Electrical control of Förster energy transfer

Bringing together compounds of intrinsically different functionality, such as inorganic nanostructures and organic molecules, constitutes a particularly powerful route to creating novel functional devices with synergetic properties found in neither of the constituents. We introduce nanophotonic functional elements combining two classes of materials, semiconductor nanocrystals and dyes, whose physical nature arises as a superposition of the properties of the individual components. The strongly absorbing rod-like nanocrystals focus the incident radiation by photopumping the weakly absorbing dye via energy transfer. The CdSe/CdS nanorods exhibit a large quantum-confined Stark effect on the single-particle level, which enables direct control of the spectral resonance between donor and acceptor required for nanoscopic F?rster-type energy transfer in single nanorod-dye couples. With this far-field manipulation of a near-field phenomenon, the emission from single dye molecules can be controlled electrically. We propose that this effect could lead to the design of single-molecule optoelectronic switches providing building blocks for more complex nanophotonic circuitry.     

A single-molecule Förster resonance energy transfer analysis of fluorescent DNA-protein conjugates for nanobiotechnology

The development of nanobiotechnological devices requires the ability to build various components with nanometer accuracy. DNA is a well-established nanoscale building block that self assembles due to specific interactions that are encoded in its sequence. Recently, it has become possible to couple proteins to DNA, thereby expanding the capabilities of DNA for use with molecular photonics and bioelectronics. Here, we present the design and characterization of a supramolecular F?rster resonance energy transfer (FRET) system by using a fluorescent protein bound to single-stranded DNA (ssDNA), a fluorophore attached to a second ssDNA molecule, and a complementary strand for hybridizing the two fluorophores together. The FRET efficiency was studied by using both ensemble and single-pair FRET measurements. The distance between the two fluorophores was determined from the single-pair FRET efficiency and could be described by a simple cylindrical model for the DNA. Hence, DNA can be used as a scaffold for positioning fluorescent proteins, as well as traditional fluorophores, with nanometer accuracy and shows great potential for use in the future of nanobiotechnology.     

Bioconjugated superstructures of CdTe nanowires and nanoparticles: multistep cascade Förster resonance energy transfer and energy channeling

Nanoparticle/nanowire assemblies with a degree of radial organization were prepared around luminescent semiconducting CdTe nanowires using bioconjugation with streptavidin and D-biotin linkers. Red-emitting nanowires (6.62 +/- 1.55 nm diameter, 512 +/- 119 nm length) and green-emitting nanoparticles (3.2 +/- 0.7 nm diameter) were surface-modified with biotin, while orange-emitting nanoparticles (4.1 +/- 1.2 nm diameter) were decorated with streptavidin. CdTe nanocrystals produced two fuzzy layers around the nanowires in which the diameter of CdTe nanoparticles decreased with the distance from the nanowire axis. F?rster resonance energy transfer (FRET) from the outside layer of nanoparticles to the central nanowire was observed for nanowires conjugated with 4.1 nm CdTe. Addition of 3.2 nm CdTe resulted in a red-orange-green optical progression with band gaps of CdTe decreasing toward the axis of the superstructure. In this case, 4-fold luminescence enhancement of the nanowire luminescence was observed and was attributed to multistep FRET. This observation indicated the accumulation of photogenerated excitons in the cascade terminal. A simple model of multiconjugated superstructure with cascade energy transfer is developed and used to describe and understand the experimental data. The experimental data and theoretical model suggest the possibility of utilization of the prepared superstructures with radial symmetry in several classes of optoelectronic devices including nanomaterials for energy collection. They can also be a convenient model object for the investigation of methods of energy funneling in nanoscale assemblies.     

Förster resonance energy transfer-based biosensors for multiparameter ratiometric imaging of Ca2+ dynamics and caspase-3 activity in single cells

As one of the principal cytoplasmic second messengers, the calcium ion (Ca(2+)) is central to a variety of intracellular signal transduction pathways. Accordingly, there is a sustained interest in methods for spatially- and temporally resolved imaging of the concentration of Ca(2+) in live cells using noninvasive methods such as genetically encoded biosensors based on F?rster resonance energy transfer (FRET) between fluorescent proteins (FPs). In recent years, protein-engineering efforts have provided the research community with FRET-based Ca(2+) biosensors that are dramatically improved in terms of enhanced emission ratio change and optimized Ca(2+) affinity for various applications. We now report the development and systematic optimization of a pair of spectrally distinct FRET-based biosensors that enable the simultaneous imaging of Ca(2+) in two compartments of a single cell without substantial spectral crosstalk between emission channels. Furthermore, we demonstrate that these new biosensors can be used in conjunction with previously reported caspase-3 substrates based on the same set of FRET pairs.     

Förster-like nonexponential energy transfer kinetics in doped nanoparticles

Computer simulation of the static donor–acceptor energy transfer in samples containing impurity-doped nanoparticles of identical size and in a bulk crystal was performed, compared, and analyzed. A new double nonexponential decay law for nanoparticles was found and explained by two stages of quenching – that of bulk donors and donors on the surface.     

Enhanced light harvesting from Först-type resonance energy transfer in the quasi-solid state dye-sensitized solar cells

The demonstrated F?rst-type resonance energy transfer (FRET) is demonstrated in quasi-solid type dye-sensitized solar cells between organic fluorescence materials as an energy donor doped in polymeric gel electrolyte and a ruthenium complex as an energy acceptor on the surface of TiO2. Strong spectral overlap of emission/absorption of the energy donor and acceptor is required to obtain high FRET efficiency. The judicious choice of the energy donor allows the enhancement of the light harvesting characters of the energy acceptor (N3) in quasi-solid dye sensitized solar cells which increases the power conversion efficiency by 25% compare to that of a pristine cell. The optimized cell architecture fabricated with the quasi-solid type electrolyte containing fluorescence materials shows a maximum efficiency of 5.08% with a short-circuit current density (J(sc)) of 12.63 mA/cm2, and an open-circuit voltage (V(oc)) of 0.70 V under illumination of simulated solar light (AM 1.5, 100 mW/cm2).     

Mn²+-bonded reduced graphene oxide with strong radiative recombination in broad visible range caused by resonant energy transfer

The photoluminescence (PL) characteristics of Mn(2+)-bonded reduced graphene oxide (rGO) are studied in details. The Mn(2+)-bonded rGO is synthesized using MnO(2)-decorated GO as the intermediate products and ideal tunable PL is obtained by enhancing the long-wavelength (450-550 nm) emission. The PL spectra excited by different wavelengths are analyzed to elucidate the mechanism, and the resonant energy transfer between Mn(2+) and sp(2) clusters of the rGO appears to be responsible for the enhanced long-wavelength emission. To examine the effect of Mn(2+) on the long-wavelength emission from the Mn(2+)-bonded rGO, the PL characteristics of Mn(2+)-bonded rGO with smaller Mn concentrations are studied and weaker emission is observed. Our theoretical calculation corroborates the experimental results.     

Visualizing resonance energy transfer in supramolecular surface patterns of β-CD-functionalized quantum dot hosts and organic dye guests by fluorescence lifetime imaging

Detection of an analyte via supramolecular host-guest binding and quantum dot (QD)-based fluorescence resonance energy transfer (FRET) signal transduction mechanism is demonstrated. Surface patterns consisting of CdSe/ZnS QDs functionalized at their periphery with β-cyclodextrin (β-CD) were obtained by immobilization of the QDs from solution onto glass substrates patterned with adamantyl-terminated poly(propylene imine) dendrimeric "glue." Subsequent formation of host-guest complexes between vacant β-CD on the QD surface and an adamantyl-functionalized lissamine rhodamine resulting in FRET was confirmed by fluorescence microscopy, spectroscopy, and fluorescence lifetime imaging microscopy (FLIM).     

Analytic study of radiative heat transfer in ultra‐fine powder insulations with dependent scattering and absorption

Abstract

In this work, the radiative heat transfer of the ultra‐fine powder insulation Aerosil 380, with dependent scattering and absorption, is investigated theoretically. The radiative transport process is modeled by the two‐flux model and the diffusion approximate method to solve the government equations of transfer. The radiative properties of Aerosil 380 have been determined by the Rayleigh scattering theory because of the small values of particle size parameter. The results show that the dependent effect of scattering will reduce the scattering efficiency; however, the absorption efficiency will be increased due to the dependent absorption. The overall thermal radiation resistance is increased by the dependent effect. A comparison of radiative thermal conductivity has been calculated by the two models. The comparison reveals that the difference is small at a mean temperature of 300°K, but that the difference goes up to about 30 percent at a mean temperature of 400°K.     

Soliton solutions of the resonant nonlinear Schrödinger’s equation in optical fibers with time-dependent coefficients by simplest equation approach

In this paper, the resonant nonlinear Schrödinger’s equation is studied with four forms of nonlinearity. This equation is also considered with time-dependent coefficients. The simplest equation method is applied to solve the governing equations and then exact 1-soliton solutions are obtained. It is shown that this method provides us with a powerful mathematical tool for solving nonlinear evolution equations with time-dependent coefficients in mathematical physics.     

Mass transfer with “memory” in electrochemical processes

Diffusion processes in porous electrodes are investigated on the basis of mass-transfer equation with memory. The equation is analyzed with the application of the Laplace transform.Translated from Inzhenerno-Fizicheskii Zhurnal, Vol. 49, No. 3, pp. 481–486, September, 1985.     

Quantitative Measurement of Drug Release Dynamics within Targeted Organelles Using Förster Resonance Energy Transfer

Measuring the release dynamics of drug molecules after their delivery to the target organelle is critical to improve therapeutic efficacy and reduce side effects. However, it remains challenging to quantitatively monitor subcellular drug release in real time. To address the knowledge gap, a novel gemini fluorescent surfactant capable of forming mitochondria-targeted and redox-responsive nanocarriers is designed. A quantitative Förster resonance energy transfer (FRET) platform is fabricated using this mitochondria-anchored fluorescent nanocarrier as a FRET donor and fluorescent drugs as a FRET acceptor. The FRET platform enables real-time measurement of drug release from organelle-targeted nanocarriers. Moreover, the obtained drug release dynamics can evaluate the duration of drug release at the subcellular level, which established a new quantitative method for organelle-targeted drug release. This quantitative FRET platform can compensate for the absent assessment of the targeted release performances of nanocarriers, offering in-depth understanding of the drug release behaviors at the subcellular targets.     

Spectroscopic properties and energy transfer in Er–Tm co-doped bismuth silicate glass

In this paper, we investigate the spectroscopic properties of and energy transfer processes in Er–Tm co-doped bismuth silicate glass. The Judd–Ofelt parameters of Er³⁺ and Tm³⁺ are calculated, and the similar values indicate that the local environments of these two kinds of rare earth ions are almost the same. When the samples are pumped at 980 nm, the emission intensity ratio of Tm:³F₄ → ³H₆ to Er:⁴I_13/2 → ⁴I_15/2 increases with increased Er³⁺ and Tm³⁺ contents, indicating energy transfer from Er:⁴I_13/2 to Tm:³F₄. When the samples are pumped at 800 nm, the emission intensity ratio of Er:⁴I_13/2 → ⁴I_15/2 to Tm:³H₄ → ³F₄ increases with increased Tm₂O₃ concentration, indicating energy transfer from Tm:³H₄ to Er:⁴I_13/2. The rate equations are given to explain the variations. The microscopic and macroscopic energy transfer parameters are calculated, and the values of energy transfer from Er:⁴I_13/2 to Tm:³F₄ are found to be higher than those of the other processes. For the Tm singly-doped glass pumped at 800 nm and Er–Tm co-doped glass pumped at 980 nm, the pumping rate needed to realize population reversion is calculated. The result shows that when the Er₂O₃ doping level is high, pumping the co-doped glass by a 980 nm laser is an effective way of obtaining a low-threshold ∼2 μm gain.     

500 Hz ultraviolet dye laser with pulse energy 1.7 mJ and potential for PLIF imaging

ABSTRACT

This paper describes a high-pulse-energy frequency-doubled ultraviolet dye laser operating at a repetition rate of 500?Hz. The pump source is a laser-diode side-pumped Q-switched Nd:YAG laser with a pulse energy of 29?mJ at 532?nm. A master oscillator power amplifier is employed to amplify the output pulse of the dye laser to 8.1?mJ at 566?nm, and by frequency doubling with BBO crystal a pulse energy of 1.7?mJ at 283?nm is achieved with a pulse width of 8?ns. This is more than four times the largest reported pulse energies generated by other fixed-frequency dye lasers when operating at repetition rates of more than 1?kHz. The conversion efficiency and stability of dye laser are discussed, which show the potential for high-speed laser diagnostics in the fields of combustion and turbulent flow detection.     

Higher order dispersion effects in the noninstantaneous nonlinear Schrödinger equation

We present a systematic analysis of the effects, of higher-order dispersion, noninstantaneous nonlinear response, as well as stochastic coefficients in optical fiber. This study is motivated by recent experimental observation of a new modulational instability spectral window induced by fourth-order dispersion in a normally dispersive single-mode optical fiber. Analytical expression of pulse amplitude is deduced with the second-order gain nonuniformity and the stimulated-Brillouin scattering-induced third-order as well as fourth-order dispersion effects involved. The influence of stochasticity, as well as the delayed Raman response in the nonconventional sidebands obtained due to the fourth-order dispersion, is considered. We note that the shape of the spectrum, and in particular the relative intensities of the higher order harmonics, is highly sensitive to the initial presence of classical noise, and can therefore be taken as a signature that the MI is seeded by vacuum fluctuations. Some direct simulations to see the evolution of different continuous wave states are reported. These show the formation of modulation instability pulses as well as transitions from lower amplitude continuous wave states to higher amplitude continuous wave states. The present results fit well with recent experimental investigations.     

Schrödinger wave equation for confinement of photon in a waveguide

In the present work, electromagnetic field confinement in a subwavelength waveguide structure is obtained using concepts of quantum mechanics and uncertainty principle. Semi-macroscopic considerations of field interaction at the dielectric interfaces are used in this work. The modal field profile in the subwavelength waveguide is obtained by considering the photon as a particle in the waveguide having finite probability of tunneling. Thus, uncertainty of position is assigned to it. The momentum uncertainty is calculated from position uncertainty. Schrödinger wave equation for the photon is written by incorporating position-momentum uncertainty. The equation is solved and the field distribution in the waveguide is obtained. The field distribution and power confinement is compared with conventional waveguide theory. They were found in good agreement with each other.