEs) hosted by two-dimensional hexagonal boron nitride (2D hBN) has sparked intense research interest. Although emitters in the vicinity of 2 eV have been studied extensively, their microscopic identity has remained elusive. The discussion of this class of SPEs has centered on point defects in the hBN crystal lattice, but none of the candidate defect structures have been able to capture the great heterogeneity in emitter properties that is observed experimentally. Employing a widely used sample preparation protocol but disentangling several confounding factors, we demonstrate conclusively that heterogeneous single-photon emission ~2 eV associated with hBN originates from organic molecules, presumably aromatic fluorophores. The appearance of those SPEs depends critically on the presence of organic processing residues during sample preparation, and emitters formed during heat treatment are not located within the hBN crystal as previously thought, but at the hBN/substrate interface. We further demonstrate that the same class of SPEs can be observed in a different 2D insulator, fluorophlogopite mica.

physics.optics↗

arXiv2023

Quantum Efficiency of Single Dibenzoterrylene Molecules in para-Dichlorobenzene at Cryogenic Temperatures

We measure the quantum efficiency (QE) of individual dibenzoterrylene (DBT) molecules embedded in para-dichlorobenzene at cryogenic temperatures. To achieve this, we apply two distinct methods based on the maximal photon emission and on the power required to saturate the zero-phonon line. We find that the outcome of the two approaches are in good agreement, reporting a large fraction of molecules with QE values above 50%, with some exceeding 70%. Furthermore, we observe no correlation between the observed lower bound on the QE and the lifetime of the molecule, suggesting that most of the molecules have a QE exceeding the established lower bound. This confirms the suitability of DBT for quantum optics experiments. In light of previous reports of low QE values at ambient conditions, our results hint at the possibility of a strong temperature dependence of the QE.

quant-ph↗

arXiv2023

On-chip interference of scattering from two individual molecules in plastic

Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of organic molecules embedded in a plastic film to a TiO$_2$ microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the molecules with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distance of about 8$\,μ$m and an optical phase difference of about $π/2$, we report on a large collective extinction of the incident light in the forward direction and the destructive interference of its scattering in the backward direction. Our work sets the ground for the coherent coupling of several molecules via a common mode and the realization of polymer-based hybrid quantum photonic circuits.

quant-ph↗

arXiv2022

High-resolution vibronic spectroscopy of a single molecule embedded in a crystal

Vibrational levels of the electronic ground states in dye molecules have not been previously explored at high resolution in solid matrices. We present new spectroscopic measurements on single polycyclic aromatic molecules of dibenzoterrylene embedded in an organic crystal made of para-dichlorobenzene. To do this, we use narrow-band continuous-wave lasers and combine spectroscopy methods based on fluorescence excitation and stimulated emission depletion (STED) to assess individual vibrational linewidths in the electronic ground state at a resolution of ~30 MHz dictated by the linewidth of the electronic excited state. In this fashion, we identify several exceptionally narrow vibronic levels with linewidths down to values around 2GHz. Additionally, we sample the distribution of vibronic wavenumbers, relaxation rates, and Franck-Condon factors, both in the electronic ground and excited states for a handful of individual molecules. We discuss various noteworthy experimental findings and compare them with the outcome of DFT calculations. The highly detailed vibronic spectra obtained in our work pave the way for studying the nanoscopic local environment of single molecules. The approach also provides an improved understanding of the vibrational relaxation mechanisms in the electronic ground state, which may help to create long-lived vibrational states for applications in quantum technology.

quant-ph↗

arXiv2022

A robust tip-less positioning device for near-field investigations: Press and Roll Scan (PROscan)

Scanning probe microscopes scan and manipulate a sharp tip in the immediate vicinity of a sample surface. The limited bandwidth of the feedback mechanism used for stabilizing the separation between the tip and the sample makes the fragile nanoscopic tip very susceptible to mechanical instabilities. We propose, demonstrate and characterize a new alternative device based on bulging a thin substrate against a second substrate and rolling them with respect each other. We showcase the power of this method by placing gold nanoparticles and semiconductor quantum dots on the two opposite substrates and positioning them with nanometer precision to enhance the fluorescence intensity and emission rate. We exhibit the passive mechanical stability of the system over more than one hour. The design concept presented in this work holds promise in a variety of other contexts, where nanoscopic features have to be positioned and kept near contact with each other.

quant-ph↗

arXiv2021

Single-molecule vacuum Rabi splitting: four-wave mixing and optical switching at the single-photon level

A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this work, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the strong coupling regime of cavity quantum electrodynamics. We report on single-photon sensitivity in nonlinear signal generation and all-optical switching. Our work promotes the use of molecules for applications such as integrated photonic circuits, operating at very low powers.

quant-ph↗

arXiv2020

Nanoscopic charge fluctuations in a gallium phosphide waveguide measured by single molecules

We present efficient coupling of single organic molecules to a gallium phosphide subwavelength waveguide (nanoguide). By examining and correlating the temporal dynamics of various single-molecule resonances at different locations along the nanoguide, we reveal light-induced fluctuations of their Stark shifts. Our observations are consistent with the predictions of a simple model based on the optical activation of a small number of charges in the GaP nanostructure.

quant-ph↗

arXiv2020

The Truncated Metallo-dielectric Omnidirectional Reflector: Collecting Single Photons in the Fundamental Gaussian Mode with 95% Efficiency

We propose a novel antenna structure which funnels single photons from a single emitter with unprecedented efficiency into a low-divergence fundamental Gaussian mode. Our device relies on the concept of creating an omnidirectional photonic bandgap to inhibit unwanted large-angle emission and to enhance small-angle defect-guided-mode emission. The new photon collection strategy is intuitively illustrated, rigorously verified and optimized by implementing an efficient body-of-revolution finite-difference time-domain method for in-plane dipole emitters. We investigate a few antenna designs to cover various boundary conditions posed by fabrication processes or material restrictions and theoretically demonstrate that collection efficiencies into the fundamental Gaussian mode exceeding 95% are achievable. Our antennas are broadband, insensitive to fabrication imperfections and compatible with a variety of solid-state emitters such as organic molecules, quantum dots and defect centers in diamond. Unidirectional and low-divergence Gaussian-mode emission from a single emitter may enable the realization of a variety of photonic quantum computer architectures as well as highly efficient light-matter interfaces.

physics.optics↗

arXiv2020

Thermal origin of light emission in non-resonant and resonant tunnel junctions

Electron tunneling is associated with light emission. In order to elucidate its generating mechanism, we provide a novel experimental ansatz that employs fixed-distance epitaxial graphene as metallic electrodes. In contrast to previous experiments, this permits an unobscured light spread from the tunnel junction, enabling both a reliable calibration of the visible to infrared emission spectrum and a detailed analysis of the dependence of the parameters involved. In an open, non-resonant geometry, the emitted light is perfectly characterized by a Planck spectrum. In an electromagnetically resonant environment, resonant radiation is added to the thermal spectrum, both being strictly proportional in intensity. In full agreement with a simple heat conduction model, we provide evidence that in both cases the light emission stems from a hot electronic subsystem in interaction with its linear electromagnetic environment. These very clear results should resolve any ambiguity about the mechanism of light emission in nano contacts.

cond-mat.mes-hall↗

arXiv2020

Partial cloaking of a gold particle by a single molecule

Extinction of light by material particles stems from losses incurred by absorption or scattering. The extinction cross section is usually treated as an additive quantity, leading to the exponential laws that govern the macroscopic attenuation of light. In this work, we demonstrate that the extinction cross section of a large gold nanoparticle can be substantially reduced, i.e., the particle becomes more transparent, if a single molecule is placed in its near field. This partial cloaking effect results from a coherent plasmonic interaction between the molecule and the nanoparticle, whereby each of them acts as a nano-antenna to modify the radiative properties of the other.

quant-ph↗

arXiv2019

Coherent nonlinear optics of quantum emitters in nanophotonic waveguides

Coherent quantum optics, where the interaction of a photon with an emitter does not scramble phase coherence, lies at the heart of many quantum optical effects and emerging technologies. Solid-state emitters coupled to nanophotonic waveguides are a promising platform for quantum devices, as this combination is scalable. Yet, reaching full coherence in these systems is challenging due to the dynamics of the solid-state environment of the emitters. Here, we review progress towards coherent light-matter interactions with solid-state quantum emitters coupled to nanophotonic waveguides. We first lay down the theoretical foundation for coherent and nonlinear light-matter interactions of a two-level system in a quasi-one-dimensional system, and then benchmark experimental realizations. We then discuss higher-order nonlinearities that arise due to the addition of photons of different frequencies, more complex energy-level schemes of the emitters, and the coupling of multiple emitters via a shared photonic mode. Throughout, we highlight protocols for applications and novel effects that are based on these coherent interactions, the steps taken towards their realization, and the challenges that remain to be overcome.

quant-ph↗