Hadi Eghlidi, Kwang Geol Lee, Xue-Wen Chen, Stephan Goetzinger, Vahid Sandoghdar
Single gold nanoparticles can act as nanoantennas for enhancing the fluorescence of emitters in their near-fields. Here we present experimental and theoretical studies of scanning antenna-based fluorescence microscopy as a function of the diameter of the gold nanoparticle. We examine the interplay between fluorescence enhancement and spatial resolution and discuss the requirements for deciphering single molecules in a dense sample. Resolutions better than 20 nm and fluorescence enhancement up to 30 times are demonstrated experimentally. By accounting for the tip shaft and the sample interface in finite-difference time-domain calculations, we explain why the measured fluorescence enhancements are higher in the presence of an interface than the values predicted for a homogeneous environment.
Xue-Wen Chen, Stephan Goetzinger, Vahid Sandoghdar
Jun 15, 2011·quant-ph·PDF In Nature Photonics 5, 166 (2011), we reported on a planar dielectric antenna that achieved 96% efficiency in collecting the photons emitted by a single molecule. In that work the transition dipole moment of the molecule was set perpendicular to the antenna plane. Here, we present an extension of that scheme that reaches collection efficiencies beyond 99% for emitters with arbitrarily oriented dipole moments. Our work opens important doors in a wide range of contexts including quantum optics, quantum metrology, nano-analytics, and biophysics. In particular, we provide antenna parameters to realize ultrabright single-photon sources in high-index materials such as semiconductor quantum dots and color centers in diamond, as well as sensitive detection of single molecules in nanofluidic devices.
Christian Ott, Stephan Götzinger, Heiko B. Weber
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.
Dominik Rattenbacher, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Jan 26, 2023·quant-ph·PDF 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.
Johannes Zirkelbach, Benjamin Gmeiner, Jan Renger, Pierre Türschmann, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Apr 17, 2020·quant-ph·PDF 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.
Pierre Türschmann, Nir Rotenberg, Jan Renger, Irina Harder, Olga Lohse, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Feb 20, 2017·quant-ph·PDF While experiments with one or two quantum emitters have become routine in various laboratories, scalable platforms for efficient optical coupling of many quantum systems remain elusive. To address this issue, we report on chip-based systems made of one-dimensional subwavelength dielectric waveguides (nanoguides) and polycyclic aromatic hydrocarbon molecules. After discussing the design and fabrication requirements, we present data on coherent linear and nonlinear spectroscopy of single molecules coupled to a nanoguide mode. Our results show that external microelectrodes as well as optical beams can be used to switch the propagation of light in a nanoguide via the Stark effect and a nonlinear optical process, respectively. The presented nanoguide 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.
Andreas Maser, Benjamin Gmeiner, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Sep 17, 2015·quant-ph·PDF The pioneering experiments of linear spectroscopy were performed using flames in the 1800s, but nonlinear optical measurements had to wait until lasers became available in the twentieth century. Because the nonlinear cross section of materials is very small, usually macroscopic bulk samples and pulsed lasers are used. Numerous efforts have explored coherent nonlinear signal generation from individual nanoparticles or small atomic ensembles with millions of atoms. Experiments on a single semiconductor quantum dot have also been reported, albeit with a very small yield. Here, we report on coherent nonlinear spectroscopy of a single molecule under continuous-wave single-pass illumination, where efficient photon-molecule coupling in a tight focus allows switching of a laser beam by less than a handful of pump photons nearly resonant with the sharp molecular transition. Aside from their fundamental importance, our results emphasize the potential of organic molecules for applications such as quantum information processing, which require strong nonlinearities.
Hrishikesh Kelkar, Daqing Wang, Diego Martín-Cano, Björn Hoffmann, Silke Christiansen, Stephan Götzinger, Vahid Sandoghdar
We report on the realization of an open plane-concave Fabry-Pérot resonator with a mode volume below $λ^3$ at optical frequencies. We discuss some of the less common features of this new microcavity regime and show that the ultrasmall mode volume allows us to detect cavity resonance shifts induced by single nanoparticles even at quality factors as low as $100$. Being based on low-reflectivity micromirrors fabricated on a silicon cantilever, our experimental arrangement provides broadband operation, tunability of the cavity resonance, lateral scanning and promise for optomechanical studies.
Pierre Türschmann, Hanna Le Jeannic, Signe F. Simonsen, Harald R. Haakh, Stephan Götzinger, Vahid Sandoghdar, Peter Lodahl, Nir Rotenberg
Jun 20, 2019·quant-ph·PDF 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.
André Pscherer, Manuel Meierhofer, Daqing Wang, Hrishikesh Kelkar, Diego Martín-Cano, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
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.
Xiao-Liu Chu, Stephan Götzinger, Vahid Sandoghdar
Aug 29, 2016·quant-ph·PDF A two-level atom cannot emit more than one photon at a time. As early as the 1980s, this quantum feature was identified as a gateway to "single-photon sources", where a regular excitation sequence would create a stream of light particles with photon number fluctuations below the shot noise. Such an intensity squeezed beam of light would be desirable for a range of applications such as quantum imaging, sensing, enhanced precision measurements and information processing. However, experimental realizations of these sources have been hindered by large losses caused by low photon collection efficiencies and photophysical shortcomings. By using a planar metallo-dielectric antenna applied to an organic molecule, we demonstrate the most regular stream of single photons reported to date. Measured intensity fluctuations reveal 2.2 dB squeezing limited by our detection efficiency, equivalent to 6.2 dB intensity squeezing right after the antenna.
Emanuel Eichhammer, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Rare earth ions in crystals exhibit narrow spectral features and hyperfine-split ground states with exceptionally long coherence times. These features make them ideal platforms for quantum information processing in the solid state. Recently, we reported on the first high-resolution spectroscopy of single Pr$^{3+}$ ions in yttrium orthosilicate (YSO) nanocrystals. While in that work we examined the less explored $^3$H$_4$-$^3$P$_0$ transition at a wavelength of 488 nm, here we extend our investigations to the $^3$H$_4$-$^1$D$_2$ transition at 606 nm. In addition, we present measurements of the second-order autocorrelation function, fluorescence lifetime, and emission spectra of single ions as well as their polarization dependencies on both transitions; these data were not within the reach of the first experiments reported earlier. Furthermore, we show that by a proper choice of the crystallite, one can obtain narrower spectral lines and, thus, resolve the hyperfine levels of the excited state. We expect our results to make single-ion spectroscopy accessible to a larger scientific community.
Tobias Utikal, Emanuel Eichhammer, Lutz Petersen, Alois Renn, Stephan Götzinger, Vahid Sandoghdar
Oct 30, 2013·quant-ph·PDF Solid-state emitters with atom-like optical and magnetic transitions are highly desirable for efficient and scalable quantum state engineering and information processing. Quantum dots, color centers and impurities embedded in inorganic hosts have attracted a great deal of attention in this context, but influences from the matrix continue to pose challenges on the degree of attainable coherence in each system. We report on a new solid-state platform based on the optical detection of single praseodymium ions via 4f intrashell transitions, which are well shielded from their surroundings. By combining cryogenic high-resolution laser spectroscopy with fluorescence microscopy, we were able to spectrally select and spatially resolve individual ions. In addition to elaborating on the essential experimental steps for achieving this long-sought goal, we demonstrate state preparation and read out of the three ground-state hyperfine levels, which are known to have lifetimes of the order of hundred seconds.
Johannes Zirkelbach, Masoud Mirzaei, Irena Deperasinska, Boleslaw Kozankiewicz, Burak Gurlek, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
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.
Michael Neumann, Xu Wei, Luis Morales-Inostroza, Seunghyun Song, Sung-Gyu Lee, Kenji Watanabe, Takashi Taniguchi, Stephan Götzinger, Young Hee Lee
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.
Hsuan-Wei Liu, Michael A. Becker, Korenobu Matsuzaki, Randhir Kumar, Stephan Götzinger, Vahid Sandoghdar
Mar 10, 2022·quant-ph·PDF 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.
Noah Mendelson, Luis Morales, Chi Li, Ritika Ritika, Minh Anh Phan Nguyen, Jacqueline Loyola-Echeverria, Sejeong Kim, Stephan Gotzinger, Milos Toth, Igor Aharonovich
Point defects in hexagonal boron nitride have emerged as a promising quantum light source due to their bright and photostable room temperature emission. In this work, we study the incorporation of quantum emitters during chemical vapor deposition growth on a nickel substrate. Combining a range of characterization techniques, we demonstrate that the incorporation of quantum emitters is limited to (001) oriented nickel grains. Such emitters display improved emission properties in terms of brightness and stability. We further utilize these emitters and integrate them with a compact optical antenna enhancing light collection from the sources. The hybrid device yields average saturation count rates of ~2.9 x106 cps and an average photon purity of ~90%. Our results advance the controlled generation of spatially distributed quantum emitters in hBN and demonstrate a key step towards on-chip devices with maximum collection efficiency.
Daqing Wang, Hrishikesh Kelkar, Diego Martin-Cano, Dominik Rattenbacher, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Sep 20, 2018·quant-ph·PDF Molecules are ubiquitous in natural phenomena and man-made products, but their use in quantum optical applications has been hampered by incoherent internal vibrations and other phononic interactions with their environment. We have now succeeded in turning an organic molecule into a coherent two-level quantum system by placing it in an optical microcavity. This allows several unprecedented observations such as 99\% extinction of a laser beam by a single molecule, saturation with less than 0.5 photon, and nonclassical generation of few-photon super-bunched light. Furthermore, we demonstrate efficient interaction of the molecule-microcavity system with single photons generated by a second molecule in a distant laboratory. Our achievements pave the way for linear and nonlinear quantum photonic circuits based on organic platforms.
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 sub-wavelength waveguides (nanoguides). We discuss fabrication and characterization of the chip-based nanophotonic elements which yield resonator finesse in the order of 20 when covered by molecular crystals. Our observed extinction dips from single molecules reach 22%, consistent with the expected Purcell enhancements up to 11 folds. 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.
Wancong Li, Luis Morales-Inostroza, Weiwang Xu, Pu Zhang, Jan Renger, Stephan Götzinger, Xue-Wen Chen
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.