PubMed · 14860502
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G D LESKOV. 1951. [Luminescent microscopy].. https://pubmed.ncbi.nlm.nih.gov/14860502/
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High-throughput screening (HTS) of chemical libraries is indispensable for drug discovery research. However, the HTS data quality for lead discovery, lead optimization, and quantitative structure activity relationship studies has been severely compromised due to the uncertain compound concentrations in screening plates. In order to address this issue, we compared various high-throughput technologies for quantification of compounds in microtiter plate format without the need for authentic compounds as standards and identified the chemiluminescence nitrogen detector (CLND) as the method of choice at the present time. However, the structure dependence of this detector has not been well studied. A proposed rule suggested that the only exception to equimolar response is for compounds that contain adjacent nitrogen atoms. The response should be zero when the adjacent nitrogen atoms are connected by a double bond and 0.5 when they are connected by a single bond. In this investigation, we studied a broad range of compounds with isolated and adjacent nitrogen atoms. We confirmed that compounds with isolated nitrogen atoms produce an equimolar response with a 15-20% variation depending on structures and compounds with adjacent nitrogen atoms connected by a double bond giving nearly zero response. We discovered that the CLND response for compounds containing adjacent nitrogen atoms that are connected with a single bond is highly structure dependent. Substitutions on the nitrogen atoms or nearby in the molecule can increase the CLND response to approach a value higher than the predicted value 0.5 (maximal value 0.82/nitrogen atom). Without substitution, much lower values than predicted (minimal value 0.0-0.08/nitrogen atom) are obtained. Therefore, the prediction of response of 0.5/nitrogen atom for compounds with adjacent nitrogen atoms connected by a single bond should be abandoned. Compounds with similar structures should be used to generate calibration curves for quantification of this class of compounds.
Because of the strong spatial confinement of electronic wave functions and reduced dielectric screening, the effects of carrier-carrier Coulomb interactions are greatly enhanced in semiconductor nanocrystals (NCs) compared with those in bulk materials. These interactions open a highly efficient decay channel via Auger recombination, which represents a dominant recombination pathway for multiexcitons in NCs. Furthermore, strong Coulomb coupling between charge carriers leads to extremely efficient direct photogeneration of multiexcitons by single photons via carrier (or exciton) multiplication. This review focuses on spectral and dynamical properties of multiexcitons in semiconductor NCs. The specific topics discussed here include the structure of NC electronic states, spectral signatures of multiexcitons in transient absorption and photoluminescence, exciton-exciton interaction energies, Auger recombination, and carrier multiplication. This chapter also briefly reviews the implications of multiexciton effects for practical technologies, such as NC lasing and photovoltaics.
The purpose of this work is to address the issue of applicability of single-molecule spectroscopy (SMS) results for conjugated polymers to "bulk" samples, e.g. conjugated polymer films. Also, some apparent inconsistencies in the literature on SMS regarding the photoluminescence spectral position of conjugated polymers are discussed. We present a series of photoluminescence spectra of thin films of the conjugated polymer poly(2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene-vinylene) (MEH-PPV) with a wide range of varying thickness. The thickness was varied from approximately 20 nm to the value corresponding to well-separated single molecules (SMS sample). The thickness variation resulted in a strong ( approximately 2000 cm(-1)) blue-shift and broadening of the spectrum. The result was reproduced on isolated molecules embedded into a PMMA matrix. This effect cannot be explained by a decrease in energy transfer "freedom" alone. We performed a comprehensive comparison of presented and elsewhere published spectra of MEH-PPV polymer and oligomers in different samples: films, solutions, isolated-molecule coatings and standard SMS samples. The comparison allows that the main reason behind the blue shift is conformational disorder, which is largely dependent on the sample. We also discuss some experimental aspects of SMS, such as representativeness of detected molecules, spectral sensitivity of a setup and temperature. Together with differences in sample preparation method, these issues can explain the existing inconsistencies in the literature.