Super-resolution localization microscopy is based on determining the positions of individual fluorescent markers in a sample. The major challenge in reaching an ever higher localization precision lies in the limited number of collected photons from single emitters. To tackle this issue, it has been shown that one can exploit the increased photostability at low temperatures, reaching localization precisions in the sub-nanometer range. Another crucial ingredient of single-molecule super-resolution imaging is the ability to activate individual emitter within a diffraction-limited spot. Here, we report on photoblinking behavior of organic dyes at low temperature and elaborate on the limitations of this ubiquitous phenomenon for selecting single molecules. We then show that recording the emission polarization not only provides access to the molecular orientation, but it also facilitates the assignment of photons to individual blinking molecules. Furthermore, we employ periodical modulation of the excitation polarization as a robust method to effectively switch fluorophores. We bench mark each approach by resolving two emitters on different DNA origami structures.
Kerker effect, superscattering, and scattering dark states in atomic antennas
Rasoul Alaee Khanghah,
Akbar Safari,
Vahid Sandoghdar,
Robert W. Boyd
Physical Review Research
2
043409
(2020)
| Journal
We study scattering phenomena such as the Kerker effect, superscattering, and scattering dark states in a subwavelength atomic antenna consisting of atoms with only electric dipole transitions. We show that an atomic antenna can exhibit arbitrarily large or small scattering cross sections depending on the geometry of the structure and the direction of the impinging light. We also demonstrate that atoms with only an electric dipole transition can exhibit a directional radiation pattern with zero backscattering when placed in a certain configuration. This is a special case of a phenomenon known as the Kerker effect, which typically occurs in the presence of both electric and magnetic transitions. Our findings open a pathway to design highly directional emitters, nonradiating sources, and highly scattering objects based on individually controlled atoms.
Differential diffusional properties in loose and tight docking prior to membrane fusion
Fusion of biological membranes, although mediated by divergent proteins, is believed to follow a common pathway. It proceeds through distinct steps including docking, merger of proximal leaflets (stalk formation), and formation of a fusion pore. However, the structure of these intermediates is difficult to study due to their short lifetime. Previously, we observed a loosely and tightly docked state preceding leaflet merger using arresting point mutations in SNARE proteins, but the nature of these states remained elusive. Here we used interferometric scattering (iSCAT) microscopy to monitor diffusion of single vesicles across the surface of giant unilamellar vesicles (GUVs). We observed that the diffusion coefficients of arrested vesicles decreased during progression through the intermediate states. Modeling allowed for predicting the number of tethering SNARE complexes upon loose docking and the size of the interacting membrane patches upon tight docking. These results shed new light on the nature of membrane-membrane interactions immediately before fusion.
Grain Dependent Growth of Bright Quantum Emitters in Hexagonal Boron Nitride
Noah Mendelson,
Luis Morales-Inostroza,
Chi Li,
Ritika Ritika,
Minh Anh Phan Nguyen,
Jacqueline Loyola-Echeverria,
Sejeong Kim,
Stephan Götzinger,
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, the incorporation of quantum emitters during chemical vapor deposition growth on a nickel substrate is studied. Combining a range of characterization techniques, it is demonstrated 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. These emitters are further utilized and integrated with a compact optical antenna enhancing light collection from the sources. The hybrid device yields average saturation count rates of ≈2.9 × 106 cps and an average photon purity of g(2)(0) ≈ 0.1. The results advance the understanding of single photon emitter incorporation during chemical vapor deposition growth and demonstrate a key step towards compact devices for achieving maximum collection efficiency.
High-precision protein-tracking with interferometric scattering microscopy
Richard W. Taylor,
Cornelia Holler,
Reza Gholami Mahmoodabadi,
Michelle Küppers,
Houman Mirzaalian Dastjerdi,
Vasily Zaburdaev,
Alexandra Schambony,
Vahid Sandoghdar
Frontiers in Cell and Developmental Biology
8
590158
(2020)
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| PDF
The mobility of proteins and lipids within the cell, sculpted oftentimes by the organisation of the membrane, reveals a great wealth of information on the function and interaction of these molecules as well as the membrane itself. Single particle tracking has proven to be a vital tool to study the mobility of individual molecules and unravel details of their behaviour. Interferometric scattering (iSCAT) microscopy is an emerging technique well suited for visualising the diffusion of gold nanoparticle-labelled membrane proteins to a spatial and temporal resolution beyond the means of traditional fluorescent labels. We discuss the applicability of interferometric single particle tracking (iSPT) microscopy to investigate the minutia in the motion of a protein through measurements visualising the mobility of the epidermal growth factor receptor in various biological scenarios on the live cell.
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
Quantum metamaterials with magnetic response at optical frequencies
Rasoul Alaee Khanghah,
Burak Gürlek,
Mohammad Albooyeh,
Diego-Martin Cano,
Vahid Sandoghdar
We propose novel quantum antennas and metamaterials with strong magnetic response at optical frequencies. Our design is based on the arrangement of natural atoms with only electric dipole transition moments at distances smaller than a wavelength of light but much larger than their physical size. In particular, we show that an atomic dimer can serve as a magnetic antenna at its antisymmetric mode to enhance the decay rate of a magnetic transition in its vicinity by several orders of magnitude. Furthermore, we study metasurfaces composed of atomic bilayers with and without cavities and show that they can fully reflect the electric and magnetic fields of light, thus, forming nearly perfect electric/magnetic mirrors. The proposed quantum metamaterials can be fabricated with available state-of-the-art technologies and promise several applications both in classical optics and quantum engineering.
suggested by editors
Point spread function in interferometric scattering microscopy (iSCAT). Part I: aberrations in defocusing and axial localization
Reza Gholami Mahmoodabadi,
Richard W. Taylor,
Martin Kaller,
Susann Spindler,
Mahdi Mazaheri,
Kiarash Kasaian,
Vahid Sandoghdar
Interferometric scattering (iSCAT) microscopy is an emerging label-free technique optimized for the sensitive detection of nano-matter. Previous iSCAT studies have approximated the point spread function in iSCAT by a Gaussian intensity distribution. However, recent efforts to track the mobility of nanoparticles in challenging speckle environments and over extended axial ranges has necessitated a quantitative description of the interferometric point spread function (iPSF). We present a robust vectorial diffraction model for the iPSF in tandem with experimental measurements and rigorous FDTD simulations. We examine the iPSF under various imaging scenarios to understand how aberrations due to the experimental configuration encode information about the nanoparticle. We show that the lateral shape of the iPSF can be used to achieve nanometric three-dimensional localization over an extended axial range on the order of 10 µm either by means of a fit to an analytical model or calibration-free unsupervised machine learning. Our results have immediate implications for three-dimensional single particle tracking in complex scattering media.
Truncated Metallo-Dielectric Omnidirectional Reflector: Collecting Single Photons in the Fundamental Gaussian Mode with 95% Efficiency
Wancong Li,
Luis Morales-Inostroza,
Weiwang Xu,
Pu Zhang,
Stephan Götzinger,
Xue-Wen Chen
We propose a novel antenna structure that funnelssingle photons from a single emitter with unprecedented efficiencyinto a low-divergence fundamental Gaussian mode. Our devicerelies on the concept of creating an omnidirectional photonicbandgap to inhibit unwanted large-angle emission and to enhancesmall-angle defect-guided-mode emission. The new photoncollection 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 boundaryconditions posed by fabrication processes or material restrictions and theoretically demonstrate that collection efficiencies into thefundamental Gaussian mode exceeding 95% are achievable. Our antennas are broadband, insensitive to fabrication imperfections andcompatible 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 photonicquantum computer architectures as well as highly efficient light−matter interfaces.
Molecule-photon interactions in phononic environments
Michael Reitz,
Christian Sommer,
Burak Gürlek,
Vahid Sandoghdar,
Diego-Martin Cano,
Claudiu Genes
Physical Review Research
2
033270
033270
(2020)
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| PDF
Molecules constitute compact hybrid quantum optical systems that can interface photons, electronic degrees of freedom, localized mechanical vibrations, and phonons. In particular, the strong vibronic interaction between electrons and nuclear motion in a molecule resembles the optomechanical radiation pressure Hamiltonian. While molecular vibrations are often in the ground state even at elevated temperatures, one still needs to get a handle on decoherence channels associated with phonons before an efficient quantum optical network based on optovibrational interactions in solid-state molecular systems could be realized. As a step towards a better understanding of decoherence in phononic environments, we take here an open quantum system approach to the nonequilibrium dynamics of guest molecules embedded in a crystal, identifying regimes of Markovian versus non-Markovian vibrational relaxation. A stochastic treatment, based on quantum Langevin equations, predicts collective vibron-vibron dynamics that resembles processes of sub- and super-radiance for radiative transitions. This in turn leads to the possibility of decoupling intramolecular vibrations from the phononic bath, allowing for enhanced coherence times of collective vibrations. For molecular polaritonics in strongly confined geometries, we also show that the imprint of optovibrational couplings onto the emerging output field results in effective polariton cross-talk rates for finite bath occupancies.
Point spread function in interferometric scattering microscopy (iSCAT). Part I: aberrations in defocusing and axial localization
Reza Gholami Mahmoodabadi,
Richard W. Taylor,
Martin Kaller,
Susann Spindler,
Mahdi Mazaheri,
Kiarash Kasaian,
Vahid Sandoghdar
Interferometric scattering (iSCAT) microscopy is an emerging label-free technique optimized for the sensitive detection of nano-matter. Previous iSCAT studies have approximated the point spread function in iSCAT by a Gaussian intensity distribution. However, recent efforts to track the mobility of nanoparticles in challenging speckle environments and over extended axial ranges has necessitated a quantitative description of the interferometric point spread function (iPSF). We present a robust vectorial diffraction model for the iPSF in tandem with experimental measurements and rigorous FDTD simulations. We examine the iPSF under various imaging scenarios to understand how aberrations due to the experimental configuration encode information about the nanoparticle. We show that the lateral shape of the iPSF can be used to achieve nanometric three-dimensional localization over an extended axial range on the order of 10 µm either by means of a fit to an analytical model or calibration-free unsupervised machine learning. Our results have immediate implications for three-dimensional single particle tracking in complex scattering media.
Sub-nanometer resolution in single-molecule photoluminescence imaging
Ben Yang,
Gong Chen,
Atif Ghafoor,
Yufan Zhang,
Yao Zhang,
Yang Zhang,
Yi Luo,
Jinlong Yang,
Vahid Sandoghdar,
Javier Aizpurua,
Zenchao Dong,
J.G. Hou
Ambitions to reach atomic resolution with light have been a major force in shaping nano-optics, whereby a central challenge is achieving highly localized optical fields. A promising approach employs plasmonic nanoantennas, but fluorescence quenching in the vicinity of metallic structures often imposes a strict limit on the attainable spatial resolution, and previous studies have reached only 8 nm resolution in fluorescence mapping. Here, we demonstrate spatially and spectrally resolved photolumines-cence imaging of a single phthalocyanine molecule coupled to nanocavity plasmons in a tunnelling junction with a spatial reso-lution down to ∼8 Å and locally map the molecular exciton energy and linewidth at sub-molecular resolution. This remarkable resolution is achieved through an exquisite nanocavity control, including tip-apex engineering with an atomistic protrusion, quenching management through emitter–metal decoupling and sub-nanometre positioning precision. Our findings provide new routes to optical imaging, spectroscopy and engineering of light–matter interactions at sub-nanometre scales.
Ultrahigh-speed imaging of rotational diffusion on a lipid bilayer
Mahdi Mazaheri,
Jens Ehrig,
Alexey Shkarin,
Vasily Zaburdaev,
Vahid Sandoghdar
We studied the rotational and translational diffusion of a single gold nanorod linked to a supported lipid bilayer with ultrahigh temporal resolution of two microseconds. By using a home-built polarization-sensitive dark-field microscope, we recorded particle trajectories with lateral precision of three nanometers and rotational precision of four degrees. The large number of trajectory points in our measurements allows us to characterize the statistics of rotational diffusion with unprecedented detail. Our data show apparent signatures of anomalous diffusion such as sublinear scaling of the mean-squared angular displacement and negative values of angular correlation function at small lag times. However, a careful analysis reveals that these effect stem from the residual noise contributions and confirms normal diffusion. Our experimental approach and observations can be extended to investigate diffusive processes of anisotropic nanoparticles in other fundamental systems such as cellular membranes or other two-dimensional fluids.
Ensemble-induced strong light-matter coupling of a single quantum emitter
Stefan Schütz,
Johannes Schachenmayer,
David Hagenmüller,
Gavin K. Brennen,
Thomas Volz,
Vahid Sandoghdar,
Thomas W. Ebbesen,
Claudiu Genes,
Guido Pupillo
We discuss a technique to strongly couple a single target quantum emitter to a cavity mode, which is enabled by virtual excitations of a nearby mesoscopic ensemble of emitters. A collective coupling of the latter to both the cavity and the target emitter induces strong photon nonlinearities in addition to polariton formation, in contrast to common schemes for ensemble strong coupling. We demonstrate that strong coupling at the level of a single emitter can be engineered via coherent and dissipative dipolar interactions with the ensemble, and provide realistic parameters for a possible implementation with <br>SiV− defects in diamond. Our scheme can find applications, amongst others, in quantum information processing or in the field of cavity-assisted quantum chemistry.
Roadmap on quantum light spectroscopy
Shaul Mukamel,
Matthias Freyberger,
Wolfgang Schleich,
Marco Bellini,
Alessandro Zavatta,
Gerd Leuchs,
Christine Silberhorn,
Robert W. Boyd,
Luis Lorenzo Sánchez-Soto,
André Stefanov,
Marco Barbieri,
Anna Paterova,
Leonid Krivitsky,
Sharon Shwartz, et al.
Journal of Physics B: Atomic, Molecular and Optical Physics; IOP Publishing, Bristol
53
7
(2020)
| Journal
Conventional spectroscopy uses classical light to detect matter properties through the variation<br>of its response with frequencies or time delays. Quantum light opens up new avenues for<br>spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and<br>through the variation of photon statistics by coupling to matter. This Roadmap article focuses on<br>using quantum light as a powerful sensing and spectroscopic tool to reveal novel information<br>about complex molecules that is not accessible by classical light. It aims at bridging the quantum<br>optics and spectroscopy communities which normally have opposite goals: manipulating<br>complex light states with simple matter e.g. qubits versus studying complex molecules with<br>simple classical light, respectively. Articles cover advances in the generation and manipulation<br>of state-of-the-art quantum light sources along with applications to sensing, spectroscopy,<br>imaging and interferometry.
Contact
Nano-Optics Division Prof. Vahid Sandoghdar
Max Planck Institute for the Science of Light Staudtstr. 2 91058 Erlangen, Germany
