Korenobu Matsuzaki, Simon Vassant, Hsuan-Wei Liu, Anke Dutschke, Björn Hoffmann, Xuewen Chen, Silke Christiansen, Matthew R. Buck, Jennifer A. Hollingsworth, Stephan Götzinger, Vahid Sandoghdar
Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other non-radiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60% and 70%, respectively, in very good agreement with the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics.
Charles Santori, Stephan Gotzinger, Yoshihisa Yamamoto, Satoshi Kako, Katsuyuki Hoshino, Yasuhiko Arakawa
We present measurements of the second-order coherence function on emission from single GaN quantum dots. In some cases a large degree of photon antibunching is observed, demonstrating isolation of a single quantum system. For a selected quantum dot, we study the dependence of photon antibunching on excitation power and temperature. Using pulsed excitation, we demonstrate an ultraviolet triggered single-photon source operating at a wavelength of 358 nm.
Daqing Wang, Hrishikesh Kelkar, Diego Martin-Cano, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Dec 15, 2016·quant-ph·PDF Organic dye molecules have been used in great many scientific and technological applications, but their wider use in quantum optics has been hampered by transitions to short-lived vibrational levels, which limit their coherence properties. To remedy this, one can take advantage of optical resonators. Here we present the first results on coherent molecule-resonator coupling, where a single polycyclic aromatic hydrocarbon molecule extinguishes 38\% of the light entering a microcavity at liquid helium temperature. We also demonstrate four-fold improvement of single-molecule stimulated emission compared to free-space focusing and set the ground for coherent mechanical manipulation of the molecular transition. Our experimental approach based on a microcavity of low mode volume and low quality factor paves the way for the realization of various nonlinear and collective quantum optical effects with molecules.
Masoud Mirzaei, Alexey Shkarin, Burak Gurlek, Johannes Zirkelbach, Ashley J. Shin, Irena Deperasińska, Boleslaw Kozankiewicz, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
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.
Jahangir Nobakht, André Pscherer, Jan Renger, Stephan Götzinger, Vahid Sandoghdar
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.
M. Celebrano, R. Lettow, P. Kukura, M. Agio, A. Renn, S. Goetzinger, V. Sandoghdar
Nov 16, 2009·quant-ph·PDF We demonstrate strong coupling of single photons emitted by individual molecules at cryogenic and ambient conditions to individual nanoparticles. We provide images obtained both in transmission and reflection, where an efficiency greater than 55% was achieved in converting incident narrow-band photons to plasmon-polaritons (plasmons) of a silver nanoparticle. Our work paves the way to spectroscopy and microscopy of nano-objects with sub-shot noise beams of light and to triggered generation of single plasmons and electrons in a well-controlled manner.
A. Mazzei, S. Gotzinger, L. de S. Menezes, G. Zumofen, O. Benson, V. Sandoghdar
Sep 24, 2007·quant-ph·PDF We present experiments where a single subwavelength scatterer is used to examine and control the back-scattering induced coupling between counterpropagating high-Q modes of a microsphere resonator. Our measurements reveal the standing wave character of the resulting symmetric and antisymmetric eigenmodes, their unbalanced intensity distributions, and the coherent nature of their coupling. We discuss our findings and the underlying classical physics in the framework common to quantum optics and provide a particularly intuitive explanation of the central processes.
Mohammad Musavinezhad, Dominik Rattenbacher, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Mar 22, 2023·quant-ph·PDF 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.
Johannes Zirkelbach, Burak Gurlek, Masoud Mirzaei, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Feb 28, 2023·quant-ph·PDF 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.
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 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.
Sanli Faez, Pierre Türschmann, Harald R. Haakh, Stephan Götzinger, Vahid Sandoghdar
We present a new scheme for performing optical spectroscopy on single molecules. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor ($β$) of 18% for the dye molecules doped in the organic crystal. Combination of extinction, fluorescence excitation and resonance fluorescence spectroscopy with microscopy provides high-resolution spatio-spectral access to a very large number of single molecules in a linear geometry. We discuss strategies for exploring a range of quantum optical phenomena, including coherent cooperative interactions in a mesoscopic ensemble of molecules mediated by a single mode of propagating photons.
Nir Rotenberg, Pierre Tuerschmann, Harald Haakh, Diego Martin-Cano, Stephan Goetzinger, Vahid Sandoghdar
Oct 11, 2016·quant-ph·PDF Nanophotonic interfaces between single emitters and light promise to enable new quantum optical technologies. Here, we use a combination of finite element simulations and analytic quantum theory to investigate the interaction of various quantum emitters with slot-waveguide rings. We predict that for rings with radii as small as 1.44 $μ$m (Q = 27,900), near-unity emitter-waveguide coupling efficiencies and emission enhancements on the order of 1300 can be achieved. By tuning the ring geometry or introducing losses, we show that realistic emitter-ring systems can be made to be either weakly or strongly coupled, so that we can observe Rabi oscillations in the decay dynamics even for micron-sized rings. Moreover, we demonstrate that slot waveguide rings can be used to directionally couple emission, again with near-unity efficiency. Our results pave the way for integrated solid-state quantum circuits involving various emitters.
David Press, Stephan Goetzinger, Stephan Reitzenstein, Carolin Hofmann, Andreas Loeffler, Martin Kamp, Alfred Forchel, Yoshihisa Yamamoto
Sep 26, 2006·quant-ph·PDF We observe antibunching in the photons emitted from a strongly-coupled single quantum dot and pillar microcavity in resonance. When the quantum dot was spectrally detuned from the cavity mode, the cavity emission remained antibunched, and also anticorrelated from the quantum dot emission. Resonant pumping of the selected quantum dot via an excited state enabled these observations by eliminating the background emitters that are usually coupled to the cavity. This device demonstrates an on-demand single photon source operating in the strong coupling regime, with a Purcell factor of 61 and quantum effciency of 97%
Mohammad Musavinezhad, Jan Renger, Johannes Zirkelbach, Tobias Utikal, Claudio U. Hail, Thomas Basché, Dimos Poulikakos, Stephan Götzinger, Vahid Sandoghdar
Feb 12, 2024·quant-ph·PDF 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.
Alexey Shkarin, Stephan Götzinger
Feb 19, 2026·quant-ph·PDF 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, light collection strategies 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.
S. Gotzinger, L. de S. Menezes, A. Mazzei, O. Benson, S. Kuhn, V. Sandoghdar
Apr 11, 2006·quant-ph·PDF We realize controlled cavity-mediated photon transfer between two single nanoparticles over a distance of several tens of micrometers. First, we show how a single nanoscopic emitter attached to a near-field probe can be coupled to high-Q whispering-gallery modes of a silica microsphere at will. Then we demonstrate transfer of energy between this and a second nanoparticle deposited on the sphere surface. We estimate the photon transfer efficiency to be about six orders of magnitude higher than that via free space propagation at comparable separations.
Y. L. A. Rezus, S. G. Walt, R. Lettow, A. Renn, G. Zumofen, S. Goetzinger, V. Sandoghdar
Oct 19, 2011·quant-ph·PDF Exploring the interaction of light and matter at the ultimate limit of single photons and single emitters is of great interest both from a fundamental point of view and for emerging applications in quantum engineering. However, the difficulty of generating single photons with specific wavelengths, bandwidths and brightness as well as the weak interaction probability of a single photon with an optical emitter pose a formidable challenge toward this goal. Here, we demonstrate a general approach based on the creation of single photons from a single emitter and their use for performing spectroscopy on a second emitter situated at a distance. Although we used organic molecules as emitters, our strategy is readily extendable to other material systems such as quantum dots and color centers. Our work ushers in a new line of experiments that provide access to the coherent and nonlinear couplings of few emitters and few propagating photons.
R. Lettow, Y. L. A. Rezus, A. Renn, G. Zumofen, E. Ikonen, S. Goetzinger, V. Sandoghdar
Nov 16, 2009·quant-ph·PDF We demonstrate two-photon interference using two remote single molecules as bright solid-state sources of indistinguishable photons. By varying the transition frequency and spectral width of one molecule, we tune and explore the effect of photon distinguishability. We discuss future improvements on the brightness of single-photon beams, their integration by large numbers on chips, and the extension of our experimental scheme to coupling and entanglement of distant molecules.
K. G. Lee, X. W. Chen, H. Eghlidi, P. Kukura, R. Lettow, A. Renn, V. Sandoghdar, S. Götzinger
Sep 20, 2010·quant-ph·PDF Single emitters have been considered as sources of single photons in various contexts such as cryptography, quantum computation, spectroscopy, and metrology. The success of these applications will crucially rely on the efficient directional emission of photons into well-defined modes. To accomplish a high efficiency, researchers have investigated microcavities at cryogenic temperatures, photonic nanowires, and near-field coupling to metallic nano-antennas. However, despite an impressive progress, the existing realizations substantially fall short of unity collection efficiency. Here we report on a theoretical and experimental study of a dielectric planar antenna, which uses a layered structure for tailoring the angular emission of a single oriented molecule. We demonstrate a collection efficiency of 96% using a microscope objective at room temperature and obtain record detection rates of about 50 MHz. Our scheme is wavelength-insensitive and can be readily extended to other solid-state emitters such as color centers and semiconductor quantum dots.
K. -G. Lee, H. Eghlidi, X-W. Chen, A. Renn, S. Götzinger, V. Sandoghdar
We report on two orders of magnitude reduction in the fluorescence lifetime when a single molecule placed in a thin film is surrounded by two gold nanospheres across the film interface. By attaching one of the gold particles to the end of a glass fiber tip, we could control the modification of the molecular fluorescence at will. We find a good agreement between our experimental data and the outcome of numerical calculations.