Strong plasmonic fluorescence enhancement of individual plant light-harvesting complexes

Plasmonic coupling of metallic nanoparticles and adjacent pigments can dramatically increase the brightness of the pigments due to the enhanced local electric field. Here, we demonstrate that the fluorescence brightness of a single plant light-harvesting complex (LHCII) can be significantly enhanced when coupled to single gold nanorods (AuNRs). The AuNRs utilized in this study were prepared via chemical reactions, and the hybrid system was constructed using a simple and economical spin-assisted layer-by-layer technique. Enhancement of fluorescence brightness of up to 240-fold was observed, accompanied by a 109-fold decrease in the average (amplitude-weighted) fluorescence lifetime from approximately 3.5 ns down to 32 ps, corresponding to an excitation enhancement of 63-fold and emission enhancement of up to 3.8-fold. This large enhancement is due to the strong spectral overlap of the longitudinal localized surface plasmon resonance of the utilized AuNRs and the absorption or emission bands of LHCII. This study provides an inexpensive strategy to explore the fluorescence dynamics of weakly emitting photosynthetic light-harvesting complexes at the single molecule level.Comment: 23 pages, 6 figures, 2 supplementary figures, and supplementary equation

Systematic study of Mn-doping trends in optical properties of (Ga,Mn)As

We report on a systematic study of optical properties of (Ga,Mn)As epilayers spanning the wide range of accessible substitutional Mn_Ga dopings. The growth and post-growth annealing procedures were optimized for each nominal Mn doping in order to obtain films which are as close as possible to uniform uncompensated (Ga,Mn)As mixed crystals. We observe a broad maximum in the mid-infrared absorption spectra whose position exhibits a prevailing blue-shift for increasing Mn-doping. In the visible range, a peak in the magnetic circular dichroism blue shifts with increasing Mn-doping. These observed trends confirm that disorder-broadened valence band states provide a better one-particle representation for the electronic structure of high-doped (Ga,Mn)As with metallic conduction than an energy spectrum assuming the Fermi level pinned in a narrow impurity band.Comment: 22 pages, 14 figure

Semiconductor Bloch equation analysis of optical Stark and Bloch-Siegert shifts in monolayers WSe2_2 and MoS2_2

We report on the theoretical and experimental investigation of valley-selective optical Stark and Bloch-Siegert shifts of exciton resonances in monolayers WSe$_2$ and MoS$_2$ induced by strong circularly polarized nonresonant optical fields. We predict and observe transient shifts of both 1sA and 1sB exciton transitions in the linear interaction regime. The theoretical description is based on semiconductor Bloch equations. The solutions of the equations are obtained with a modified perturbation technique, which takes into account many-body Coulomb interaction effects. These solutions allow to explain the polarization dependence of the shifts and calculate their values analytically. We found experimentally the limits of the applicability of the theoretical description by observing the transient exciton spectra change due to many-body effects at high field amplitudes of the driving wave.Comment: 20 pages, 9 figures, this manuscript is related to the "Giant valley-selective Stark and Bloch-Siegert shifts of exciton resonances in WSe$_2$ and MoS$_2$ monolayers" manuscrip

Giant valley-selective Stark and Bloch-Siegert shifts of exciton resonances in WSe2_2 and MoS2_2 monolayers

In this letter we demonstrate that the valley degeneracy of exciton states in monolayers of WSe$_2$ and MoS$_2$ can be lifted by the interaction with strong circularly-polarized infrared pulses with durations of only few periods of the electric field whose photon energy is much lower than the energy of the excitonic transition. The observed valley-sensitive blue shifts of excitonic absorption lines are consequences of optical Stark and Bloch-Siegert shifts acting exclusively on the opposite valleys of the monolayer. We measured the transient valley-selective changes of sample reflectivity for 1sA as well as for 1sB exciton transitions corresponding to the two most intensive resonances in the studied materials. For the studied phenomena we developed a theoretical description based on semiconductor Bloch equations, which goes beyond the simple two-level model used in previous investigations. The theoretical approach takes into account Coulomb many-body effects in the monolayer and provides a unified description of both types of shifts. The detected room-temperature excitonic energy shifts of up to 30\,meV pave the way for practical applications of these effects.Comment: 6 pages, 3 figures, the manuscript is related to the "Semiconductor Bloch equation analysis of optical Stark and Bloch-Siegert shifts in monolayers WSe$_2$ and MoS$_2$" manuscrip

Polarization-controlled optimal scatter suppression in transient absorption spectroscopy

Ultrafast transient absorption spectroscopy is a powerful technique to study fast photo-induced processes, such as electron, proton and energy transfer, isomerization and molecular dynamics, in a diverse range of samples, including solid state materials and proteins. Many such experiments suffer from signal distortion by scattered excitation light, in particular close to the excitation (pump) frequency. Scattered light can be effectively suppressed by a polarizer oriented perpendicular to the excitation polarization and positioned behind the sample in the optical path of the probe beam. However, this introduces anisotropic polarization contributions into the recorded signal. We present an approach based on setting specific polarizations of the pump and probe pulses, combined with a polarizer behind the sample. Together, this controls the signal-to-scatter ratio (SSR), while maintaining isotropic signal. We present SSR for the full range of polarizations and analytically derive the optimal configuration at angles of 40.5° between probe and pump and of 66.9° between polarizer and pump polarizations. This improves SSR by 33 52 ≈. (or 3 compared to polarizer parallel to probe). The calculations are validated by transient absorption experiments on the common fluorescent dye Rhodamine B. This approach provides a simple method to considerably improve the SSR in transient absorption spectroscopy

Exciton spin dynamics in spherical CdS quantum dots

Exciton spin dynamics in quasi-spherical CdS quantum dots is studied in detail experimentally and theoretically. Exciton states are calculated using the 6-band k.p Hamiltonian. It is shown that for various sets of Luttinger parameters, when the wurtzite lattice crystal field splitting and Coulomb interaction between the electron-hole pair are taken into account exactly, both the electron and hole wavefunction in the lowest exciton state are of S-type. This rules out the spatial-symmetry-induced origin of the dark exciton in CdS quantum dots. The exciton bleaching dynamics is studied using time- and polarization-resolved transient absorption technique of ultrafast laser spectroscopy. Several samples with a different mean size of CdS quantum dots in different glass matrices were investigated. This enabled the separation of effects that are typical for one particular sample from those that are general for this type of material. The experimentally determined dependence of the electron spin relaxation rate on the radius of quantum dots agrees well with that computed theoretically.Comment: 24 pages, 10 figure

Direct measurement of the three dimensional magnetization vector trajectory in GaMnAs by a magneto-optical pump-and-probe method

We report on a quantitative experimental determination of the three-dimensional magnetization vector trajectory in GaMnAs by means of the static and time-resolved pump-and-probe magneto-optical measurements. The experiments are performed in a normal incidence geometry and the time evolution of the magnetization vector is obtained without any numerical modeling of magnetization dynamics. Our experimental method utilizes different polarization dependences of the polar Kerr effect and magnetic linear dichroism to disentangle the pump-induced out-of-plane and in-plane motions of magnetization, respectively. We demonstrate that the method is sensitive enough to allow for the determination of small angle excitations of the magnetization in GaMnAs. The method is readily applicable to other magnetic materials with sufficiently strong circular and linear magneto-optical effects.Comment: main paper: 7 pages, 3 figures; supplementary information: 11 pages, 6 figure

Comparison of micromagnetic parameters of the ferromagnetic semiconductors (Ga,Mn)(As,P) and (Ga,Mn)As

We report on the determination of micromagnetic parameters of epilayers of the ferromagnetic semiconductor (Ga,Mn)As, which has an easy axis in the sample plane, and (Ga,Mn)(As,P), which has an easy axis perpendicular to the sample plane.We use an optical analog of ferromagnetic resonancewhere the laser-pulse-induced precession of magnetization is measured directly in the time domain. By the analysis of a single set of pump-and-probe magneto-optical data, we determined the magnetic anisotropy fields, the spin stiffness, and the Gilbert damping constant in these two materials. We show that incorporation of 10% of phosphorus in (Ga,Mn)As with 6% of manganese leads not only to the expected sign change of the perpendicular-to-plane anisotropy field but also to an increase of the Gilbert damping and to a reduction of the spin stiffness. The observed changes in the micromagnetic parameters upon incorporating P in (Ga,Mn)As are consistent with the reduced hole density, conductivity, and Curie temperature of the (Ga,Mn)(As,P) material.We also show that the apparent magnetization precession damping is stronger for the n=1 spinwave resonance mode than for the n=0 uniform magnetization precession mode