Efficient transfer of metallophosphor excitons via confined polaritons in organic nanocrystals

We investigate the transfer of phosphorescent energy between co-assembled metallophosphors in crystalline nanostructures [Angew. Chem. Int. Ed. 57 7820(2018) and J. Am. Chem. Soc. 140 4269(2018)]. Neither Dexter's nor Forster's mechanism of resonance energy transfer(RET) could account fully for the observed rates, which exceed 85% with significant temperature dependence. But there exists an alternative pathway on RET mediated by intermediate states of resonantly confined exciton–polaritons. Such a mechanism was used to analyze artificial photosynthesis in organic fluorescents [Phys.Rev. Lett. 122 257402(2019)]. For metallophosphors, the confined modes act as extended states lying between the molecular S_(1) and T_(1) states, offering a bridge for the long-lived T_(1) excitons to migrate from donors to acceptors. Population dynamics with parameters taken entirely based on experiments fits the observed lifetimes of phosphorescence across a broad range of doping and temperature.

Effect of electron-electron interaction on polarization process of exciton and biexciton in conjugated polymer

By using one-dimensional tight-binding model modified to include electron-electric field interaction and electron-electron interaction,we theoretically explore the polarization process of exciton and biexciton in cis-polyacetylene.The dynamical simulation is performed by adopting the non-adiabatic evolution approach.The results show that under the effect of moderate electric field,when the strength of electron-electron interaction is weak,the singlet exciton is stable but its polarization presents obvious oscillation.With the enhancement of interaction,it is dissociated into polaron pairs,the spin-flip of which can be observed through modulating the interaction strength.For the triplet exciton,the strong electron-electron interaction restrains its normal polarization,but it is still stable.In the case of biexciton,the strong electron-electron interaction not only dissociate it,but also flip its charge distribution.The yield of the possible states formed after the dissociation of exciton and biexciton is also calculated.

Behavior of exciton in direct−indirect band gap Al_(x)Ga_(1−x)As crystal lattice quantum wells

Excitons have significant impacts on the properties of semiconductors.They exhibit significantly different properties when a direct semiconductor turns in to an indirect one by doping.Huybrecht variational method is also found to influence the study of exciton ground state energy and ground state binding energy in Al_(x)Ga_(1−x)As semiconductor spherical quantum dots.The Al_(x)Ga_(1−x)As is considered to be a direct semiconductor at AI concentration below 0.45,and an indirect one at the concentration above 0.45.With regards to the former,the ground state binding energy increases and decreases with AI concentration and eigenfrequency,respectively;however,while the ground state energy increases with AI concentration,it is marginally influenced by eigenfrequency.On the other hand,considering the latter,while the ground state binding energy increases with AI concentration,it decreases with eigenfrequency;nevertheless,the ground state energy increases both with AI concentration and eigenfrequency.Hence,for the better practical performance of the semiconductors,the properties of the excitons are suggested to vary by adjusting AI concentration and eigenfrequency.

Dispersion of exciton-polariton based on ZnO/MgZnO quantum wells at room temperature

We report observation of dispersion for coupled exciton-polariton in a plate microcavity combining with ZnO/MgZnO multi-quantum well (QW) at room temperature. Benefited from the large exciton binding energy and giant oscillator strength, the room-temperature Rabi splitting energy can be enhanced to be as large as 60 meV. The results of excitonic polariton dispersion can be well described using the coupling wave model. It is demonstrated that mode modification between polariton branches allowing, just by controlling the pumping location, to tune the photonic fraction in the different detuning can be investigated comprehensively. Our results present a direct observation of the exciton-polariton dispersions based on two-dimensional oxide semiconductor quantum wells, thus provide a feasible road for coupling of exciton with photon and pave the way for realizing novel polariton-type optoelectronic devices.

The Role of Radiative Surface Modes and Longitudinal Excitons in the Formation of Exciton-Polariton Luminescence Spectra of CdS-Type Crystals

The low-temperature (T = 2 K) exciton-polariton luminescence (EPL) spectra in the vicinity of the exciton-resonance frequency An=1 for CdS-type crystals have been theoretically and experimentally investigated with allowance for the mechanical exciton decay . The results of the numerical calculations of the partial and interference contributions of the bulk and radiative surface spectral modes to the EPL in the geometry of additional s- and p-polarized waves emitted into vacuum are analyzed. It is shown that the contributions of purely longitudinal excitons and their interference with polaritons of the upper dispersion branch near the longitudinal frequency ωL to the EPL are small (∼10% - 30%);nevertheless, they must be taken into account to obtain quantitative agreement with experimental data. Specifically these contributions are responsible for the formation of an additional line (along with the fundamental AT line) in the case of oblique incidence of radiation.

Exciton-polariton based WS_(2)polarization modulator controlled by optical Stark beam

The recent era of fast optical manipulation and optical devices owe a lot to exciton-polaritons being lighter in mass,faster in speed and stronger in nonlinearity due to hybrid light-matter characteristics.The room temperature existence of polaritons in two dimensional materials opens up new avenues to the design and analysis of all optical devices and has gained the researchers attention.Here,spin-selective optical Stark effect is introduced to form a waveguide effect in uniform community of polaritons,and is used to realize polarization modulation of polaritons.The proposed device basically takes advantage of the spin-sensitive properties of optical Stark effect of polaritons inside the WS_(2)microcavity so as to guide different modes and modulate polarization of polaritons.It is shown that polaritonic wavepacket of different mode profiles can be generated by changing intensity of the optical Stark beam and the polarization of polaritons can be controlled and changed periodically along the formed waveguide by introduction birefringence that is sensitive to polarization degree of the optical Stark beam.

Hybrid Exciton—Polaritons in a Bad Microcavity Containing the Organic and Inorganic Quantum Wells

We study the hybrid exciton-polaritons in a bad microcavity containing the organic and inorganic quantum wells. The corresponding polariton states are given. The analytical solution and numerical result of the stationary spectrum for the cavity field are finished.

Active control of surface plasmon polaritons with phase change materials

Active control of surface plasmon polaritons(SPPs)is highly desired for nanophotonics.Here we employ a phase change material Ge_(2)Sb_(2)Te_(5)(GST)to actively manipulate the propagating direction of SPPs at the telecom wavelength.By utilizing the phase transition-induced refractive index change of GST,coupled with interference effects,a nanoantenna pair containing GST is designed to realize switchable one-way launching of SPPs.Devices based on the nanoantenna pairs are proposed to manipulate SPPs,including the direction tuning of SPP beams,switchable SPP focusing,and switchable cosine–Gauss SPP beam generating.Our design can be employed in compact optical circuits and photonics integration.

Modulational instability of a resonantly polariton condensate in discrete lattices

We study modulational instability of a resonantly polariton condensate in a discrete lattice.Employing a discrete gain-saturation model,we derive the dispersion relation for the modulational instability by means of the linear-stability analysis.Effects of the pumping strength,the nonlinearity,the strength of the detuning,and the coupling strength on the modulation instability are investigated.It is found that the interplay between these parameters will dramatically change the modulational instability condition.We believe that the predicted results in this work can be useful for future possible experiment of exciton-polariton condensate in lattices.

Interaction of moiréexcitons with cavity photons in two-dimensional semiconductor hetero-bilayers

Moirématerials,composed of two single-layer two-dimensional semiconductors,are important because they are good platforms for studying strongly correlated physics.Among them,moirématerials based on transition metal dichalcogenides(TMDs)have been intensively studied.The hetero-bilayer can support moiréinterlayer excitons if there is a small twist angle or small lattice constant difference between the TMDs in the hetero-bilayer and form a type-Ⅱ band alignment.The coupling of moiréinterlayer excitons to cavity modes can induce exotic phenomena.Here,we review recent advances in the coupling of moiréinterlayer excitons to cavities,and comment on the current difficulties and possible future research directions in this field.

Propagation of surface magnetoplasmon polaritons in a symmetric waveguide with two-dimensional electron gas

The properties of surface magnetoplasmon polaritons(SMPPs)in a symmetric structure,composed of two semi-infinite regions of high-density two-dimensional electron gas(2DEG)separated by a thin film in Voigt configuration,are investigated.The normal and absorption dispersion relations for the transverse magnetic polarization are derived by correlating Maxwell’s equation and the boundary conditions.It is demonstrated that the features of SMPPs are greatly influenced by the external magnetic field,collision frequency of 2DEG,the dielectric constant,and the thickness of the thin film,suggesting that the locations and propagation lengths of SMPPs can be governed accordingly.It is shown that the symmetry of the physical geometry preserves the symmetry of the dispersion relations of SMPPs.Furthermore,it is discovered that as the external magnetic field increases,the penetration depth of SMPPs decreases,while their energy loss reduces,implying that plasmons can propagate for longer distances.Additionally,it is observed that SMPPs in the symmetric configuration have a longer lifetime than those in the asymmetric configuration.

Thickness-dependent exciton relaxation dynamics of few-layer rhenium diselenide

Rhenium diselenide(ReSe_(2))has gathered much attention due to its low symmetry of lattice structure,which makes it possess in-plane anisotropic optical,electrical as well as excitonic properties and further enables ReSe_(2)have an important application in optoelectronic devices.Here,we report the thickness-dependent exciton relaxation dynamics of mechanically exfoliated few-layer ReSe_(2)flakes by using time-resolved pump–probe transient transmission spectroscopies.The results reveal two thickness-dependent relaxation processes of the excitons.The fast one correlates with the exciton formation(i.e.,the conversion of hot carriers to excitons),while the slow one is attributed to the exciton recombination dominated by defect-assisted exciton trapping besides photon emission channel.The decrease of scattering probability caused by defects leads to the increase of fast lifetime with thickness,and the increase of slow lifetime with thickness is related to the trap-mediated exciton depopulation induced by surface defects.Polarization-dependent transient spectroscopy indicates the isotropic exciton dynamics in the two-dimensional(2D)plane.These results are insightful for better understanding of excitonic dynamics of ReSe_(2)materials and its application in future optoelectronic and electronic devices.

Polarization Simultons in CARS by Polaritons

The system of shortened Maxwell’s equations simulating the processes of evolution of the stimulated Raman scattering (SRS) by polaritons in anisotropic dipole-active crystals is obtained. The theory was developed for the case of cubic crystals which become anisotropic due to the deformation of the dielectric constant by the linearly polarized pump wave. The pump field is a linearly polarized plane electromagnetic wave. We report the results of the theoretical investigation of the possibility of the existence of a regime of pulse propagation as simultaneous travel of solitary waves in coherent anti-Stokes stimulated Raman scattering by polaritons in anisotropic crystals. The emphasis was made on the existence of both Stokes and anti-Stokes pulses propagating with two stable and perpendicular to the direction of travel polarizations. We showed the theoretical possibility of simultaneous propagation of pulses not only at frequencies of Stokes and anti-Stokes waves but the pump frequency as well. We obtained the expression for the gain factor g. It is also shown that the expression for g is consistent with the experimental results for the spectra of ZnS.

Direct fabrication of flexible tensile sensors enabled by polariton energy transfer based on graphene nanosheet films

A fundamental problem in the direct manufacturing of flexible devices is the low melting temperature of flexible substrates,which hinders the development of flexible electronics.Proposed here is an electron-cyclotron-resonance sputtering system that can batch-fabricate devices directly on flexible substrates under a low temperature by virtue of the polariton energy transfer between the plasma and the material.Flexible graphene nanosheet-embedded carbon(F-GNEC)films are manufactured directly on polyimide,polyethylene terephthalate,and polydimethylsiloxane,and how the substrate bias(electron energy),microwave power(plasma flux and energy),and magnetic field(electron flux)affect the nanostructure of the F-GNEC films is investigated,indicating that electron energy and flux contribute to the formation of standing graphene nanosheets in the film.The films have good uniformity of distribution in a large size(17 mm×17 mm),and tensile and angle sensors with a high gauge factor(0.92)and fast response(50 ms)for a machine hand are obtained by virtue of the unique nanostructure of the F-GNEC film.This work sheds light on the quantum manufacturing of carbon sensors and its applications for intelligent machine hands and virtual-reality technology.

Melting of electronic/excitonic crystals in 2D semiconductor moirépatterns:A perspective from the Lindemann criterion

Using the Lindemann criterion,we analyzed the quantum and thermal melting of electronic/excitonic crystals recently discovered in two-dimensional(2D)semiconductor moirépatterns.We show that the finite 2D screening of the atomically thin material can suppress(enhance)the inter-site Coulomb(dipolar)interaction strength,thus inhibits(facilitates)the formation of the electronic(excitonic)crystal.Meanwhile,a strong enough moiréconfinement is found to be essential for realizing the crystal phase with a wavelength near 10 nm or shorter.From the calculated Lindemann ratio which quantifies the fluctuation of the site displacement,we estimate that the crystal will melt into a liquid above a critical temperature ranging from several tens Kelvin to above 100 K(depending on the system parameters).

Exciton radiative lifetime in CdSe quantum dots

Colloidal CdSe quantum dots(QDs)are promising materials for solar cells because of their simple preparation pro-cess and compatibility with flexible substrates.The QD radiative recombination lifetime has attracted enormous attention as it affects the probability of photogenerated charges leaving the QDs and being collected at the battery electrodes.However,the scaling law for the exciton radiative lifetime in CdSe QDs is still a puzzle.This article presents a novel explanation that recon-ciles this controversy.Our calculations agree with the experimental measurements of all three divergent trends in a broadened energy window.Further,we proved that the exciton radiative lifetime is a consequence of the thermal average of decays for all thermally accessible exciton states.Each of the contradictory size-dependent patterns reflects this trend in a specific size range.As the optical band gap increases,the radiative lifetime decreases in larger QDs,increases in smaller QDs,and is weakly depend-ent on size in the intermediate energy region.This study addresses the inconsistencies in the scaling law of the exciton life-time and gives a unified interpretation over a widened framework.Moreover,it provides valuable guidance for carrier separa-tion in the thin film solar cell of CdSe QDs.

共轭高聚物双分子结构中激子电致解离的动力学研究

通过绝热动力学方法,研究了共轭高聚物双分子结构中激子对外加电场的响应.当外电场强度超过某个临界值时,激子会被解离成一对自由的电子与空穴.对于双分子结构中的激子,其临界解离电场除了受电子与电子相互作用以及电声相互作用影响之外,还受分子间相互作用的影响.由动力学演化的计算得到,激子临界解离电场强度随分子间相互作用强度的增大而呈非线性降低;随电子与电子相互作用强度的增大呈非线性减小的变化;但是,随电声耦合强度的增大却呈现出线性增大的变化.

探测激子极化激元在超薄范德华微晶中的光传播

激子极化激元是一种准粒子,过渡金属二硫族化合物材料即使在室温下也能支持传播激子极化子,是非常好的纳米光子学研究平台.已有研究表明,通过散射型扫描近场光学显微镜可以对过渡金属二硫族化合物薄片中激子极化激元进行实空间探测,但波导厚度仅限于低至30 nm.本文采用三种不同波长的入射光(1550和1064 nm的近红外以及633 nm的可见光),通过基于原子力显微镜的散射型扫描近场光学显微镜测量,探测到MoS2和WSe2薄片中激子极化子普通横电模式的纳米光学成像.在厚度分别低至~3 nm(相当于4原子层)和~8 nm(相当于12原子层)的超薄MoS2和WSe2薄片上,可以清楚地观察到干涉条纹图案,大大打破了之前的测量厚度限制.当厚度接近几个原子层时,波矢量始终保持在1.6k0~1.7k0左右,而不是理论预言的1k0.这些模式的特性表明,体系是由近乎悬浮的过渡金属二硫族化合物薄片的三层对称波导构成,其对激子极性子的传播产生限域效应.研究结果为探索基于超薄过渡金属二硫族化合物材料的近红外区极化器件提供了深入的理解和开辟了新的途径.