Laser scanning microscope for low temperature single molecule and microscale spectroscopy based on gradient index optics
08 Apr 1999-Review of Scientific Instruments (American Institute of Physics)-Vol. 70, Iss: 4, pp 2041-2045
TL;DR: In this article, a scanning optical microscope for low temperature imaging and spectroscopy with a gradient index rod-shaped microlens as an objective lens is presented, where the solid immersion effect enhances the resolution to 310 nm of the full width at half-maximum at the wavelength of 545 nm.
Abstract: A scanning optical microscope for low temperature imaging and spectroscopy with a gradient index rod-shaped microlens as an objective lens is presented. The solid immersion effect enhances the resolution to 310 nm of the full-width at half-maximum at the wavelength of 545 nm. Laser scanning mechanism located outside an optical cryostat enables to achieve large scanning ranges independent of temperature. The performance is demonstrated at 1.6 K on single molecules of terrylene in a dodecane crystal and on molecular J aggregates in thin polymer films.
Citations
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TL;DR: In this article, single-molecule spectroscopy (SMS) has been used for a variety of applications including molecular photophysics, quantum optics, and molecular dynamics.
Abstract: Single-molecule spectroscopy (SMS) combines some of the advantages of local probe microscopies with those of optics. Since this field came into being 10 years ago, it has expanded at a breathtaking pace. From the first cryogenic experiments up to the recent studies of basic processes in molecular biology, single-molecule methods have found their way into an ever broadening range of applications. Their common feature is the complete elimination of ensemble averaging. By exposing individual variations as well as dynamical fluctuations, SMS provides new insights into any system with spatial or temporal inhomogeneity. The present article illustrates single molecule spectroscopic experiments at cryogenic temperatures, mainly from the authors' group. The results reviewed here range from molecular photophysics, to the dynamics of the solid matrix around the molecule, and to the interactions between a single molecule and electromagnetic fields, i.e., quantum optics. SMS is now ripe for a variety of applications i...
315 citations
TL;DR: This review presents an overview of the common techniques for single-molecule fluorescence spectroscopy applied to photosynthetic systems and describes selected experiments that provide a new understanding of the impact of heterogeneity on light harvesting and thus how these systems are optimized to capture sunlight under physiological conditions.
Abstract: Photosynthesis begins when a network of pigment–protein complexes captures solar energy and transports it to the reaction center, where charge separation occurs. When necessary (under low light conditions), photosynthetic organisms perform this energy transport and charge separation with near unity quantum efficiency. Remarkably, this high efficiency is maintained under physiological conditions, which include thermal fluctuations of the pigment–protein complexes and changing local environments. These conditions introduce multiple types of heterogeneity in the pigment–protein complexes, including structural heterogeneity, energetic heterogeneity, and functional heterogeneity. Understanding how photosynthetic light-harvesting functions in the face of these fluctuations requires understanding this heterogeneity, which, in turn, requires characterization of individual pigment–protein complexes. Single-molecule spectroscopy has the power to probe individual complexes. In this review, we present an overview of ...
80 citations
TL;DR: In this paper, the capabilities of LSM as a spatially-resolved method of testing high-Tc superconductivity (HTS) materials and devices are described.
Abstract: The capabilities of laser scanning microscopy (LSM) as a spatially-resolved method of testing high-Tc superconductivity (HTS) materials and devices are described. The earlier results obtained by the authors are briefly reviewed. Some novel applications of LSM are illustrated, including imaging the HTS responses in rf mode, probing the superconducting properties of HTS single crystals, and development of two-beam laser scanning microscopy. The existence of the phase slip lines mechanism of resistivity in HTS materials is proven by LSM imaging.
60 citations
TL;DR: In this article, the capabilities of laser scanning microscopy (LSM) as a spatially resolved method of testing high-Tc materials and devices are described, and some novel applications of the LSM are illustrated, including imaging the HTS responses in rf mode, probing the superconducting properties of HTS single crystals.
Abstract: The work describes the capabilities of Laser Scanning Microscopy (LSM) as a spatially resolved method of testing high_Tc materials and devices. The earlier results obtained by the authors are briefly reviewed. Some novel applications of the LSM are illustrated, including imaging the HTS responses in rf mode, probing the superconducting properties of HTS single crystals, development of twobeam laser scanning microscopy. The existence of the phase slip lines mechanism of resistivity in HTS materials is proven by LSM imaging.
59 citations
TL;DR: In this article, the synthesis of semiconductor nanocrystals (CdSe) by pyrolysis of organometallic reagents and their optical properties are reported. But the authors do not specify the relative amount of precursors to be injected into the coordinating solvent, e.g. TOPO.
33 citations
References
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TL;DR: Individual carbocyanine dye molecules in a sub-monolayer spread have been imaged with near-field scanning optical microscopy and the orientation of each molecular dipole can be determined to map the electric field distribution in the near- field aperture with molecular spatial resolution.
Abstract: Individual carbocyanine dye molecules in a sub-monolayer spread have been imaged with near-field scanning optical microscopy. Molecules can be repeatedly detected and spatially localized (to ∼λ/50 where λ is the wavelength of light) with a sensitivity of at least 0.005 molecules/(Hz)1/2 and the orientation of each molecular dipole can be determined. This information is exploited to map the electric field distribution in the near-field aperture with molecular spatial resolution.
1,201 citations
TL;DR: Experiments clearly prove that narrow peaks in the fluorescence excitation spectrum of a pentacene-doped p-terphenyl crystal stem from single molecules, and show the feasibility of the optical study of a single molecule and its local environment.
Abstract: Experiments clearly prove that narrow peaks in the fluorescence-excitation spectrum of a pentacene-doped p-terphenyl crystal stem from single molecules. This claim is supported by the distribution, width, and height of the peaks, as well as by the correlation of the emitted light and the sudden drops and surges of the emission of certain peaks. We attribute these to the hole burning of a single molecule. These results show the feasibility of the optical study of a single molecule and its local environment.
973 citations
TL;DR: In this article, a real-time optical microscope was developed that operates on the same principle as a liquid immersion microscope, with the liquid replaced by a solid lens of high refractive index material.
Abstract: A new type of real‐time optical microscope has been developed that operates on the same principle as a liquid immersion microscope, with the liquid replaced by a solid lens of high refractive index material. Using a lens with an index n=2 and 436 nm illumination, this microscope has resolved 100 nm lines and spaces and has demonstrated a factor of two improvement in the edge response over a confocal microscope.
683 citations
TL;DR: Confocal fluorescence microscopy coupled with a diffraction-limited laser beam and a high-efficiency detection system has been used to study the diffusive movement and emission process of individual fluorescent molecules in the liquid phase at room temperature.
Abstract: Confocal fluorescence microscopy coupled with a diffraction-limited laser beam and a high-efficiency detection system has been used to study the diffusive movement and emission process of individual fluorescent molecules in the liquid phase at room temperature. The high detection sensitivity achieved at fast data acquisition speeds (greater than 1 kilohertz) allows real-time observation of single-molecule fluorescence without statistical analysis. The results show fluorescence-cycle saturation at the single-molecule level and multiple recrossings of a single molecule into and out of the probe volume as well as the triplet state.
576 citations