Measuring the Number of Independent Emitters in Single-Molecule Fluorescence Images and Trajectories Using Coincident Photons

Weston, Kenneth D.; Dyck, Martina; Tinnefeld, Philip; Müller, Christian; Herten, Dirk‐Peter; Sauer, Markus

doi:10.1021/ac025730z

Cited by 127 publications

(198 citation statements)

References 38 publications

(59 reference statements)

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“…20 Generally, the photon statistics of conjugated polymers can be used to estimate the number of independently emitting chromophores under the assumption that the chromophores exhibit the same brightness. 21,22 Intuitively, one would expect that the number of independently emitting chromophores simply decreases during a PL quenching event and that the photon statistics therefore change towards a more non-classical distribution (i.e. improved photon antibunching).…”

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confidence: 99%

Impact of charge carrier injection on single-chain photophysics of conjugated polymers

Hofmann

Vogelsang

Lupton

2016

Applied Physics Letters

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Charges in conjugated polymer materials have a strong impact on the photophysics and their interaction with the primary excited state species has to be taken into account in understanding device properties. Here, we employ single-molecule spectroscopy to unravel the influence of charges on several photoluminescence (PL) observables. The charges are injected either stochastically by a photochemical process, or deterministically in a hole-injection sandwich device configuration. We find that upon charge injection, besides a blue-shift of the PL emission and a shortening of the PL lifetime due to quenching and blocking of the lowest-energy chromophores, the non-classical photon arrival time distribution of the multichromophoric chain is modified towards a more classical distribution. Surprisingly, the fidelity of photon antibunching deteriorates upon charging, whereas one would actually expect the number of chromophores to be reduced. A qualitative model is presented to explain the observed PL changes. The results are of interest to developing a microscopic understanding of the intrinsic charge-exciton quenching interaction in devices.

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confidence: 99%

Impact of charge carrier injection on single-chain photophysics of conjugated polymers

Hofmann

Vogelsang

Lupton

2016

Applied Physics Letters

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“…24,25 With pulsed excitation, a peak at zero delay time of the crosscorrelation function G (2) (τ) of the recorded luminescence signal is absent only for a single emitter. 23,26,27 This strong antibunching is a clear indication of the fact that, due to its finite excited state lifetime, a single emitter such as a single isolated NV center cannot emit two photons at the same time.…”

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confidence: 99%

Three-Dimensional Stimulated Emission Depletion Microscopy of Nitrogen-Vacancy Centers in Diamond Using Continuous-Wave Light

et al. 2009

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Charged nitrogen-vacancy (NV) color centers in diamond are excellent luminescence sources for far-field fluorescence nanoscopy by stimulated emission depletion (STED).Here we show that these photostable color centers can be visualized by STED using simple continuous-wave or high repetition pulsed lasers (76 MHz) at wavelengths >700 nm for STED. Furthermore, we show that NV centers can be imaged in three dimensions (3D) inside the diamond crystal and present single-photon signatures of single color centers recorded in high density samples, demonstrating a new recording scheme for STED and related far-field nanoscopy approaches. Finally, we exemplify the potential of using nanodiamonds containing NV centers as luminescence tags in STED microscopy. Our results offer new experimental avenues in nanooptics, nanotechnology, and the life sciences.Far-field fluorescence microscopy is one of the most important tools for noninvasive imaging of the interior of transparent objects. However, the resolution of its standard versions is limited by diffraction which precludes discerning similar features that are closer together than about half the wavelength λ of the light used, i.e., about 200 nm. 1 Stimulated emission depletion (STED) microscopy 2,3 has fundamentally overcome the limits set by diffraction by transiently switching off the fluorescence ability of the dye by stimulated emission, so as to allow neighboring features to be registered sequentially in time by scanning. With standard fluorophores, STED microscopy routinely offers a spatial resolution in the 20-50 nm range and has successfully been applied to approaching key problems in biology. 4,5 However, in some applications, STED microscopy is challenged by the limited photostability of the fluorescent markers, which reduces fluorescence brightness and prevents long-term observations. A solution is to employ fluorescent probes with less-photobleaching like luminescent semiconductor quantum dot (QD) nanocrystals 6,7 or nitrogen-vacancy (NV) color centers in diamonds. 8,9 Unfortunately, the fact that the absorption band of most QDs overlaps with that for their emission has hampered their applicability to STED microscopy. In contrast, NV centers in diamond have recently turned out as excellent luminescence sources in STED microscopy, with no observable photobleaching.10 Initial STED microscopy images of NV centers in diamond featured an up to 6 nm spatial resolution in the focal plane (x,y). However, they were recorded inside bulk diamond, with a fixed wavelength of 775 nm for STED and with a rather low (8 MHz) repetition pulsed laser system. While the low repetition rate may be highly favorable for obtaining the maximum possible resolution with NV centers, it also entails long image acquisition times preventing their application as fluorescent tags in the life sciences and elsewhere. Here, we show that STED nanoscopy on NV centers is viable with tunable continuous-wave (CW) or quasi-CW high-repetitive 76 MHz pulsed laser sources and that it discerns individu...

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“…At the single-molecule level, the EET efficiencies of individual cyclic porphyrin arrays were examined by carrying out coincidence measurement [17,18]. This measurement allows for the observation of singlet-singlet annihilation processes occurring in a single molecule (figure 6a) [26,27].…”

Section: Phil Trans R Soc a (2012)mentioning

confidence: 99%

Excitation energy migration processes in various multi-porphyrin assemblies

Yang

Kim

2012

Phil. Trans. R. Soc. A.

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The electronic interactions and excitation energy transfer (EET) processes of a variety of multi-porphyrin arrays with linear, cyclic and box architectures have been explored. Directly meso-meso linked linear arrays (Z N ) exhibit strong excitonic coupling with an exciton coherence length of approximately 6 porphyrin units, while fused linear arrays (T N ) exhibit extensive p-conjugation over the whole array. The excitonic coherence length in directly linked cyclic porphyrin rings (CZ N ) was determined to be approximately 2.7 porphyrin units by simultaneous analysis of fluorescence intensities and lifetimes at the single-molecule level. By performing transient absorption (TA) and TA anisotropy decay measurements, the EET rates in m-phenylene linked cyclic porphyrin wheels C12ZA and C24ZB were determined to be 4 and 36 ps −1 , respectively. With increasing the size of C N ZA, the EET efficiencies decrease owing to the structural distortions that produce considerable non-radiative decay pathways. Finally, the EET rates of self-assembled porphyrin boxes consisting of directly linked diporphyrins, B1A, B2A and B3A, are 48, 98 and 361 ps −1 , respectively. The EET rates of porphyrin boxes consisting of alkynylenebridged diporphyrins, B2B and B4B, depend on the conformation of building blocks (planar or orthogonal) rather than the length of alkynylene linkers.

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Measuring the Number of Independent Emitters in Single-Molecule Fluorescence Images and Trajectories Using Coincident Photons

Cited by 127 publications

References 38 publications

Impact of charge carrier injection on single-chain photophysics of conjugated polymers

Impact of charge carrier injection on single-chain photophysics of conjugated polymers

Three-Dimensional Stimulated Emission Depletion Microscopy of Nitrogen-Vacancy Centers in Diamond Using Continuous-Wave Light

Excitation energy migration processes in various multi-porphyrin assemblies

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