Cavity-free efficient coupling between emitters and guided modes is of great<br>current interest for nonlinear quantum optics as well as efficient and scalable<br>quantum information processing. In this work, we extend these activities to the<br>coupling of organic dye molecules to a highly confined mode of a nanofiber,<br>allowing mirrorless and low-threshold laser action in an effective mode volume<br>of less than 100 femtoliters. We model this laser system based on<br>semi-classical rate equations and present an analytic compact form of the laser<br>output intensity. Despite the lack of a cavity structure, we achieve a coupling<br>efficiency of the spontaneous emission to the waveguide mode of 0.07(0.01), in<br>agreement with our calculations. In a further experiment, we also demonstrate<br>the use of a plasmonic nanoparticle as a dispersive output coupler. Our laser<br>architecture is promising for a number of applications in optofluidics and<br>provides a fundamental model system for studying nonresonant feedback<br>stimulated emission.
Coherent Interaction of Light and Single Molecules in a Dielectric
Nanoguide
Sanli Faez,
Pierre Tuerschmann,
Harald R. Haakh,
Stephan Goetzinger,
Vahid Sandoghdar
Many of the currently pursued experiments in quantum optics would greatly benefit from a strong interaction between light and matter. Here, we present a simple new scheme for the efficient coupling of single molecules and photons. 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 (beta) of 18% for the dye molecules doped in the organic crystal. A 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 polaritonic interactions in a mesoscopic ensemble of molecules mediated by a single mode of propagating photons.
Experimental realization of an optical antenna designed for collecting 99% of photons from a quantum emitter
X. -L. Chu,
T. J. K. Brenner,
X. -W. Chen,
Y. Ghosh,
J. A. Hollingsworth,
V. Sandoghdar,
Stephan Götzinger
A light source that emits single photons at well-defined times and into a well-defined mode would be a decisive asset for quantum information processing, quantum metrology, and sub-shot-noise detection of absorption. One of the central challenges in the realization of such a deterministic device based on a single quantum emitter concerns the collection of the photons, which are radiated into a 4 pi solid angle. Here, we present the fabrication and characterization of an optical antenna designed to convert the dipolar radiation of an arbitrarily oriented quantum emitter to a directional beam with more than 99% efficiency. Our approach is extremely versatile and can be used for more efficient detection of nanoscopic emitters ranging from semiconductor quantum dots to dye molecules, color centers, or rare-earth ions in various environments. Having addressed the issue of collection efficiency, we also discuss the photophysical limitations of the existing quantum emitters for the realization of a deterministic single-photon source. (C) 2014 Optical Society of America
Large Suppression of Quantum Fluctuations of Light from a Single Emitter
by an Optical Nanostructure
Diego-Martin Cano,
Harald R. Haakh,
Karim Murr,
Mario Agio
We investigate the reduction of the electromagnetic field fluctuations in resonance fluorescence from a single emitter coupled to an optical nanostructure. We find that such hybrid systems can lead to the creation of squeezed states of light, with quantum fluctuations significantly below the shot-noise level. Moreover, the physical conditions for achieving squeezing are strongly relaxed with respect to an emitter in free space. A high degree of control over squeezed light is feasible both in the far and near fields, opening the pathway to its manipulation and applications on the nanoscale with state-of-the-art setups.
Light propagation in conjugated polymer nanowires decoupled from a
substrate
Light-emitting conjugated polymer nanowires are vertically grown and remotely manipulated into a freestanding straight or curved structure in three-dimension. This approach enabled us to eliminate substrate coupling, a critical issue in nanowire photonics in the past decade. We for the first time accomplished characterization of propagation and bending losses of nanowires completely decoupled from a substrate.
Tracking Single Particles on Supported Lipid Membranes: Multimobility
Diffusion and Nanoscopic Confinement
Chia-Lung Hsieh,
Susann Spindler,
Jens Ehrig,
Vahid Sandoghdar
The Journal of Physical Chemistry B
118
1545-1554
(2014)
| Journal
Supported lipid bilayers have been studied intensively over the past two decades. In this work, we study the diffusion of single gold nanoparticles (GNPs) with diameter of 20 nm attached to GM1 ganglioside or DOPE lipids at different concentrations in supported DOPC bilayers. The indefinite photostability of GNPs combined with the high sensitivity of interferometric scattering microscopy (iSCAT) allows us to achieve 1.9 nm spatial precision at 1 ms temporal resolution, while maintaining long recording times. Our trajectories visualize strong transient confinements within domains as small as 20 nm, and the statistical analysis of the data reveals multiple mobilities and deviations from normal diffusion. We present a detailed analysis of our findings and provide interpretations regarding the effect of the supporting substrate and GM1 clustering. We also comment on the use of high-speed iSCAT for investigating diffusion of lipids, proteins, or viruses in lipid membranes with unprecedented spatial and temporal resolution.
Direct optical sensing of single unlabelled proteins and
super-resolution imaging of their binding sites
Detection of single analyte molecules without the use of any label would improve the sensitivity of current biosensors by orders of magnitude to the ultimate graininess of biological matter. Over two decades, scientists have succeeded in pushing the limits of optical detection to single molecules using fluorescence. However, restrictions in photophysics and labelling protocols make this technique less attractive for biosensing. Recently, mechanisms based on vibrational spectroscopy, photothermal detection, plasmonics and microcavities have been explored for fluorescence-free detection of single biomolecules. Here, we show that interferometric detection of scattering (iSCAT) can achieve this goal in a direct and label-free fashion. In particular, we demonstrate detection of cancer marker proteins in buffer solution and in the presence of other abundant proteins. Furthermore, we present super-resolution imaging of protein binding with nanometer localization precision. The ease of iSCAT instrumentation promises a breakthrough for label-free studies of interactions involving proteins and other small biomolecules.
Cryogenic Colocalization Microscopy for Nanometer-Distance Measurements
Siegfried Weisenburger,
Bo Jing,
Dominik Haenni,
Luc Reymond,
Benjamin Schuler,
Alois Renn,
Vahid Sandoghdar
The main limiting factor in spatial resolution of localization microscopy is the number of detected photons. Recently we showed that cryogenic measurements improve the photostability of fluorophores, giving access to Angstrom precision in localization of single molecules. Here, we extend this method to colocalize two fluorophores attached to well-defined positions of a double-stranded DNA. By measuring the separations of the fluorophore pairs prepared at different design positions, we verify the feasibility of cryogenic distance measurement with sub-nanometer accuracy. We discuss the important challenges of our method as well as its potential for further improvement and various applications.
We theoretically propose a temporal cloaking scheme based on accelerating wave packets. A part of a monochromatic light wave is endowed with a discontinuous nonlinear frequency chirp, so that two opposite accelerating caustics are created in space-time as the different frequency components propagate in the presence of dispersion. The two caustics open a biconvex time gap that contains negligible optical energy, thus concealing the enclosed events. In contrast to previous temporal cloaking schemes, where light propagates successively through two different media with opposite dispersions, accelerating wave packets open and close the cloaked time window continuously in a single dispersive medium. In addition, biconvex time gaps can be tailored into arbitrary shapes and offer a larger suppression of intensity compared with their rhombic counterparts. (C) 2014 Optical Society of America
Deep-subwavelength negative-index waveguiding enabled by coupled
conformal surface plasmons
R. Quesada,
D. Martin-Cano,
F. J. Garcia-Vidal,
J. Bravo-Abad
In this Letter we introduce a novel route for achieving negative-group-velocity waveguiding at deep-subwavelength scales. Our scheme is based on the strong electromagnetic coupling between two conformal surface plasmon structures. Using symmetry arguments and detailed numerical simulations, we show that the coupled system can be geometrically tailored to yield negative-index dispersion. A high degree of subwavelength modal confinement, of lambda/10 in the transversal dimensions, is also demonstrated. These results can assist in the development of ultrathin surface circuitry for the low-frequency region (microwave and terahertz regimes) of the electromagnetic spectrum. (C) 2014 Optical Society of America
Dynamical Casimir-Polder interaction between an atom and surface
plasmons
Harald R. Haakh,
Carsten Henkel,
Salvatore Spagnolo,
Lucia Rizzuto,
Roberto Passante
We investigate the time-dependent Casimir-Polder potential of a polarizable two-level atom placed near a surface of arbitrary material, after a sudden change in the parameters of the system. Different initial conditions are taken into account. For an initially bare ground-state atom, the time-dependent Casimir-Polder energy reveals how the atom is "being dressed" by virtual, matter-assisted photons. We also study the transient behavior of the Casimir-Polder interaction between the atom and the surface starting from a partially dressed state, after an externally induced change in the atomic level structure or transition dipoles. The Heisenberg equations are solved through an iterative technique for both atomic and field operators in the medium-assisted electromagnetic field quantization scheme. We analyze, in particular, how the time evolution of the interaction energy depends on the optical properties of the surface, in particular on the dispersion relation of surface plasmon polaritons. The physical significance and the limits of validity of the obtained results are discussed in detail.
Synthesis of a Covalent Monolayer Sheet by Photochemical Anthracene Dimerization at the Air/Water Interface and its Mechanical Characterization by AFM Indentation
Payam Payamyar,
Khaled Kaja,
Carlos Ruiz-Vargas,
Andreas Stemmer,
Daniel J. Murray,
Carey J. Johnson,
Benjamin T. King,
Florian Schiffmann,
Joost VandeVondele,
Alois Renn,
S. Götzinger,
Paola Ceroni,
Andri Schuetz,
Lay-Theng Lee, et al.
Label-free characterization of biomembranes: from structure to dynamics
Alireza Mashaghi,
Samaneh Mashaghi,
Ilya Reviakine,
Ron M. A. Heeren,
Vahid Sandoghdar,
Mischa Bonn
Chemical Society Reviews
43
887-900
(2014)
| Journal
We review recent progress in the study of the structure and dynamics of phospholipid membranes and associated proteins, using novel label-free analytical tools. We describe these techniques and illustrate them with examples highlighting current capabilities and limitations. Recent advances in applying such techniques to biological and model membranes for biophysical studies and biosensing applications are presented, and future prospects are discussed.
Analysis of parahydrogen polarized spin system in low magnetic fields
P. Tuerschmann,
J. Colell,
T. Theis,
B. Bluemich,
S. Appelt
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
16
(29)
15411-15421
(2014)
| Journal
Nuclear magnetic resonance (NMR) spectra of spin systems polarized either thermally or by parahydrogen exhibit strikingly different field dependencies. Thermally polarized spin systems show the well-known roof effect, observed when reducing magnetic field strengths which precludes the independent determination of chemical shift differences and J-coupling constants at low-fields. Quantum mechanical analysis of the NMR spectra with respect to polarization method, pulsed state preparation, and transition probabilities reveals that spectra of parahydrogen polarized systems feature an "inverse roof effect" in the regime where the chemical shift difference delta nu is smaller than J. This inverse roof effect allows for the extraction of both J-coupling and chemical shift information down to very low fields. Based on a two-spin system, the observed non-linear magnetic field dependence of the splitting of spectral lines is predicted. We develop a general solution for the steady state density matrix of a parahydrogen polarized three-spin system including a heteronucleus which allows explaining experimentally observed H-1 spectra. The analysis of three-spin density matrix illustrates two pathways for an efficient polarization transfer from parahydrogen to C-13 nuclei. Examination of the experimental data facilitates the extraction of all relevant NMR parameters using single-scan, high-resolution H-1 and C-13 NMR spectroscopy at low fields at a fraction of the cost associated with cryogenically cooled high-field NMR spectrometers.
Scanning-aperture trapping and manipulation of single charged
nanoparticles
Although trapping and manipulation of small objects have been of interest for a range of applications and many clever techniques have been devised, new methods are still in great demand for handling different materials and geometries. Here, we report on an electrostatic trap that is created in an aqueous medium between the aperture of a nanopipette and a glass substrate without the need for external potentials. After a thorough characterization of the trapping conditions, we show that we can displace or release a particle at will. Furthermore, we demonstrate trapping and manipulation of nanoparticles and lipid vesicles attached to lipid bilayers, paving the way for controlled studies of forces and diffusion associated with biological membranes. We expect the technique to find interesting applications also in other areas such as optonanofluidics and plasmonics.
Conformational distribution of surface-adsorbed fibronectin molecules
explored by single molecule localization microscopy
E. Klotzsch,
I. Schoen,
J. Ries,
A. Renn,
V. Sandoghdar,
V. Vogel
Adsorbed proteins that promote cell adhesion mediate the response of cells to biomaterials and scaffolds. As proteins undergo conformational changes upon surface adsorption, their functional display may be significantly affected by surface chemistry or solution conditions during the adsorption process. A high-resolution localization microscopy technique is extended here to probe the conformation of individual fibronectin (Fn) molecules at the glass-water interface under physiological buffer conditions. To map distances, four available cysteines located on the modules FnIII(7) and FnIII(15) of dimeric Fn were site-specifically labeled with Cy3B, and their relative positions were determined by stepwise photobleaching with nanometer precision. The four labels on single Fn molecules did not show a uniform or linear arrangement. The distances between label positions were distributed asymmetrically around 33 nm with a tail towards higher distances. Exposure of Fn to denaturing solution conditions during adsorption increased the average distances up to 43 nm for 4 M guanidinium HCl, while changing the solution conditions after the adsorption had no effect, indicating that the observed intra-molecular distances are locked-in during the adsorption process. Also surface coatings of different hydrophobicity altered the conformational distribution, shifting label distances from a median of 24 nm on hydrophilic to 49 nm on hydrophobic surfaces. These results further highlight that the conformation of macromolecules at interfaces depends on the adsorption history. While illustrated here for surface adsorbed Fn, the power of localization-based microscopy extends the repertoire of techniques to characterize biomolecules at interfaces.
Single-molecule optical spectroscopy
Michel Orrit,
Taekjip Ha,
Vahid Sandoghdar
Chemical Society Reviews
43
973-976
(2014)
| Journal
Spectroscopic detection and state preparation of a single praseodymium ion in a crystal
Tobias Utikal,
Emanuel Eichhammer,
L. Petersen,
Alois Renn,
Stephan Götzinger,
Vahid Sandoghdar
The narrow optical transitions and long spin coherence times of rare earth ions in crystals make them desirable for a number of applications ranging from solid-state spectroscopy and laser physics to quantum information processing. However, investigations of these features have not been possible at the single-ion level. Here we show that the combination of cryogenic high-resolution laser spectroscopy with optical microscopy allows one to spectrally select individual praseodymium ions in yttrium orthosilicate. Furthermore, this spectral selectivity makes it possible to resolve neighbouring ions with a spatial precision of the order of 10 nm. 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.
Contact
Nano-Optics Division Prof. Vahid Sandoghdar
Max Planck Institute for the Science of Light Staudtstr. 2 91058 Erlangen, Germany
