Probing ultrafast energy transfer between excitons and plasmons in the ultrastrong coupling regime

Cataloged from PDF version of article.We investigate ultrafast energy transfer between excitons and plasmons in ensembles of core-shell type nanoparticles consisting of metal core covered with a concentric thin J-aggregate (JA) shell. The high electric field localization by the Ag nanoprisms and the high oscillator strength of the JAs allow us to probe this interaction in the ultrastrong plasmon-exciton coupling regime. Linear and nonlinear optical properties of the coupled system have been measured using transient absorption spectroscopy revealing that the hybrid system shows half-plasmonic and half-excitonic properties. The tunability of the nanoprism plasmon resonance provides a flexible platform to study the dynamics of the hybrid state in a broad range of wavelengths. (C) 2014 AIP Publishing LLC

On well-posedness of the nonlocal boundary value problem for parabolic difference equations

We consider the nonlocal boundary value problem for difference equations (uk−uk−1)/τ+Auk=φk, 1≤k≤N, Nτ=1, and u0=u[λ/τ]+φ, 0<λ≤1, in an arbitrary Banach space E with the strongly positive operator A. The well-posedness of this nonlocal boundary value problem for difference equations in various Banach spaces is studied. In applications, the stability and coercive stability estimates in Hölder norms for the solutions of the difference scheme of the mixed-type boundary value problems for the parabolic equations are obtained. Some results of numerical experiments are given

The seasonal behavior of the refractive index of the ionosphere over the equatorial region

In this study, the seasonal behavior of the refractive index of the ionosphere over equator region is investigated both for collisional and collisionless cases by using the real geometry of Earth’s magnetic field for north hemisphere with respect to latitudes. It is observed that there is a harmony between the behavior of the electron density distribution and extra ordinary waves both for collisional and collisionless cases at hmF2 peak in the ionosphere.Bu çalışmada, ekvator bölgesinde iyonosferin kırılma indisinin mevsimsel davranışı, dünyanın gerçek manyetik alan geometrisi kullanılarak hem çarpışmalı hemde çarpışmasız durumlarda, kuzey yarım küre için enleme göre çalışılmıştır. İyonsferin hmF2 (F2- bölgesinin tepe yüksekliği) de çarpışmalı ve çarpışmasız durum için elektron yoğunlu dağılımı ile exra-ordinary dalgnın davranışı arasında bir uyum olduğu görülmüştü

Tunable Plexcitonic Nanoparticles: A Model System for Studying Plasmon-Exciton Interaction from the Weak to the Ultrastrong Coupling Regime

Controlling the number of dye molecules on metallic nanoparticles, which in turn affects the magnitude of Rabi splitting energy, is crucial for obtaining hybrid metal core-organic shell nanoparticles with tunable optical properties in the visible spectrum since the magnitude of the Rabi splitting energy directly determines the strength of the coupling between plasmonic nanoparticles and dye molecules. In this work, we present a new method for the synthesis of plexcitonic nanoparticles, and thus we are able to control the number of dye molecules self-assembled on Ag nanoprisms (Ag NPs) by adjusting the concentration of dye molecules used in the synthesis. Indeed, individual dye molecules self-assemble into J-aggregates on Ag NPs. Thus, in the finite-element simulations and experimental data of the hybrid metal organic nanoparticles, we observed a transition from weak coupling to the ultrastrong coupling regime. Besides, ultrafast energy transfer between plasmonic nanoparticles and excitonic aggregated dye molecules has been extensively studied as a function of Rabi splitting energy. We observe that the lifetime of the polariton states increases with the coupling strength and the upper polaritons are short-lived, whereas the lower polaritons are long-lived. Hybrid metal-organic nanoparticles presented in this study (i) have tunable Rabi splitting energies, (ii) are easy to prepare in large quantities in aqueous medium, (iii) can be uniformly assembled on solid substrates, (iv) have resonance frequencies in the visible spectrum, and (v) have small mode volume, thus making them an excellent model system for studying light-matter interaction at nanoscale dimensions from the weak to ultrastrong coupling regime. © 2016 American Chemical Society

Fabrication of Supramolecular n/p-Nanowires via Coassembly of Oppositely Charged Peptide-Chromophore Systems in Aqueous Media

Fabrication of supramolecular electroactive materials at the nanoscale with well-defined size, shape, composition, and organization in aqueous medium is a current challenge. Herein we report construction of supramolecular charge-transfer complex one-dimensional (1D) nanowires consisting of highly ordered mixed-stack π-electron donor-acceptor (D-A) domains. We synthesized n-type and p-type β-sheet forming short peptide-chromophore conjugates, which assemble separately into well-ordered nanofibers in aqueous media. These complementary p-type and n-type nanofibers coassemble via hydrogen bonding, charge-transfer complex, and electrostatic interactions to generate highly uniform supramolecular n/p-coassembled 1D nanowires. This molecular design ensures highly ordered arrangement of D-A stacks within n/p-coassembled supramolecular nanowires. The supramolecular n/p-coassembled nanowires were found to be formed by A-D-A unit cells having an association constant (KA) of 5.18 × 105 M-1. In addition, electrical measurements revealed that supramolecular n/p-coassembled nanowires are approximately 2400 and 10 times more conductive than individual n-type and p-type nanofibers, respectively. This facile strategy allows fabrication of well-defined supramolecular electroactive nanomaterials in aqueous media, which can find a variety of applications in optoelectronics, photovoltaics, organic chromophore arrays, and bioelectronics. © 2017 American Chemical Society

Ultrafast electron/energy transfer and intersystem crossing mechanisms in bodipy-porphyrin compounds

Meso-substituted borondipyrromethene (BODIPY)-porphyrin compounds that include free base porphyrin with two different numbers of BODIPY groups (BDP-TTP and 3BDP-TTP) were designed and synthesized to analyze intramolecular energy transfer mechanisms of meso-substituted BODIPY-porphyrin dyads and the effect of the different numbers of BODIPY groups connected to free-base porphyrin on the energy transfer mechanism. Absorption spectra of BODIPY-porphyrin conjugates showed wide absorption features in the visible region, and that is highly valuable to increase light-harvesting efficiency. Fluorescence spectra of the studied compounds proved that BODIPY emission intensity decreased upon the photoexcitation of the BODIPY core, due to the energy transfer from BODIPY unit to porphyrin. In addition, ultrafast pump-probe spectroscopy measurements indicated that the energy transfer of the 3BDP-TTP compound (about 3 ps) is faster than the BDP-TTP compound (about 22 ps). Since the BODIPY core directly binds to the porphyrin unit, rapid energy transfer was seen for both compounds. Thus, the energy transfer rate increased with an increasing number of BODIPY moiety connected to free-base porphyrin

Ultrafast transient optical loss dynamics in exciton-plasmon nano-assemblies

We study the exciton-plasmon dynamics that lead to optical loss mitigation via ultrafast transient absorption spectroscopy (UTAS) on hybrid aggregates of core-shell quantum dots (QDs) and Au nanoparticles (NPs). We highlight that generating hot electrons in plasmonic NPs contributes to the transient differential absorption spectrum under optical excitation. The results suggest modifying the method of analyzing the transient absorption spectra of loss mitigated systems. Additionally, we investigate the effect of Electron Oscillation frequency-Phonon Resonance Detuning (EOPRD) on loss mitigation efficiency. Moreover, power dependent UTAS reveal a frequency pulling like effect in the transient bleach maximum towards the gain emission. We show that the appropriate choice of the pump wavelength and by changing the pump power we can conclusively prove the existence of loss mitigation using UTAS. Finally, we study the transient kinetics of hybrid gain-plasmon systems and report interesting hybrid transient kinetics. © 2017 The Royal Society of Chemistry

Expanding the clinical and immunological phenotypes of PAX1-deficient SCID and CID patients

Paired box 1 (PAX1) deficiency has been reported in a small number of patients diagnosed with otofaciocervical syndrome type 2 (OFCS2). We described six new patients who demonstrated variable clinical penetrance. Reduced transcriptional activity of pathogenic variants confirmed partial or complete PAX1 deficiency. Thymic aplasia and hypoplasia were associated with impaired T cell immunity. Corrective treatment was required in 4/6 patients. Hematopoietic stem cell transplantation resulted in poor immune reconstitution with absent naïve T cells, contrasting with the superior recovery of T cell immunity after thymus transplantation. Normal ex vivo differentiation of PAX1-deficient CD34+ cells into mature T cells demonstrated the absence of a hematopoietic cell-intrinsic defect. New overlapping features with DiGeorge syndrome included primary hypoparathyroidism (n = 5) and congenital heart defects (n = 2), in line with PAX1 expression during early embryogenesis. Our results highlight new features of PAX1 deficiency, which are relevant to improving early diagnosis and identifying patients requiring corrective treatment