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Principles Of Fluorescence Spectroscopy

Noble metal nanoparticles are capable of confining resonant photons in such a manner as to induce coherent surface plasmon oscillation of their conduction band electrons, a phenomenon leading to two important properties. Firstly, the confinement of the photon to the nanoparticle's dimensions leads to a large increase in its electromagnetic field and consequently great enhancement of all the nanoparticle's radiative properties, such as absorption and scattering. Moreover, by confining the photon's wavelength to the nanoparticle's small dimensions, there exists enhanced imaging resolving powers, which extend well below the diffraction limit, a property of considerable importance in potential device applications. Secondly, the strongly absorbed light by the nanoparticles is followed by a rapid dephasing of the coherent electron motion in tandem with an equally rapid energy transfer to the lattice, a process integral to the technologically relevant photothermal properties of plasmonic nanoparticles. Of all the possible nanoparticle shapes, gold nanorods are especially intriguing as they offer strong plasmonic fields while exhibiting excellent tunability and biocompatibility. We begin this review of gold nanorods by summarizing their radiative and nonradiative properties. Their various synthetic methods are then outlined with an emphasis on the seed-mediated chemical growth. In particular, we describe nanorod spontaneous self-assembly, chemically driven assembly, and polymer-based alignment. The final section details current studies aimed at applications in the biological and biomedical fields.

Gold Nanorods: From Synthesis and Properties to Biological and Biomedical Applications

Organic materials that exhibit thermally activated delayed fluorescence (TADF) are an attractive class of functional materials that have witnessed a booming development in recent years. Since Adachi et al. reported high-performance TADF-OLED devices in 2012, there have been many reports regarding the design and synthesis of new TADF luminogens, which have various molecular structures and are used for different applications. In this review, we summarize and discuss the latest progress concerning this rapidly developing research field, in which the majority of the reported TADF systems are discussed, along with their derived structure–property relationships, TADF mechanisms and applications. We hope that such a review provides a clear outlook of these novel functional materials for a broad range of scientists within different disciplinary areas and attracts more researchers to devote themselves to this interesting research field.

Recent advances in organic thermally activated delayed fluorescence materials.

Optical Studies of Dynamics in Noble Metal Nanostructures

Ultrafast two-dimensional infrared (2D-IR) vibrational echo spectroscopy can probe structural dynamics under thermal equilibrium conditions on time scales ranging from femtoseconds to approximately 100 ps and longer. One of the important uses of 2D-IR spectroscopy is to monitor the dynamical evolution of a molecular system by reporting the time dependent frequency fluctuations of an ensemble of vibrational probes. The vibrational frequency-frequency correlation function (FFCF) is the connection between the experimental observables and the microscopic molecular dynamics and is thus the central object of interest in studying dynamics with 2D-IR vibrational echo spectroscopy. A new observable is presented that greatly simplifies the extraction of the FFCF from experimental data. The observable is the inverse of the center line slope (CLS) of the 2D spectrum. The CLS is the inverse of the slope of the line that connects the maxima of the peaks of a series of cuts through the 2D spectrum that are parallel to the frequency axis associated with the first electric field-matter interaction. The CLS varies from a maximum of 1 to 0 as spectral diffusion proceeds. It is shown analytically to second order in time that the CLS is the T(w) (time between pulses 2 and 3) dependent part of the FFCF. The procedure to extract the FFCF from the CLS is described, and it is shown that the T(w) independent homogeneous contribution to the FFCF can also be recovered to yield the full FFCF. The method is demonstrated by extracting FFCFs from families of calculated 2D-IR spectra and the linear absorption spectra produced from known FFCFs. Sources and magnitudes of errors in the procedure are quantified, and it is shown that in most circumstances, they are negligible. It is also demonstrated that the CLS is essentially unaffected by Fourier filtering methods (apodization), which can significantly increase the efficiency of data acquisition and spectral resolution, when the apodization is applied along the axis used for obtaining the CLS and is symmetrical about tau=0. The CLS is also unchanged by finite pulse durations that broaden 2D spectra.

Frequency-frequency correlation functions and apodization in two-dimensional infrared vibrational echo spectroscopy: A new approach

hydrogen bond dynamics in aqueous solutions (20) and other hydrogen-bonded liquids (21). Water molecules around monatomic ions provide the simplest system for the investigation of the dynamics of water in the presence of charges. Therefore, examining the dynamics of water in simple ionic solutions, such as sodium bromide (NaBr), can provide valuable insights that will increase understanding of chemical processes and biological systems that involve charged species in aqueous solutions. In pure water, water molecules are hydrogen-bonded to neighboring water molecules in a more or less tetrahedral geometry making an extended hydrogen bond network. Hydrogen bonds are continually breaking and reforming, and hydrogen bond lengths (strengths) are continually changing (9). The structure of water fluctuates on femtosecond to picosecond time scales (6, 9). The slowest component of the fluctuations is associated with the global structural rearrangement of the hydrogen bond network (7). As salt is dissolved in water, water molecules form hydration shells around ions, and consequently the local hydrogen bond network is perturbed. In this paper, a very detailed study of the hydrogen bond dynamics of water in highly concentrated NaBr solutions is presented. Four experimental observables, which are based on measurements on the OD stretch mode of HOD in H2O, were used. Ultrafast 2D IR vibrational echo experiments were used to measure spectral diffusion, which is directly related to the time evolution of the hydrogen bond structure. Polarization-selective IR pump–probe experiments were used to measure orientational relaxation dynamics of water, which is affected by the interactions of water molecules with their surroundings. The IR pump–

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Hydrogen bond dynamics in aqueous NaBr solutions

Ultrafast two dimensional infrared (2D-IR) vibra- tional echo spectroscopy has emerged as a powerful method for the study of molecular dynamics under thermal equilibrium con- ditions occurring on ultrafast time scales. Here, we describe ex- perimental details of 2D-IR vibrational echo spectroscopy in- cluding the experimental setup, pulse sequence, heterodyne de- tection, and extraction of the mainly absorptive part of the 2D- IR spectrum. As an experimental example, the measurements of the hydrogen bond dynamics of neat water and water in a high concentration of NaBr solution are presented and compared. The experiments are performed on OD stretching vibration of dilute HOD in H2O to eliminate contributions from vibrational exci- tation transport. A new experimental observable for extracting dynamical information that yields the frequency-frequency cor- relation function is presented. The observable is the inverse of the center line slope (CLS) of the 2D spectrum, which varies from a maximum of 1 to 0 as spectral diffusion proceeds. The CLS is the inverse of the slope of the line that connects the maxima of the peaks of a series of cuts through the 2D spectrum that are parallel to the frequency axis associated with the first radiation field-matter interaction. Comparisons of the dynamics obtained from the data on water and the concentrated NaBr solutions show that the hydrogen bond dynamics of water around ions are much slower than in bulk water.

/pdf/ultrafast-2d-ir-vibrational-echo-spectroscopy-a-probe-of-42u9chjl7w.pdf

Ultrafast 2D-IR vibrational echo spectroscopy: A probe of molecular dynamics

A novel strategy for designing highly efficient and activatable photosensitizers that can effectively generate reactive oxygen species (ROS) under both normoxia and hypoxia is proposed. Replacing both oxygen atoms in conventional naphthalimides (RNI-O) with sulfur atoms led to dramatic changes in the photophysical properties. The remarkable fluorescence quenching (ΦPL ≈ 0) of the resulting thionaphthalimides (RNI-S) suggested that the intersystem crossing from the singlet excited state to the reactive triplet state was enhanced by the sulfur substitution. Surprisingly, the singlet oxygen quantum yield of RNI-S gradually increased with increasing electron-donating ability of the 4-R substituents (MANI-S, ΦΔ ≈ 1.00, in air-saturated acetonitrile). Theoretical studies revealed that small singlet-triplet energy gaps and large spin-orbit coupling could be responsible for the efficient population of the triplet state of RNI-S. In particular, the ROS generation ability of MANI-S was suppressed under physiological conditions due to their self-assembly and was significantly recovered in cancer cells. More importantly, cellular experiments showed that MANI-S still produced a considerable amount of ROS even under severely hypoxic conditions (1% O2) through a type-I mechanism.

An Emerging Molecular Design Approach to Heavy-Atom-Free Photosensitizers for Enhanced Photodynamic Therapy under Hypoxia

Hydrogen bond dynamics of water in highly concentrated NaBr salt solutions and reverse micelles are studied using ultrafast 2D-IR vibrational echo spectroscopy and polarization-selective IR pump−probe experiments performed on the OD hydroxyl stretch of dilute HOD in H2O. The vibrational echo experiments measure spectral diffusion, and the pump−probe experiments measure orientational relaxation. Both experimental observables are directly related to the structural dynamics of water's hydrogen bond network. The measurements performed on NaBr solutions as a function of concentration show that the hydrogen bond dynamics slow as the NaBr concentration increases. The most pronounced change is in the longest time scale dynamics which are related to the global rearrangement of the hydrogen bond structure. Complete hydrogen bond network randomization slows by a factor of ∼3 in ∼6 M NaBr solution compared to that in bulk water. The hydrogen bond dynamics of water in nanoscopically confined environments are studied b...

Sungnam Park

Papers

Frequency-frequency correlation functions and apodization in two-dimensional infrared vibrational echo spectroscopy: A new approach

Hydrogen bond dynamics in aqueous NaBr solutions

Ultrafast 2D-IR vibrational echo spectroscopy: A probe of molecular dynamics

An Emerging Molecular Design Approach to Heavy-Atom-Free Photosensitizers for Enhanced Photodynamic Therapy under Hypoxia

Water dynamics--the effects of ions and nanoconfinement.