Dr. Jan Renger

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

Mohammad Musavinezhad, Alexey Shkarin, Dominik Rattenbacher, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

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

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

Dominik Rattenbacher, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

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 TiO2 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 8μm 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.

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

Alexey Shkarin, Dominik Rattenbacher, Jan Renger, Simon Hönl, Tobias Utikal, Paul Seidler, Stephan Götzinger, Vahid Sandoghdar

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

Nanostructured alkali-metal vapor cells

Tom F. Cutler, William J. Hamlyn, Jan Renger, Kate A. Whittaker, Danielle Pizzey, Ifan G. Hughes, Vahid Sandoghdar, Charles S. Adams

Atom-light interactions in nano-scale systems hold great promise for novel technologies based on integrated emitters and optical modes. We present the design architecture, construction method,<br>and characterization of an all-glass alkali-metal vapor cell with nanometer-scale internal structure. Our cell has a glue-free design which allows versatile optical access, in particular with high numerical aperture optics. By performing spectroscopy in different illumination and detection schemes, we investigate atomic densities and velocity distributions in various nanoscopic landscapes. We apply a two-photon excitation scheme to atoms confined in one dimension within our cells, achieving a resonance line-width of 32 MHz in a counter-propagating geometry, and 57.5 MHz in a co-propagating geometry. Both of these are considerably narrower than the Doppler width (GHz), and are limited<br>by transit time broadening and velocity selection. We also demonstrate sub-Doppler line-widths for atoms confined in two dimensions to micron-sized channels. Furthermore, we illustrate control over vapor density within our cells through nano-scale confinement alone, which could offer a scalable route towards room-temperature devices with single atoms within an interaction volume. Our design offers a robust platform for miniaturized devices that could easily be combined with integrated<br>photonic circuits.

suggested by editors

Partial cloaking of a gold particle by a single molecule

Johannes Zirkelbach, Benjamin Gmeiner, Jan Renger, Pierre Türschmann, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

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<br>more transparent, if a single molecule is placed in its near field. This partial cloaking eect 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.

suggested by editors

Coherent coupling of single molecules to on-chip ring resonators

Dominik Rattenbacher, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

We report on cryogenic coupling of organic molecules to ring microresonators obtained by looping subwavelength waveguides (nanoguides). We discuss fabrication and characterization of the chip-based nanophotonic elements which yield a resonator finesse in the order of 20 when covered by molecular crystals. Our observed extinction dips from single molecules reach 22%, consistent with an expected enhancement factor of up to 11 for the molecular emission into the nanoguide. Future efforts will aim at efficient coupling of a handful of molecules via their interaction with a ring microresonator mode, setting the ground for the realization of quantum optical cooperative effects.

Nanoprinting organic molecules at the quantum level

Claudio U. Hail, Christian Höller, Korenobu Matsuzaki, Patrik Rohner, Jan Renger, Vahid Sandoghdar, Dimos Poulikakos, Hadi Eghlidi

Organic compounds present a powerful platform for nanotechnological applications. In particular, molecules suitable for optical functionalities such as single photon generation and energy transfer have great promise for complex nanophotonic circuitry due to their large variety of spectral properties, efficient absorption and emission, and ease of synthesis. Optimal integration, however, calls for control over position and orientation of individual molecules. While various methods have been explored for reaching this regime in the past, none satisfies requirements necessary for practical applications. Here, we present direct non-contact electrohydrodynamic nanoprinting of a countable number of photostable and oriented molecules in a nanocrystal host with subwavelength positioning accuracy. We demonstrate the power of our approach by writing arbitrary patterns and controlled coupling of single molecules to the near field of optical nanostructures. Placement precision, high yield and fabrication facility of our method open many doors for the realization of novel nanophotonic devices.

Chip-Based All-Optical Control of Single Molecules Coherently Coupled to a Nanoguide

Pierre Tuerschmann, Nir Rotenberg, Jan Renger, Irina Harder, Olga Lohse, Tobias Utikal, Stephan Goetzinger, Vahid Sandoghdar

The feasibility of many proposals in nano quantum-optics depends on the efficient coupling of photons to individual quantum emitters, the possibility to control this interaction on demand, and the scalability of the experimental platform. To address these issues, we report on chip-based systems made of one-dimensional subwavelength dielectric waveguides (nanoguides) and polycyclic aromatic hydrocarbon molecules. We discuss the design and fabrication requirements, present data on extinction spectroscopy of single molecules coupled to a nanoguide mode, and show how an external optical beam can switch the propagation of light via a nonlinear optical process. The presented architecture paves the way for the investigation of many-body phenomena and polaritonic states and can be readily extended to more complex geometries for the realization of quantum integrated photonic circuits.

Pushing the Photon Limit: Nanoantennas Increase Maximal Photon Stream and Total Photon Number

Emilie Wientjes, Jan Renger, Richard Cogdell, Niek F. van Hulst

Nanoantennas are well-known for their effective role in fluorescence enhancement, both in excitation and emission. Enhancements of 3-4 orders of magnitude have been reported. Yet in practice, the photon emission is limited by saturation due to the time that a molecule spends in singlet and especially triplet excited states. The maximal photon stream restricts the attainable enhancement. Furthermore, the total number of photons emitted is limited by photobleaching. The limited brightness and observation time are a drawback for applications, especially in biology. Here we challenge this photon limit, showing that nanoantennas can actually increase both saturation intensity and photostability. So far, this limit-shifting role of nanoantennas has hardly been explored. Specifically, we demonstrate that single light-harvesting complexes, under saturating excitation conditions, show over a 50-fold antenna-enhanced photon emission stream, with 10-fold more total photons, up to 108 detected photons, before photobleaching. This work shows yet another facet of the great potential of nanoantennas in the world of single-molecule biology.