Computational study of energy transfer in two-dimensional J-aggregates

We perform a computational analysis of the intra- and interband energy transfer in two-dimensional J-aggregates. Each aggregate is represented as a two-dimensional array (LB-film or self-assembled film) of two kinds of cyanine dyes. We consider the J-aggregate whose J-band is located at a shorter wavelength to be a donor and an aggregate or a small impurity with longer wavelength to be an acceptor. Light absorption in the blue wing of the donor aggregate gives rise to the population of its excitonic states. The depopulation of these states is possible by (a) radiative transfer to the ground state, (b) intraband energy transfer, and (c) interband energy transfer to the acceptor. We study the dependence of energy transfer on properties such as the energy gap, the diagonal disorder, and the exciton–phonon interaction strength. Experimentally observable parameters, such as the position and form of luminescence spectrum, and results of the kinetic spectroscopy measurements strongly depend upon the density of states in excitonic bands, rates of energy exchange between states and oscillator strengths for luminescent transitions originating from these states.     

Nonequilibrium accumulation of surface species and triboelectric charging in single component particulate systems

Triboelectric charging occurs in granular systems composed of chemically identical particles even though there is no apparent driving force for charge transfer. We show that such charging can result from nonequilibrium dynamics in which collision-induced electron transfer generates electron accumulation on a particle-size-dependent subset of the system. This idea rationalizes experimental results that suggest that smaller particles charge negatively while the large ones charge positively. This effect occurs generally when there are high energy electrons on a surface that cannot equilibrate to lower energy states on the same surface, but can transfer to lower energy states on other particles during collisions.     

Coherent control of Forster energy transfer in nanoparticle molecules: energy nanogates and plasmonic heat pulses

We study how Forster energy transfer from a semiconductor quantum dot to a metallic nanoparticle can be gated using quantum coherence in quantum dots. We show this allows us to use a laser field to open the flow of the energy transfer for a given period of time (on-state) before it is switched off to about zero. Utilizing such an energy gating process it is shown that quantum-dot-metallic-nanoparticle systems (meta-molecules) can act as functional nanoheaters capable of generating heat pulses with temporal widths determined by their environmental and physical parameters. We discuss the physics behind the energy nanogates using molecular states of such meta-molecules and the resonance fluorescence of the quantum dots.     

Long range inductive power transfer with superconducting oscillators

Resonant inductive power transfer has demonstrated the transfer of 60 W at distances in excess of 2 m with as much as 40% efficiency. The loss mechanisms include internal dissipation and radiated power. By constructing superconducting oscillators and operating at lower frequencies, both of these loss mechanisms are reduced, and this same power can be transferred at distances in excess of 100 m. A performance analysis of such a system is presented, along with proposed low-loss coil and capacitor designs to achieve this performance.     

采用非绝热动力学模拟探究溶剂效应对桨-轮形状的给体-受体复合物的激发态弛豫动力学的影响

充分理解给体-受体复合物的激发态动力学在实验和理论上都具有非常重要的意义. 本文首次结合电子结构计算和非绝热动力学模拟,探索了最近合成的一个桨-轮形状的给体-受体复合物的光致动力学过程,该复合物由三个氟硼二吡咯基团和一个六氧杂并三苯构成. 根据计算结果,得出结论,桨-轮形状的给体-受体复合物共轭物在激发时将被提升到氟硼二吡咯片段的局部激发状态,然后发生超快局部激发电子态到电荷转移电子态的激子转移. 与先前实验工作中提出的光致电子转移机理不同,这种激子转移过程伴随着从氟硼二吡咯基团到六氧杂并三苯基团上的空穴. 此外,还发现溶剂效应在该体系的光致动力学中起着重要作用. 具体而言,强极性的乙腈溶剂加速了空穴转移动力学,这可以归因于溶剂对电荷转移状态的显著影响,即局部激发和电荷转移激子之间的能隙大大减小,而与此同时非绝热耦合增加,这两个因素都可以促进空穴转移过程. 目前的工作不仅为桨-轮形状的给体-受体复合物的潜在光诱导机制提供了有价值的见解,而且有助于未来设计具有更好光电性能的新型给体-受体复合物.     

Diffusion approximations of the two dimensional master equation

The effects of rotational energy transfer on unimolecular dissociation are assessed using a two-dimensional master equation approach. The collision operator for such a system can be very large, and approximations are sought that reduce the size of the matrix that has to be stored. The density of states of the vibrational energy is large for most molecules and can be treated as virtually continuous. As a consequence, motion in vibrational energy space can be treated using a diffusion equation approach. This reduces the storage requirements greatly and increases the speed at which diagonalization occurs. Results are presented for the dissociation of ethane and methane.     

Population coherent control of Rydberg potassium atom via adiabatic passage

The time-dependent multilevel approach(TDMA) and B-spline expansion technique are used to study the coherent population transfer between the quantum states of a potassium atom by a single frequency-chirped microwave pulse.The Rydberg potassium atom energy levels of n=6-15,l=0-5 states in zero field are calculated and the results are in good agreement with other theoretical values.The time evolutions of the population transfer of the six states from n=70 to n=75 in different microwave fields are obtained.The results show that the coherent control of the population transfer from the lower states to the higher ones can be accomplished by optimizing the microwave pulse parameters.     

Parametric channeling and collapse of beams of charged particles with internal structure in crystals: 2. Parametric processes during channeling of atomic ions, nuclei, and relativistic electrons in crystals

Features of parametric effects during channeling of atomic ions, nuclei, and relativistic electrons (positrons) in crystals were considered. It was shown that parametric coupling between ion channeling states in the field of crystal axes and planes and electronic states in the ion volume leads to the possibility of “parametric collapse” of the beam, i.e., a decrease in the oscillation amplitude of the atomic ion in the channel due to periodic transfer of the ion oscillation energy to the inner electron of the atom. The same effect can be used to cool beams due to energy transfer to intrinsic nuclear states with low energy levels. It was shown that parametric cooling of beams with a decrease in the transverse energy can also occur during axial channeling of relativistic electron beams. This process results from the parametric coupling between channeling states, which are caused by the particle charge and electron spin states in an effective magnetic field induced in the moving coordinate system.     

Inter-Layer Energy Transfer through Wetting-Layer States in Bi-layer InGaAs/GaAs Quantum-Dot Structures with Thick Barriers

The inter-layer energy transfer in a bi-layer InGaAs/GaAs quantum dot structure with a thick GaAs barrier is studied using temperature-dependent photoluminescence. The abnormal enhancement of the photoluminescence of the QDs in the layer with a larger amount of coverage considering the resonant Forster energy transfer between the at 110K is observed, which can be explained by wetting layer states at elevated temperatures.     

Laser induced collisional energy transfer in Sr—Li system

A four-state model considering the relative velocity distribution function for calculating the cross section of laserinduced collisional energy transfer in a Sr-Li system is presented and profiles of laser-induced collision cross section are obtained.The resulting spectra obtained from different intermediate states are strongly asymmetrical in an opposite asymmetry.Both of the two intermediate states have contributions to the final state,and none of the intermediate states should be neglected.The peak of the laser-induced collisional energy transfer(LICET) profile shifts toward the red and the FWHM becomes narrower obviously with laser field intensity increasing.A cross section of 1.2 × 10-12 cm 2 at a laser field intensity of 2.17 × 10 7 V/m is obtained,which indicates that this collision process can be an effective way to transfer energy selectively from a storage state to a target state.The existence of saturation for cross section with the increase of the laser intensity shows that the high-intensity redistribution of transition probabilities is an important feature of this process,which is not accounted for in a two-state treatment.     

ESR study of europium ions in hydrolyzed CaF2: Eu crystals

Oxidation and reduction processes of europium ions in CaF₂ were studied by optical and ESR methods. Europium ions can be readily oxidized from the divalent to the trivalent states by heat-treatment above 600°C in a moist air atmosphere. The conversion can be well approximated by first order kinetics with an activation energy of 0.75 eV.

The reverse conversion from the trivalent to the divalent states can be accomplished by exposure to ionizing X-ray radiation. However, those reduced europium ions are thermally unstable and bleached completely by heating to 200°C. The decay process by low temperature annealing also follows first order kinetics with an activation energy of 0.60 eV. The conversions between the two states are explained by electron transfer.     

Dipole blockade at Förster resonances in high resolution laser excitation of Rydberg states of cesium atoms

High resolution laser excitation of np Rydberg states of cesium atoms shows a dipole blockade at F?rster resonances corresponding to the resonant dipole-dipole energy transfer of the np+np --> ns+(n+1)s reaction. The dipole-dipole interaction can be tuned on and off by the Stark effect, and such a process, observed for relatively low n(25-41), is promising for quantum gate devices. Both Penning ionization and saturation in the laser excitation can limit the range of observation of the dipole blockade.     

Transferring entangled states of photonic cat-state qubits in circuit QED

We propose a method for transferring quantum entangled states of two photonic cat-state qubits(cqubits)from two microwave cavities to the other two microwave cavities.This proposal is realized by using four microwave cavities coupled to a superconducting flux qutrit.Because of using four cavities with different frequencies,the inter-cavity crosstalk is significantly reduced.Since only one coupler qutrit is used,the circuit resource is minimized.The entanglement transfer is completed with a singlestep operation only,thus this proposal is quite simple.The third energy level of the coupler qutrit is not populated during the state transfer,therefore decoherence from the higher energy level is greatly suppressed.Our numerical simulations show that high-fidelity transfer of two-cqubit entangled states from two transmission line resonators to the other two transmission line resonators is feasible with current circuit QED technology.This proposal is universal and can be applied to accomplish the same task in a wide range of physical systems,such as four microwave or optical cavities,which are coupled to a natural or artificial three-level atom.     

Time allocation improvement method for UAV-based wireless energy transfer cooperative mobile edge

Wireless power transfer (WPT) and mobile edge computing (MEC) are two advanced technologies that could improve the computing power and range of mobile devices. However, by integrating the unmanned aerial vehicle (UAV) into wireless powered MEC systems, wireless energy transfer will be susceptible to the “double near–far” effect. Therefore, in order to further overcome the influence of the “double near–far” effect, this paper considers the optimization of time slot allocation for UAV-assisted wireless powered cooperative MEC system, which includes an access point (UAV) and two mobile devices. The purpose of the study is to minimize the total transmission energy of the UAV while satisfying the delay and size of the computational tasks, so this paper proposed a 2:1:1 time-slot optimization allocation method. The method exploits the synergy of users so that the mobile device which is closer to the UAV acts as an offloading relay, by combining power and time slot optimization to minimize the total energy consumption of the UAV. Compared with the equal time slot scheme before the improvement, this method can not only utilize the wireless transmission energy to charge the mobile device for more time in the first period, but also can save the time of data transmission of the closer device in the third period, and it can enhance the rate of data transmission of the mobile devices at the same time. The results show that the task capacity of the system computed will be increased compared to the original scheme; the total transmission rate of the whole system is also improved by the same order of magnitude. The simulation results verify the effectiveness and reliability of the algorithm of the paper, and the comprehensive performance of the system can be maximized by the flexible offloading algorithm.     

啁啾微波场中里德伯锂原子的相干激发与控制

运用含时多态展开方法和B-样条函数研究了微波场中里德伯锂原子高激发态的性质,得到锂原子量子态n=70-75,l=0-5的能量,并分析了里德伯锂原子高激发态n=70-75,l=0-5在微波场中的跃迁几率.结果表明:通过优化微波场参数可以实现量子系统从初始态到目标态的完全跃迁,且在跃迁过程中,每个l态都起至关重要的作用.     

A Theory of Electronic Energy Transfer in Complex Molecular Systems

The Förster theory for energy transfer is critically reviewed in the context of the present-day theory of nonradiative transitions, and the fundamental tenets of the Förster theory are shown to be erroneous. A new theory of electronic energy transfer is constructed taking into account the electronic transition theory. The intermolecular interaction between donor and acceptor molecules is assumed to perturb electron states of isolated molecules before the donor-molecule excitation. A distinguishing characteristic of the intermolecular interaction is spatial delocalization of the wave functions of electron states of the interacting molecules. It is this fact that has made it possible to realize ordinary photophysical processes between electron states of various molecules in a bimolecular system. In the experiments under study, the result of the intermolecular nonradiative photoprocess is given as evidence of electronic energy transfer from the donor molecule to the acceptor molecule.     

Förster Energy Transfer in Arrays of Epitaxial CdSe/ZnSe Quantum Dots Involving Bright and Dark Excitons

Using time-resolved photoluminescence (PL) spectroscopy, we establish the presence of the Förster energy transfer mechanism between two arrays of epitaxial CdSe/ZnSe quantum dots (QDs) of different sizes. The mechanism operates through dipole–dipole interaction between ground excitonic states of the smaller QDs and excited states of the larger QDs. The dependence of energy transfer efficiency on the width of barrier separating the QD insets is shown to be in line with the Förster mechanism. The temperature dependence of the PL decay times and PL intensity suggests the involvement of dark excitons in the energy transfer process.     

Femtosecond time-resolved energy transfer from CdSe nanoparticles to phthalocyanines

The first real-time observation of the early events during energy transfer from a photoexcited CdSe nanoparticle to an attached phthalocyanine molecule are presented in terms of a femtosecond spectroscopic pump–probe study of the energy transfer in conjugates of CdSe nanoparticles (NPs) and silicon phthalocyanines (Pcs) with 120 fs time resolution. Four different silicon phthalocyanines have been conjugated to CdSe NPs. All of these have proven potential for photodynamic therapy (PDT). In such NP-Pc conjugates efficient energy transfer (ET) from CdSe NPs to Pcs occurs upon selective photoexcitation of the NP moiety. Spectral analysis as well as time-resolved fluorescence up-conversion measurements revealed the structure and dynamics of the investigated conjugates. Femtosecond transient differential absorption (TDA) spectroscopy was used for the investigation of the non-radiative carrier and ET dynamics. The formation of excitons, trapped carriers states, as well as stimulated emission was monitored in the TDA spectra and the corresponding lifetimes of these states were recorded. The time component for energy transfer was found to be between 15 and 35 ps. The ET efficiencies are found to be 20-70% for the four Pc conjugates, according to fluorescence quenching experiments. Moreover, as a result of the conjugation between NP and the Pcs the photoluminescence efficiency of the Pc moieties in the conjugates do not strictly follow the quantum yields of the bare phthalocyanines. PACS 73.63.Bd