Strong Excitation Regime Research Articles

Coherent Raman Scattering Spectral Shapes in a Strong Excitation Regime (Model Calculations)

Coherent Raman Scattering Spectral Shapes in a Strong Excitation Regime (Model Calculations)

Metallic photoluminescence of plasmonic nanoparticles in both weak and strong excitation regimes

Abstract The luminescent nature of plasmonic nanoparticles (NPs) has been intensively investigated in recent years. Plasmon-enhanced electronic Raman scattering and the radiation channels of metallic photoluminescence (PL) involving conventional carrier recombinations and emergent particle plasmons are proposed in the past few decades but largely limited to weak excitation regimes. Here, we systematically examine the PL evolution of plasmonic NPs under different excitation power levels. The spectral resonances and chromaticity of PL are investigated within and beyond the scope of geometry conservation. Results indicate the nature of PL in plasmonic NPs could be a process of graybody radiation, including one factor of plasmonic emissivity in the weak excitation regime and the other factor of blackbody radiation in the strong excitation regime. This comprehensive analysis provides a fundamental understanding of the luminescent nature of plasmonic NPs and highlights their potential applications in transient temperature detection at the nanometer scale.

Modulation of the Transient Magnetization of an EuO/Co Bilayer Tuned by Optical Excitation

AbstractThe magnetic proximity effect provides a promising way to increase the low Curie temperature (TC) of europium monoxide (EuO) toward or even above room temperature, while keeping its stoichiometry and insulating properties. This work studies EuO/Co bilayers using static and time‐resolved magneto‐optical Kerr effect measurements, and explores the influence of magnetic proximity on TC and on the spin dynamics in EuO. Excitation above the EuO bandgap results in an ultrafast enhancement of the EuO magnetization followed by a demagnetization within nanoseconds. This behaviour is also visible upon selectively photoexciting Co in the EuO/Co bilayer placed in an out‐of‐plane magnetic field, which is attributed to propagation of a superdiffusive spin current from Co into EuO. As the spin dynamics of Co shows a transient thermal demagnetization, the bilayer provides a system where the transient magneto‐optical signal can be tuned in amplitude and sign by varying external parameters such as the sample temperature or pump fluence. Moreover, in a strong excitation regime it is possible to measure the magnetic hysteresis of the underlying EuO, which is present up to room temperature – giving experimental evidence for the presence of a tuneable magnetic proximity coupling between Co and EuO.

Biexciton Blinking in CdSe-Based Quantum Dots.

Experiments on single colloidal quantum dots (QDs) have revealed temporal fluctuations in the emission efficiency of the single-exciton state. These fluctuations, often termed "blinking", are caused by opening/closing of charge-carrier traps and/or charging/discharging of the QD. In the regime of strong optical excitation, multiexciton states are formed. The emission efficiencies of multiexcitons are lower because of Auger processes, but a quantitative characterization is challenging. Here, we quantify fluctuations of the biexciton efficiency for single CdSe/CdS/ZnS core-shell QDs. We find that the biexciton efficiency "blinks" significantly. The additional electron due to charging of a QD accelerates Auger recombination by a factor of 2 compared to the neutral biexciton, while opening/closing of a charge-carrier trap leads to an increase of the nonradiative recombination rate by a factor of 4. To understand the fast rate of trap-assisted recombination, we propose a revised model for trap-assisted recombination based on reversible trapping. Finally, we discuss the implications of biexciton blinking for lasing applications.

Power-Dependent Characteristics of Spin Current Transfer in Metal Bilayer Devices under High-Power Pulse Excitation.

The power-dependent transfer characteristics of spin currents generated at the interface of the permalloy/Pt bilayer device have been investigated over a wide power range from a few tens of milliwatt to 396 W. We built a high-power pulse excitation system for spin pumping, which achieves large electromotive force (EMF) values of 10 mV at 396 W excitation through the inverse spin Hall effect (ISHE) and demonstrates that the EMF generation after pulse excitation is very fast. Under strong pulse microwave excitation more than 80 W, the EMF spectrum exhibits an asymmetrical lineshape, which is well reproduced by simulations that take into account the fold-over effect due to the nonlinear ferromagnetic resonance excitation. The maximum output power at an external load through spin pumping and the ISHE is shown to increase in proportion to the square of the input microwave power (Pin) in the power range below 80 W. This power generation proportional to Pin2 is unique to spin current-mediated power flow. In the strong excitation regime with the fold-over type EMF spectra, the EMF values of the peak magnetic field position are found to increase less linearly due to spectral broadening. This feature can be used for power generation that increases nonlinearly with respect to the input excitation power, where the nonlinearity is adjusted by varying the magnetic field position.

Third-order photon cross-correlations in resonance fluorescence

We investigated third-order correlations between photons from a single quantum dot's resonance fluorescence in the strong excitation regime originating from opposite sidebands of the power spectrum. The three-time correlation measurements for photons filtered using three independent Fabry-Perot etalons resulted in correlation maps with ``antibunching'' features as a consequence of correlations originating from the same sideband, and ``bunching ridges'' due to opposite sideband correlated photons.

Subradiance and superradiance-to-subradiance transition in dilute atomic clouds

We experimentally study subradiance in a dilute cloud of ultracold rubidium (Rb) atoms where $n \lambda_a^3 \approx 10^{-2}$ ($n$: atomic density, $\lambda_a$ excitation wavelength) and the on-resonance optical depth of the cloud is of order unity. We show that in the strong excitation regime, the subradiant time-scales depend on the excitation fraction of the cloud; i.e., to the intensity of the excitation pulse. In this regime, the decay dynamics are highly complicated and there is not a single decay time-constant. Instead, the decay time constant varies during the dynamics. Specifically, we were able to observe signatures of superradiant-to-subradiant transition; i. e., initially the decay rate is faster than independent decay (superradiant emission), while at later times it transitions to slower (subradiant emission). We also discuss a theoretical model whose numerical results are in good agreement with the experiments.

Ultrafast nematic-orbital excitation in FeSe

The electronic nematic phase is an unconventional state of matter that spontaneously breaks the rotational symmetry of electrons. In iron-pnictides/chalcogenides and cuprates, the nematic ordering and fluctuations have been suggested to have as-yet-unconfirmed roles in superconductivity. However, most studies have been conducted in thermal equilibrium, where the dynamical property and excitation can be masked by the coupling with the lattice. Here we use femtosecond optical pulse to perturb the electronic nematic order in FeSe. Through time-, energy-, momentum- and orbital-resolved photo-emission spectroscopy, we detect the ultrafast dynamics of electronic nematicity. In the strong-excitation regime, through the observation of Fermi surface anisotropy, we find a quick disappearance of the nematicity followed by a heavily-damped oscillation. This short-life nematicity oscillation is seemingly related to the imbalance of Fe 3dxz and dyz orbitals. These phenomena show critical behavior as a function of pump fluence. Our real-time observations reveal the nature of the electronic nematic excitation instantly decoupled from the underlying lattice.

Spatiotemporal profile of yoked superfluorescence from Rb vapor in the strong-excitation regime

We investigated both spatial and temporal profiles of the 420-nm yoked superfluorescence (YSF) from the atomic vapor of rubidium by driving the $5S\ensuremath{-}5D$ two-photon transition with an ultrashort laser pulse. By increasing the pump-pulse power beyond the saturation intensity, the spatial profile of the 420-nm YSF periodically changed between a central bright spot and a ring-shaped radial profile. The temporal profile of the 420-nm YSF was measured with a sampling oscilloscope with a time resolution of 50 ps. The experimental results were successfully reproduced by simulations using the Maxwell-Bloch equations. The simulated results confirmed that, in the strong excitation regime, the 420-nm emission from the lower transition component of the YSF is significantly delayed with respect to the 5.2-$\ensuremath{\mu}\mathrm{m}$ emission from the upper transition, while they are overlapped in the weak excitation regime.

Unconventional double-bended saturation of carrier occupation in optically excited graphene due to many-particle interactions

Saturation of carrier occupation in optically excited materials is a well-established phenomenon. However, so far, the observed saturation effects have always occurred in the strong-excitation regime and have been explained by Pauli blocking of the optically filled quantum states. On the basis of microscopic theory combined with ultrafast pump-probe experiments, we reveal a new low-intensity saturation regime in graphene that is purely based on many-particle scattering and not Pauli blocking. This results in an unconventional double-bended saturation behaviour: both bendings separately follow the standard saturation model exhibiting two saturation fluences; however, the corresponding fluences differ by three orders of magnitude and have different physical origin. Our results demonstrate that this new and unexpected behaviour can be ascribed to an interplay between time-dependent many-particle scattering and phase-space filling effects.

Ultrafast photo-induced dynamics across the metal-insulator transition of VO2

The transient reflectivity of VO2 films across the metal-insulator transition clearly shows that with low-fluence excitation, when insulating domains are dominant, energy transfer from the optically excited electrons to the lattice is not instantaneous, but precedes the superheating-driven expansion of the metallic domains. This implies that the phase transition in the coexistence regime is lattice-, not electronically-driven, at weak laser excitation. The superheated phonons provide the latent heat required for the propagation of the optically-induced phase transition. For VO2 this transition path is significantly different from what has been reported in the strong-excitation regime. We also observe a slow-down of the superheating-driven expansion of the metallic domains around the metal-insulator transition, which is possibly due to the competition among several co-existing phases, or an emergent critical-like behavior.

Directive Surface Plasmons on Tunable Two-Dimensional Hyperbolic Metasurfaces and Black Phosphorus: Green’s Function and Complex Plane Analysis

We study the electromagnetic response of two- and quasi-two-dimensional hyperbolic materials, on which a simple dipole source can excite a well-confined and tunable surface plasmon polariton (SPP). The analysis is based on the Green's function for an anisotropic two-dimensional surface, which nominally requires the evaluation of a two-dimensional Sommerfeld integral. We show that for the SPP contribution this integral can be evaluated efficiently in a mixed continuous-discrete form as a continuous spectrum contribution (branch cut integral) of a residue term, in distinction to the isotropic case, where the SPP is simply given as a discrete residue term. The regime of strong SPP excitation is discussed, and complex-plane singularities are identified, leading to physical insight into the excited SPP. We also present a stationary phase solution valid for large radial distances. Examples are presented using graphene strips to form a hyperbolic metasurface, and thin-film black phosphorus. The Green's function and complex-plane analysis developed allows for the exploration of hyperbolic plasmons in general 2D materials.

Recombination channels in optically excited graphene

We present a theoretical study on the efficiency of non-radiative recombination channels in optically excited graphene on a substrate. We find that depending on the strength of the excitation pulse and the dielectric constant of the applied substrate, either Auger or phonon-induced recombination prevails. The favorable conditions for Auger recombination are (i) strong excitation regime providing a large number of scattering partners and (ii) low-dielectric substrates, which only weakly screen the Coulomb interaction. The gained insights are important for achieving a population inversion in graphene that is temporally limited by the presented recombination channels. Carrier recombination channels in optically excited graphene.

Plasmon enhancement mechanism for the upconversion processes in NaYF4:Yb(3+),Er(3+) nanoparticles: Maxwell versus Förster.

Rare-earth activated upconversion materials are receiving renewed attention for their potential applications in bioimaging and solar energy conversion. To enhance the upconversion efficiency, surface plasmon has been employed but the reported enhancements vary widely and the exact enhancement mechanisms are not clearly understood. In this study, we synthesized upconversion nanoparticles (UCNPs) coated with amphiphilic polymer which makes UCNPs water soluble and negatively charged. We then designed and fabricated a silver nanograting on which three monolayers of UCNPs were deposited by polyelectrolyte-mediated layer-by-layer deposition technique. The final structures exhibited surface plasmon resonance at the absorption wavelength of UCNP. The green and red photoluminescence intensity of UCNPs on nanograting was up to 16 and 39 times higher than the reference sample deposited on flat silver film, respectively. A thorough analysis of rate equations showed that the enhancement was due entirely to absorption enhancement in the strong excitation regime, while the enhancement of both absorption and Förster energy transfer contribute in the weak excitation regime. The Purcell factor was found to be small and unimportant because the fast nonradiative decay dominates the relaxation process. From the experimentally observed enhancements, we concluded 3.1× and 1.7× enhancements for absorption and Förster energy transfer, respectively. This study clearly shows the plasmon enhancement mechanism and its excitation power dependence. It provides the basis for comparison of the enhancements of various plasmonic UCNP systems in the literature. It also lays the foundation for rational design of optical plasmonic structures for upconversion enhancement.

Model of the photoexcitation processes of a two-level molecule coherently coupled to an optical antenna

We theoretically investigate photoexcitation processes of a two-level molecular system coherently coupled with an antenna system having a significant dissipation. The auxiliary antenna enables the whole system to exhibit anomalous optical effects by controlling the coupling with the molecule. For example, in the weak excitation regime, the quantum interference yields a distinctive energy transparency through the antenna, which drastically reduces the energy dissipation. On the other hand, in the strong excitation regime, a population inversion of the two-level molecule appears due to the nonlinear effect. Both phenomena can be explained by regarding the antenna and molecule as one quantum-mechanically coupled system. Such an approach drives further research to exploit the full potential of the coupled systems.

Asymptotic exchange coupling of quasi-one-dimensional excitons in carbon nanotubes

An analytical expression is obtained for the biexciton binding energy as a function of the interexciton distance and binding energy of constituent quasi-one-dimensional excitons in carbon nanotubes. This allows one to trace biexciton energy variation and relevant nonlinear absorption under external conditions whereby the exciton binding energy varies. The nonlinear absorption line shapes calculated exhibit characteristic asymmetric (Rabi) splitting as the exciton energy is tuned to the nearest interband plasmon resonance. These results are useful for tunable optoelectronic device applications of optically excited semiconducting carbon nanotubes, including the strong excitation regime with optical nonlinearities.

Stable optical-signal emitter based on a semiconductor photonic dot

We propose a polariton hyperparametric oscillator (PHO) based on a semiconductor photonic dot at the micro/nano scale. By theoretical derivations and numerical calculations, we find that the PHO not only amplify weak signals like general large-planar polariton amplifiers, but also depress strong signals unusually. The coexistence of such signal amplification and depression can cause a stable signal emission being almost independent of the excitation instabilities in the strong-excitation regime. It has been verified that the instability of the signal emission, increasing with the increase of the excitation instabilities, is only about one to two percent deviation from its average intensity even under strong instable excitations. Hence, the PHO can serve as a stable optical-signal emitter in micro/nano optical systems.

Ultrafast Gates for Single Atomic Qubits

We demonstrate single-qubit operations on a trapped atom hyperfine qubit using a single ultrafast pulse from a mode-locked laser. We shape the pulse from the laser and perform a π rotation of the qubit in less than 50 ps with a population transfer exceeding 99% and negligible effects from spontaneous emission or ac Stark shifts. The gate time is significantly shorter than the period of atomic motion in the trap (Ω(Rabi)/ν(trap)>10(4)), demonstrating that this interaction takes place deep within the strong excitation regime.

Exciton–plasmon coupling and biexcitonic nonlinearities in individual carbon nanotubes

Optical response of small-diameter ( ≲ 1 nm ) semiconducting carbon nanotubes is discussed under the variable exciton-surface-plasmon coupling both in the linear excitation regime and in the non-linear excitation regime with the photoinduced biexcitonic states formation. The Rabi splitting effect ∼0.1 eV takes place in both cases, indicating the strong exciton–plasmon coupling both for single excitons and for biexcitons as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube. These results should be useful for the development of new tunable optoelectronic device applications of optically excited semiconducting carbon nanotubes, including the strong excitation regime with optical non-linearities.

Energy Transfer and Avalanche Upconversion of NdxY1−xVO4 Nanocrystals

We explore Nd concentration and excitation power dependences of the avalanche upconversion of NdxY1–x VO4 (x = 0–1) nanocrystals with uniform size and shape. The avalanche threshold power caused by the near-resonant energy transfer between 4F5/2 → 4I13/2 and 4F5/2 → 2G9/2 significantly decreases as the Nd3+ concentration increases. The off-resonant energy transfer between 4F5/2 → 4I13/2 and 4F5/2 → 4G11/2 in the strong excitation regime leads to apparent broadening on the blue-side of the upconversion spectrum of NdVO4 nanocrystals.