Two-photon emission in coupled biexciton quantum dot–cavity system: Phonon-assisted model

We theoretically analyze the steady state emission spectrum and transient temporal dynamics in a coupled biexciton quantum dot（QD）–cavity system. For steady state, a phonon-assisted biexciton–exciton cascade model under continuous wave（CW） excitation is presented to explain the asymmetric QD–cavity emission spectrum intensities（intensities of cavity,exciton, and biexciton emission peak） in off-resonance condition. Results demonstrate that the electron–phonon process is crucial to the asymmetry of emission spectrum intensity. Moreover the transient characteristics of the biexciton–exciton cascade system under pulse excitation show abundant nonlinear temporal dynamic behaviors, including complicated oscillations which are caused by the four-level structure of QD model. We also reveal that under off-resonance condition the cavity outputs are slightly reduced due to the electron–phonon interaction.

Effect of interchain coupling on a biexciton in organic polymers

The effect of interchain coupling on the formation and the stability of a biexciton is studied in poly （p-phenylene vinylene） chains in the framework of the tight-binding approach. We obtain an intrachain exciton and biexciton as well as an interchain exciton and biexciton through a double-photon excitation.It is found that a biexciton is energetically favourable to two single excitons even when there exists an interchain coupling.There is a turnover value t⊥c of the interchain coupling for the formation of a biexciton,beyond which two excitons are combined into one biexciton.The binding energy of a biexciton is calculated to decrease with the increase of interchain coupling,which indicates that a biexciton is relatively stable in polymers with a weak interchain coupling.The conclusion is consistent with the experimental observations.In addition,a suggestion about how to improve the yielding efficiency or the formation of biexcitons in actual applications is given.

Phase control of group-velocity-based biexciton coherence in a multiple quantum well nanostructure

A double cascade-type four-level multiple-quantum-well-based exciton-biexciton transitions are proposed. The study is carried out on a 4.8-rim ZnSe single-quantum well which is embedded into ZnMgSSe cladding layers and pseudomor- phically grown by molecular beam epitaxy on a （0 0 1） GaAs substrate. It is displayed that the exciton spin relaxation and relative phases between applied fields can influence the transient and steady-state behaviors of absorption, dispersion, and group velocity of two weak probe and signal fields. Also, transient behaviors of electron population of different levels are discussed. It is found that the probe or signal amplification occurs in the absence of population inversion.

Long-lived Single Excitons, Trions, and Biexcitons in CdSe/CdTe Type-II Colloidal Quantum Wells

Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential electron transfer processes, which leads to a complicated situation that excited states involves not only excitons （electron-hole pairs） but also multi-excitons and charged excitons. While long-lived excitons can be obtained in various systems （e.g., semiconductor nanocrystals）, multi-excitons and charged excitons are typically shorted-lived due to nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the third carrier on a few to hundreds of picoseconds timescale. In this work, we report a study of excitons, trions （an exciton plus an additional charge）, and biexcitons in CdSe/CdTe colloidal quantum wells or nanoplatelets. The type- II band alignment effectively separates electrons and holes in space, leading to a single exciton lifetime of 340 ns which is -2 order of magnitudes longer than that in plane CdSe nanoplatelets. More importantly, the electron-hole separation also dramatically slows down Auger decay, giving rise to a trion lifetime of 70 ns and a biexciton lifetime of 11 ns, among the longest values ever reported for colloidal nanocrystals. The long-lived exciton, trion, and biexciton states, combined with the intrinsically strong light-absorption capability of two-dimensional systems, enable the CdSe/CdTe type-II nanoplatelets as promising light harvesters for efficient solar-to-fuel conversion reactions.

Second-Order Correlation Function for Asymmetric-to-Symmetric Transitions due to Spectrally Indistinguishable Biexciton Cascade Emission

We report the observed photon bunching statistics of biexciton cascade emission at zero time delay in single quantum dots by second-order correlation function g（2） （T） measurements under continuous wave excitation. It is found that the bunching phenomenon is independent of the biexciton binding energy when it varies from 0.59 meV to nearly zero. The photon bunching takes place when the exeiton photon is not spectrally distinguishable from the biexciton photon, and either of them can trigger the %tart＇ in a Hanbury-Brown and Twiss setup. However, if the exciton energy is spectrally distinguishable from the biexciton, the photon statistics will become asymmetric and a cross-bunching lineshape can be obtained. The theoretical calculations based on a model of three-level rate-equation analysis are consistent with the result of g（2）（τ） correlation function measurements.

Lateral quantum confinement regulates charge carrier transfer and biexciton interaction in CdSe/CdSeS core/crown nanoplatelets

Charge carrier dynamics essentially determines the performance of various optoelectronic applications of colloidal semiconductor nanocrystals.Among them,two-dimensional nanoplatelets provide new adjustment freedom for their unique core/crown heterostructures.Herein,we demonstrate that by fine-tuning the core size and the lateral quantum confinement,the charge carrier transfer rate from the crown to the core can be varied by one order of magnitude in CdSe/CdSeS core/alloy-crown nanoplatelets.In addition,the transfer can be affected by a carrier blocking mechanism,i.e.,the filled carriers hinder further possible transfer.Furthermore,we found that the biexciton interaction is oppositely affected by quantum confinement and electron delocalization,resulting in a non-monotonic variation of the biexciton binding energy with the emission wavelength.This work provides new observations and insights into the charge carrier transfer dynamics and exciton interactions in colloidal nanoplatelets and will promote their further applications in lasing,display,sensing,etc.

Excited state biexcitons in monolayer WSe_(2)driven by vertically grown graphene nanosheets with high-density electron trapping edges

Interface engineering in atomically thin transition metal dichalcogenides(TMDs)is becoming an important and powerful technique to alter their properties,enabling new optoelectronic applications and quantum devices.Interface engineering in a monolayer WSe_(2)sample via introduction of high-density edges of standing structured graphene nanosheets(GNs)is realized.A strong photoluminescence(PL)emission peak from intravalley and intervalley trions at about 750 nm is observed at the room temperature,which indicated the heavily p-type doping of the monolayer WSe_(2)/thin graphene nanosheet-embedded carbon(TGNEC)film heterostructure.We also successfully triggered the emission of biexcitons(excited state biexciton)in a monolayer WSe_(2),via the electron trapping centers of edge quantum wells of a TGNEC film.The PL emission of a monolayer WSe_(2)/GNEC film is quenched by capturing the photoexcited electrons to reduce the electron-hole recombination rate.This study can be an important benchmark for the extensive understanding of light–matter interaction in TMDs,and their dynamics.

Biexciton Auger recombination in mono-dispersed, quantum-confined CsPbBr3 perovskite nanocrystals obeys universal volume-scaling

Auger recombination has been a long?standing obstacle to many prospective applications of colloidal quantum dots (QDs) ranging from lasing, light-emitting diodes to bio-labeling. As such, understanding the physical underpinnings and scaling laws for Auger recombination is essential to these applications. Previous studies of biexciton Auger recombination in various QDs established a universal scaling of biexciton lifetime (rxx) with QD volume (V):τxx =γV. However, recent measurements on perovskite nanocrystals (NCs), an emerging class of enablers for light harvest!ng and emitting applications, showed significant deviations from this universal scaling law, likely because the measured NCs are weakly-confined and also have relatively broad size-distributions. Here we study biexciton Auger recombination in mono-dispersed (size distributions within 1.7%—9.0%), quantunvconfined CsPbBr3 NCs (with confinement energy up to 410 meV) synthesized using a latest approach based on thermodynamic equilibrium control. Our measurements clearly reproduce the volume-scaling of τxx in confined CsPbBb QDs. However, the scaling factor γ(0.085 ± 0.001 ps/nm^3) is one order of magnitude lower than that reported for CdSe and PbSe QDs (1.00 ± 0.05 ps/nm^3), suggest!ng unique mechanisms enhancing Auger recombination rate in perovskite NCs.

半导体量子点中双激子的双光子共振吸收

从基本的非线性光学三阶极化率出发 ,分析半导体量子点中双激子的双光子共振吸收三阶极化率 ,得到 2个入射频率光电场和只有 1个入射频率光电场的简并情况下双光子共振吸收三阶极化率 ,讨论了三阶极化率的实部和虚部在双光子共振频率附近的行为 ,随着共振频率宽度的增大 ,三阶极化率的实部和虚部很快减小 。

流体静压原位调节单量子点中单双激子能量及精细结构劈裂

在对In As单量子点施加流体静压的实验中,使用了带有压电陶瓷的连续加压装置,在低温连续施加流体静压的情况下,可以调节量子点单激子能量兰移约320 me V。在对不同流体静压下单激子发光的二阶关联函数测量之后,证明流体静压并不影响单激子发光的单光子特性。同时通过流体静压,可以实现量子点双激子态由反束缚态到束缚态的转变,并且给出了这一过程的偏振分辨光谱图。最后观察到单量子点精细结构劈裂随流体静压的增加而增加,而且精细结构劈裂的增加量可以达到约150μe V。

通过飞秒泵浦探测技术研究PbS纳米颗粒的激发态瞬态动力学过程

利用飞秒泵浦探测技术研究了PbS半导体纳米颗粒复合的S iO2溶胶凝胶薄膜的瞬态动力学过程。通过改变激发探测波长和激发光强度,研究引起PbS半导体纳米颗粒的非线性吸收的两种机制。当激发探测波长选在激子吸收峰附近(620 nm)时,由于激子的饱和吸收引起的光致漂白,当激发波长选在激子能态的低能侧(753,800 nm),同时观察到激子的饱和吸收和双激子效应引起的光致吸收。研究了激子的饱和吸收和双激子效应引起的激发态吸收随激发态电子-空穴对浓度的变化关系,表明双激子效应与载流子浓度有很大关系。在高激发强度下,双激子效应引起的诱导吸收远远大于激子跃迁引起的光致漂白,双激子效应在非线性吸收中起着决定性作用。

TURNING-OVER OF THE ELECTRIC DIPOLE IN A POLYMER

The transition from the biexciton to the exciton can turn over the direction of the electric dipole of a polymericmolecule. This turning-over action combined with the photoinduced polarization reversion can be used as a switch. Theswitching speed is governed by the relaxation time of the turning-over process, which can be determined by a dynamicalsimulation.

聚乙炔中双激子和两个单激子的稳态性质

在Su-Schrieffer-Heeger(SSH)模型基础上,计入长程电子关联的影响,研究聚乙炔分子链中双激子态与2个单激子态的稳态性质,比较不同关联强度下激子的晶格位形、能级、电荷密度波、自旋密度波以及吸收谱线。结果表明:零电子关联下分子链中的2个单激子不能稳定存在;激子半径均随着关联强度的增加而减小;与双激子的2个能级精细结构相比,2个单激子的能隙出现4个精细结构;2类激子的电荷密度波、自旋密度波与吸收谱线均随关联强度变化,并呈现显著区别。以上结果为区分分子链中2类激子的行为提供了依据,结果显示在激子行为中必须考虑电子与其的关联性。

PNB聚合物中双激子对静电场的响应

在Baranowski B櫣ttner Voit模型下,研究了计入静电场后聚对苯亚胺PNB(pernigraniline base)中的双激子(biexciton)激发态.数值计算表明,当电场为零时,双激子是自陷的极化子双激子;随着电场强度E的增加,缺陷将沿电场方向发生移动;而当E 1.8×104V/cm时,双激子将被静电场解离,形成正、负双极化子(bipolaron)而束缚在链端.这与赵等人关于高分子(如PPV,PPQ等)在强电场下,双激子不能产生而只能形成双极化子的结论相似.计算中没有出现反向极化现象.

二维双激子束缚能的研究

用简单的几何模型计算了双激子体系的束缚能，得到二维双激子与单激子的束缚能比率随σ＝ｍ＊ｅ／ｍ＊ｈ从０．３２４到０．２２８之间变化。

Backward Charge Transfer in Conjugated Polymers

It has been known that the static polarizability of a polymer chain with a biexciton is negative. In order to understand this peculiar fact, this paper studies the dynamical process of the charge transfer in the polymer chain induced by an external electric held E during forming the biexciton. The time dependence of the charge distribution in the chain reveals that the charge transfer is backward: the positive charge shifts in the opposite direction of the external electric field. Such a backward charge transfer (BCT) produces an opposite dipole, which makes the polarization negative. The effect of electron interaction on the BCT is illustrated.

量子点中双激子的关联能(英文)

采用精确对角化方法,研究了限制在半导体量子点中双激子的量子尺寸效应.计算了双激子量子点的基态和低激发态的关联能随限制强度大小变化的关系,揭示了双激子量子点的基态和低激发态能谱的重要性质.我们发现随着限制强度的增加,双激子量子点的基态和低激发态的关联能变化是不同的;我们还发现限制可以引起不同低激发态能级的偶然简并和能级的反转.这些性质都与系统的交换和旋转对称性有关.

单量子点光谱与激子动力学研究进展

胶体半导体量子点具有宽带吸收、窄带发射、发光量子产率高、发射波长连续可调等优点,是制备发光二极管、太阳能电池、探测器、激光器等光电器件的优质材料.单量子点光谱能够消除系综平均效应,可以在单粒子水平上获取量子点材料的结构和动力学信息及与其他材料间的电荷、能量转移动力学等.相关研究结果能够指引量子点材料的设计和为量子点的相关应用提供机理基础.另外基于单量子点可以开展纳米尺度上光与物质的相互作用研究,制备单光子源和纠缠光子源等.本文综述了单量子点光谱与激子动力学近期的相关研究进展,主要包括单量子点的光致发光闪烁特性和调控方式、单激子和多激子动力学研究及双激子辐射特性的调控等.最后简要地讨论了单量子点光谱未来可能的发展趋势.

电场调谐InAs量子点激子精细结构劈裂

在低温5K下,采用光致发光光谱及外加偏压调谐InAs量子点激子精细结构劈裂,研究了不同量子点激子的精细结构劈裂值大小,以及垂直电场有效地调谐激子的精细结构劈裂.对于具有较小精细结构劈裂的量子点样品,外加偏压可以使其精细结构劈裂值减小到小于激子的本征光谱宽度,从而实现基于单双激子纠缠态的制备.

半导体量子点中的双激子发光

双激子发光是半导体材料在高激发强度下形成两个激子后复合发光的一种物理过程。相较于块体材料,量子点体积小、载流子受限、能级分立,从而具有独特的双激子发光特性,具体表现为双激子结合能大,级联发射中的光子对是极化反对称的,激子对的俄歇复合效应强。从双激子发光研究的发展历程出发,重点介绍了量子点双激子发光的基本原理、光谱特性,特别是量子效应对量子纠缠和光增益的影响。讨论了量子点双激子发光在纠缠光源、量子点激光器等方面的应用潜力和目前所面临的挑战。