Optical detection and probing of single dopant molecules of pentacene in a p-terphenyl host crystal by means of absorption spectroscopy

Kador, Lothar; Horne, D. E.; Moerner, W. E.

doi:10.1021/j100367a011

Cited by 83 publications

(44 citation statements)

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“…The first SMS experiments in 1989 by Moerner and Kador utilized either of two powerful double-modulation FMS absorption techniques, laser FMS with Stark secondary modulation (FM-Stark) or FMS with ultrasonic strain secondary modulation (FM-US) 1, 37 . Secondary modulation was required in order to remove the effects of residual amplitude modulation produced by the imperfect phase modulator 38 .…”

Section: Introductionmentioning

confidence: 99%

Single-molecule spectroscopy and imaging over the decades

2015

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As of 2015, it has been 26 years since the first optical detection and spectroscopy of single molecules in condensed matter. This area of science has expanded far beyond the early low temperature studies in crystals to include single molecules in cells, polymers, and in solution. The early steps relied upon high-resolution spectroscopy of inhomogeneously broadened optical absorption profiles of molecular impurities in solids at low temperatures. Spectral fine structure arising directly from the position-dependent fluctuations of the number of molecules in resonance led to the attainment of the single-molecule limit in 1989 using frequency-modulation laser spectroscopy. In the early 1990's, a variety of fascinating physical effects were observed for individual molecules, including imaging of the light from single molecules as well as observations of spectral diffusion, optical switching and the ability to select different single molecules in the same focal volume simply by tuning the pumping laser frequency. In the room temperature regime, researchers showed that bursts of light from single molecules could be detected in solution, leading to imaging and microscopy by a variety of methods. Studies of single copies of the green fluorescent protein also uncovered surprises, especially the blinking and photoinduced recovery of emitters, which stimulated further development of photoswitchable fluorescent protein labels. All of these early steps provided important fundamentals underpinning the development of super-resolution microscopy based on single-molecule localization and active control of emitting concentration. Current thrust areas include extensions to three-dimensional imaging with high precision, orientational analysis of single molecules, and direct measurements of photodynamics and transport properties for single molecules trapped in solution by suppression of Brownian motion. Without question, a huge variety of studies of single molecules performed by many talented scientists all over the world have extended our knowledge of the nanoscale and microscopic mechanisms previously hidden by ensemble averaging.

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Section: Introductionmentioning

confidence: 99%

Single-molecule spectroscopy and imaging over the decades

2015

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“…The first SMS experiments in 1989 utilized either of two powerful double-modulation FMS absorption techniques, laser FMS with Stark secondary modulation (FM-Stark) or FMS with ultrasonic strain secondary modulation (FM-US) (1,32). Secondary modulation was required in order to remove the effects of residual amplitude modulation produced by the imperfect phase modulator (33).…”

Section: Figure 8 Herementioning

confidence: 99%

Nobel Lecture: Single-molecule spectroscopy, imaging, and photocontrol: Foundations for super-resolution microscopy

Moerner

2015

Rev. Mod. Phys.

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The initial steps toward optical detection and spectroscopy of single molecules in condensed matter arose out of the study of inhomogeneously broadened optical absorption profiles of molecular impurities in solids at low temperatures. Spectral signatures relating to the fluctuations of the number of molecules in resonance led to the attainment of the single-molecule limit in 1989 using frequency-modulation laser spectroscopy. In the early 90's, many fascinating physical effects were observed for individual molecules, and the imaging of single molecules as well as observations of spectral diffusion, optical switching and the ability to select different single molecules in the same focal volume simply by tuning the pumping laser frequency provided important forerunners of the later superresolution microscopy with single molecules. In the room temperature regime, imaging of single copies of the green fluorescent protein also uncovered surprises, especially the blinking and photoinduced recovery of emitters, which stimulated further development of photoswitchable fluorescent protein labels. Because each single fluorophore acts a light source roughly 1 nm in size, microscopic observation and localization of individual fluorophores is a key ingredient to imaging beyond the optical diffraction limit. Combining this with active control of the number of emitting molecules in the pumped volume led to the super-resolution imaging of Eric Betzig and others, a new frontier for optical microscopy beyond the diffraction limit. The background leading up to these observations is described and current developments are summarized. The early days Introduction and early inspirationsI want to thank the Nobel Committee for Chemistry, the Royal Swedish Academy of Sciences, and the Nobel Foundation for selecting me for this prize recognizing the development of super-resolved fluorescence microscopy. I am truly honored to share the prize with my two esteemed colleagues, Stefan Hell and Eric Betzig. My primary contributions center on the first optical detection and spectroscopy of single molecules in the condensed phase(1), and on the observations of imaging, blinking and photocontrol not only for single molecules at low temperatures in solids, but also for useful variants of the green fluorescent protein at room temperature (2). This lecture describes the context of the events leading up to these advances as well as a portion of the subsequent developments both around the world and in my laboratory.In the mid-1980's, I derived much early inspiration from amazing advances that were occurring around the world where single nanoscale quantum systems were detected and explored for both scientific and technological reasons. Some of these were (i) the spectroscopy of single electrons or ions confined in vacuum electromagnetic traps (3-5), (ii) scanning tunneling microscopy (STM) (6) and atomic force microscopy (AFM) (7), and (iii) the study of ion currents in single membrane-embedded ion channels (8). But why not optical detection and ...

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“…Moerner and M. Orrit [1,2]. This technique offers a unique opportunity to study at molecular scale physical, photophysical and even biological processes [3,4] and is a rapidly growing field.…”

Section: Introductionmentioning

confidence: 99%

Original Tools for Single-Molecule Spectroscopy

et al. 2001

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Characterizing individually nanoparticles or probing complex environments by single molecule can be a powerful approach provided that spectroscopic techniques, tailored to such systems, have been developed to extract pertinent physico-chemical parameters of interest. In the paper, we report on two techniques that were missing in SingleMolecule Spectroscopy (SMS) toolbox. The first concerns polarization. Due to molecule anisotropy, 3D-molecular orientation is a well-defined parameter. In principle, SMS can take advantage of this property to study 3D-orientation dynamics of the molecule or its environment anisotropy.Unfortunately, information from such measurements is largely reduced because molecules are not efficiently detected when their optical dipole is orientated close to the optical axis. We analyze theoretically this problem and demonstrate experimentally one of its solutions. The second tool is more fundamental. It is chemical analysis of single nanoobjects at room temperature, which is not possible when analyzing fluorescence. With the example of Single-Wall carbon NanoTubes (SWNTs), we show that enhanced Raman spectroscopy allows us to image tiny rope or single SWNTs. We also present preliminary results on enhanced Raman chemical imaging and chemical colocalization.

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Optical detection and probing of single dopant molecules of pentacene in a p-terphenyl host crystal by means of absorption spectroscopy

Cited by 83 publications

References 1 publication

Single-molecule spectroscopy and imaging over the decades

Single-molecule spectroscopy and imaging over the decades

Nobel Lecture: Single-molecule spectroscopy, imaging, and photocontrol: Foundations for super-resolution microscopy

Original Tools for Single-Molecule Spectroscopy

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