Single-molecule orientations determined by direct emission pattern imaging

Lieb, M.; Zavislan, James M.; Novotny, Lukas

doi:10.1364/josab.21.001210

Cited by 398 publications

(414 citation statements)

References 26 publications

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“…The highly directional (doughnut like) emission stems from the fact that the terrylene dipole is oriented nearly perpendicular to the substrate plane [11]. As has been shown very recently [12], by analyzing this image we can determine the tilt angle θ of the dipole. From the cross section in Fig.…”

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confidence: 87%

Measuring the Quantum Efficiency of the Optical Emission of Single Radiating Dipoles Using a Scanning Mirror

et al. 2005

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Using scanning probe techniques, we show the controlled manipulation of the radiation from single dipoles. In one experiment we study the modification of the fluorescence lifetime of a single molecular dipole in front of a movable silver mirror. A second experiment demonstrates the changing plasmon spectrum of a gold nanoparticle in front of a dielectric mirror. Comparison of our data with theoretical models allows determination of the quantum efficiency of each radiating dipole.It is a well established matter that the radiation of an oscillating electric dipole can be manipulated if it is placed in front of a planar interface [1]. Experiments investigating this system date back to Drexhage [2] who looked at the influence of a metallic mirror on the fluorescence lifetime of ensembles of Eu 3+ ions. By preparing a large number of samples, each with a different spacing between the mirror and the emitter layer, two major effects were observed. Firstly, it was shown that the decay rate (Γ) oscillates at large distances due to the retarded interaction of the dipoles with their own reflected fields. Secondly, it was shown that Γ is strongly modified very close to the mirror due to the energy transfer to the metal [1,2]. Since that time, numerous works have investigated the modification of spontaneous emission from ensembles in thin dielectric layers [1]. Various key parameters such as the dipole's orientation, its distance to the interface and its quantum efficiency are, however, averaged in ensemble measurements.Due to challenges such as detection sensitivity, photostability and position control, experiments with single emitters have been scarce. Some researchers have nevertheless shown effects of the local dielectric environment by adding an index matching fluid to eliminate an interface [3,4] or by introducing the subwavelength boundary of a sharp tip [5,6]. In this work we study the fluorescence lifetime and intensity of a single molecule at a well-defined orientation and position, while moving an external silver mirror in its vicinity. We also examine the plasmon spectrum of a well-characterized single gold nanoparticle at various locations in front of a dielectric mirror. These experiments allow us to demonstrate, for the first time, both the far-field modulation and the nearfield modification of the total decay rate (Γ) for individual dipoles. Since the far-field modulations are only due to changes in the radiative decay rate (Γ r ) we can determine the quantum efficiency η = Γ r /Γ of each dipole.A theoretical description of dipole decay in multi-layer structures was first developed by Chance et al. [7] and has been expanded by many authors to cover numerous * Present address:FOM-Institute for Atomic and Molecular Physics (AMOLF), 1098 SJ Amsterdam, The Netherlands † Present address:Niels Bohr Institute, 2100 Copenhagen, Denmark ‡ Electronic address: vahid.sandoghdar@ethz.ch situations. In particular, Sullivan and Hall [8] present an elegant plane wave solution that can easily be adapted to our system. For a s...

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confidence: 87%

Measuring the Quantum Efficiency of the Optical Emission of Single Radiating Dipoles Using a Scanning Mirror

et al. 2005

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“…The angular distribution of the emission light intensity can be characterized by two spherical angles, θ and φ (Figure 3 A) and can be directly imaged on the back focal plane of the objective [38] . The details about Fourier imaging can be found in the paper by Lieb et al [39] . Fourier imaging has become a useful technique to study the directional properties in research of plasmonics [40 -42] .…”

Section: Direction and Polarization Of Emitted Lightmentioning

confidence: 99%

Nanowire-based plasmonic waveguides and devices for integrated nanophotonic circuits

Wei

2012

Nanophotonics

120

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The fast development of plasmonics have greatly advanced our understanding to the abundant phenomena related to surface plamon polaritons (SPPs) and improved our ability to manipulate light at the nanometer scale. With tightly confi ned local fi eld, SPPs can be transmitted in waveguides of subwavelength dimensions. Nanophotonic circuits built with plasmonic elements can be scaled down to dimensions compatible with semiconductor-based nanoelectronic circuits, which provides a potential solution for the next-generation information technology. Different structures have been explored as plasmonic waveguides for potential integration applications. This review is focused on metallic nanowire waveguides and functional components in nanowire networks. We reviewed recent progress in research about plasmon generation, emission direction and polarization, group velocity, loss and propagation length, and the near-fi eld distribution revealed by quantum dot fl uorescence imaging. Electrical generation and detection of SPPs moves towards the building of plasmonic circuits, where bulky external light sources and detectors may be omitted. The coupling between metal nanowires and emitters is important for tailoring light-matter interactions, and for various potential applications. In multi-nanowire structures, plasmon signal control and processing are introduced. The working principles of these nanowire-based devices, which are based on the control to the near fi eld distributions, will become the design rule for nanophotonic circuits with higher complexity for optical signal processing. The recent developments in hybrid photonic-plasmonic waveguides and devices are promising for making devices with unprecedented performance.

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“…Approaches have been developed that rely on excitation and/or emission with multiple polarizations (19,20), introduction of defocus and pattern matching (21), direct imaging of pupil functions (22), and use of annular illumination to create characteristic field distributions (23) to name a few. The alternating measurement of 2D position and orientation has also been addressed (24).…”

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confidence: 99%

“…2A). Qualitatively, this asymmetry is introduced because the asymmetric pupil functions of SM dipoles (22) are multiplied by the DH-PSF phase mask, causing various spatial frequencies of the ordinary DH-PSF to be attenuated as a function of orientation and defocus. We quantify the lobe asymmetry as…”

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confidence: 99%

Simultaneous, accurate measurement of the 3D position and orientation of single molecules

Backlund¹,

Lew²,

Backer

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

190

214

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Recently, single molecule-based superresolution fluorescence microscopy has surpassed the diffraction limit to improve resolution to the order of 20 nm or better. These methods typically use image fitting that assumes an isotropic emission pattern from the single emitters as well as control of the emitter concentration. However, anisotropic single-molecule emission patterns arise from the transition dipole when it is rotationally immobile, depending highly on the molecule's 3D orientation and z position. Failure to account for this fact can lead to significant lateral (x, y) mislocalizations (up to ∼50-200 nm). This systematic error can cause distortions in the reconstructed images, which can translate into degraded resolution. Using parameters uniquely inherent in the double-lobed nature of the Double-Helix Point Spread Function, we account for such mislocalizations and simultaneously measure 3D molecular orientation and 3D position. Mislocalizations during an axial scan of a single molecule manifest themselves as an apparent lateral shift in its position, which causes the standard deviation (SD) of its lateral position to appear larger than the SD expected from photon shot noise. By correcting each localization based on an estimated orientation, we are able to improve SDs in lateral localization from ∼2× worse than photon-limited precision (48 vs. 25 nm) to within 5 nm of photon-limited precision. Furthermore, by averaging many estimations of orientation over different depths, we are able to improve from a lateral SD of 116 (∼4× worse than the photonlimited precision; 28 nm) to 34 nm (within 6 nm of the photon limit).

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Single-molecule orientations determined by direct emission pattern imaging

Cited by 398 publications

References 26 publications

Measuring the Quantum Efficiency of the Optical Emission of Single Radiating Dipoles Using a Scanning Mirror

Measuring the Quantum Efficiency of the Optical Emission of Single Radiating Dipoles Using a Scanning Mirror

Nanowire-based plasmonic waveguides and devices for integrated nanophotonic circuits

Simultaneous, accurate measurement of the 3D position and orientation of single molecules

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