Academic literature on the topic 'Coherent generation of excitonic complex states'

A dialogue game is presented that enables us to generate coherent elementary conversational sequences at the speech act level. Central to this approach is the fact that the cognitive states of players change as a result of the interpretation of speech acts and that these changes provoke the production of a subsequent speech act. The rules of the game are roughly based on the Gricean maxims of co-operation — i.e., agents are forbidden to put forward information they do not believe and are forbidden to ask anything they already believe; the Gricean maxim of relevance is determined by a so-called imbalance in the players’ belief and desire states. As in realistic conversational situations, it is assumed that the information needed to answer a question can be present in a distributed manner. Consequently, the structure of the dialogues may become rather complex, and may result in the generation of counter-questions and sub-dialogues. It will be shown that the structure and the coherence of conversational units do not necessarily have to be the product of a complex planning process or a speech act grammar, but can be based on elementary generation rules that take only into account the local context. As a result, the conversational game does not suffer from the same computational complexity as existing planning models for speech act generation. Although simple in its basic form, the framework enables us to produce abstract conversations with some properties that agree strikingly with dialogue properties found in Conversation Analysis.

Cavity quantum electrodynamics has been studied as a potential approach to modify free charge carrier generation in donor–acceptor heterojunctions because of the delocalization and controllable energy level properties of hybridized light–matter states known as polaritons. However, in many experimental systems, cavity coupling decreases charge separation. Here, we theoretically study the quantum dynamics of a coherent and dissipative donor–acceptor cavity system, to investigate the dynamical mechanism and further discover the conditions under which polaritons may enhance free charge carrier generation. We use open quantum system methods based on single-pulse pumping to find that polaritons have the potential to connect excitonic states and charge separated states, further enhancing free charge generation on an ultrafast timescale of several hundred femtoseconds. The mechanism involves polaritons with optimal energy levels that allow the exciton to overcome the high Coulomb barrier induced by electron–hole attraction. Moreover, we propose that a second-hybridization between a polariton state and dark states with similar energy enables the formation of the hybrid charge separated states that are optically active. These two mechanisms lead to a maximum of 50% enhancement of free charge carrier generation on a short timescale. However, our simulation reveals that on the longer timescale of picoseconds, internal conversion and cavity loss dominate and suppress free charge carrier generation, reproducing the experimental results. Thus, our work shows that polaritons can affect the charge separation mechanism and promote free charge carrier generation efficiency, but predominantly on a short timescale after photoexcitation.

Abstract Efficient devices for light harvesting and photon sensing are fundamental building blocks of basic energy science and many essential technologies. Recent efforts have turned to biomimicry to design the next generation of light-capturing devices, partially fueled by an appreciation of the fantastic efficiency of the initial stages of natural photosynthetic systems at capturing photons. In such systems extended excitonic states are thought to play a fundamental functional role, inducing cooperative coherent effects, such as superabsorption of light and supertransfer of photoexcitations. Inspired by this observation, we design an artificial light-harvesting and photodetection device that maximally harnesses cooperative effects to enhance efficiency. The design relies on separating absorption and transfer processes (energetically and spatially) in order to overcome the fundamental obstacle to exploiting cooperative effects to enhance light capture: the enhanced emission processes that accompany superabsorption. This engineered separation of processes greatly improves the efficiency and the scalability of the system.

Active matter, both synthetic and biological, demonstrates complex spatiotemporal self-organization and the emergence of collective behavior. A coherent rotational motion, the vortex phase, is of great interest because of its ability to orchestrate well-organized motion of self-propelled particles over large distances. However, its generation without geometrical confinement has been a challenge. Here, we show by experiments and computational modeling that concentrated magnetic rollers self-organize into multivortex states in an unconfined environment. We find that the neighboring vortices more likely occur with the opposite sense of rotation. Our studies provide insights into the mechanism for the emergence of coherent collective motion on the macroscale from the coupling between microscale rotation and translation of individual active elements. These results may stimulate design strategies for self-assembled dynamic materials and microrobotics.

AbstractUnderstanding and controlling the nonlinear optical properties and coherent quantum evolution of complex multilevel systems out of equilibrium is essential for the new semiconductor device generation. In this work, we investigate the nonlinear system properties of an unbiased quantum cascade structure by performing two-dimensional THz spectroscopy. We study the time-resolved coherent quantum evolution after it is driven far from equilibrium by strong THz pulses and demonstrate the existence of multiple nonlinear signals originating from the engineered subbands and find the lifetimes of those states to be in the order of 4–8 ps. Moreover, we observe a coherent population exchange among the first four intersubband levels during the relaxation, which have been confirmed with our simulation. We model the experimental results with a time-resolved density matrix based on the master equation in Lindblad form, including both coherent and incoherent transitions between all density matrix elements. This allows us to replicate qualitatively the experimental observations and provides access to their microscopic origin.

In this work, we consider an environment formed by incoherent photons as a resource for controlling open quantum systems via an incoherent control. We exploit a coherent control in the Hamiltonian and an incoherent control in the dissipator which induces the time-dependent decoherence rates γk(t) (via time-dependent spectral density of incoherent photons) for generation of single-qubit gates for a two-level open quantum system which evolves according to the Gorini–Kossakowski–Sudarshan–Lindblad (GKSL) master equation with time-dependent coefficients determined by these coherent and incoherent controls. The control problem is formulated as minimization of the objective functional, which is the sum of Hilbert-Schmidt norms between four fixed basis states evolved under the GKSL master equation with controls and the same four states evolved under the ideal gate transformation. The exact expression for the gradient of the objective functional with respect to piecewise constant controls is obtained. Subsequent optimization is performed using a gradient type algorithm with an adaptive step size that leads to oscillating behaviour of the gradient norm vs. iterations. Optimal trajectories in the Bloch ball for various initial states are computed. A relation of quantum gate generation with optimization on complex Stiefel manifolds is discussed. We develop methodology and apply it here for unitary gates as a testing example. The next step is to apply the method for generation of non-unitary processes and to multi-level quantum systems.

We studied the high-harmonic generation (HHG) of a two-level-system (TLS) driven by an intense monochromatic phase-locked laser based on complex spectral analysis with the Floquet method. In contrast with phenomenological approaches, this analysis deals with the whole process as a coherent quantum process based on microscopic dynamics. We have obtained the time-frequency resolved spectrum of spontaneous HHG single-photon emission from an excited TLS driven by a laser field. Characteristic spectral features of the HHG, such as the plateau and cutoff, are reproduced by the present model. Because the emitted high-harmonic photon is represented as a superposition of different frequencies, the Fano profile appears in the long-time spectrum as a result of the quantum interference of the emitted photon. We reveal that the condition of the quantum interference depends on the initial phase of the driving laser field. We have also clarified that the change in spectral features from the short-time regime to the long-time regime is attributed to the interference between the interference from the Floquet resonance states and the dressed radiation field.

Phonons, and in particular surface acoustic wave phonons, have been proposed as a means to coherently couple distant solid-state quantum systems. Individual phonons in a resonant structure can be controlled and detected by superconducting qubits, enabling the coherent generation and measurement of complex stationary phonon states. We report the deterministic emission and capture of itinerant surface acoustic wave phonons, enabling the quantum entanglement of two superconducting qubits. Using a 2-millimeter-long acoustic quantum communication channel, equivalent to a 500-nanosecond delay line, we demonstrate the emission and recapture of a phonon by one superconducting qubit, quantum state transfer between two superconducting qubits with a 67% efficiency, and, by partial transfer of a phonon, generation of an entangled Bell pair with a fidelity of 84%.

Layered transition metal dichalcogenides (TMDCs) host a variety of strongly bound exciton complexes that control the optical properties in these materials. Apart from spin and valley, layer index provides an additional degree of freedom in a few-layer-thick lm. While in the 1H monolayer TMD inversion symmetry is broken, and the reflection symmetry is maintained but, in the bilayer, it is reversed. Trions are excitonic species with a positive or negative charge, and thus, unlike neutral excitons, the flow of trions can generate a net detectable charge current. Trions under favourable doping conditions can be created in a coherent manner using resonant excitation. The neutral biexciton (bound state of two excitons) can assemble further to create a charged state with another electron or hole. Generally, in W-based TMDs these ve-particle quinton states dominate the population density and this can also be engineered to produce photocurrent at cryogenic temperature. In the firrst work, we show that in a few-layer TMDC lm, the wave functions of the conduction and valence-band-edge states contributing to the K(K0) valley are spatially con ned in the alternate layers - giving rise to direct (quasi-)intralayer bright exciton and lower-energy interlayer dark excitons. Depending on the spin and valley con figuration, the bright-exciton state is further found to be a coherent superposition of two layer- induced states, one (E type) distributed in the even layers and the other (O type) in the odd layers. The intralayer nature of the bright exciton manifests as a relatively weak dependence of the exciton binding energy on the thickness of the few-layer lm, and the binding energy is maintained up to 50 meV in the bulk limit - which is an order of magnitude higher than conventional semiconductors. Fast Stokes energy transfer from the intralayer bright state to the interlayer dark states provides a clear signature in the layer-dependent broadening of the photoluminescence peak and plays a key role in the suppression of the photoluminescence intensity observed in TMDCs with thickness beyond a monolayer. In the second work, we show that bilayer WS2 exhibits a quantum con ned Stark effect (QCSE) that is linear with the applied out-of-plane electric field, in contrast to a quadratic one for a monolayer because of the contrasting symmetries between monolayer and bilayer. The interplay between the unique layer degree of freedom in the bilayer and the field-driven partial interconversion between intralayer and interlayer excitons generates a giant tunability of the exciton oscillator strength. This makes bilayer WS2 a promising candidate for an atomically thin, tuneable electro-absorption modulator at the exciton resonance, particularly when stacked on top of a graphene layer that provides an ultrafast nonradiative relaxation channel. By tweaking the biasing confi guration, we further show that the excitonic response can be largely tuned through electrostatic doping, by efficiently transferring the oscillator strength from neutral to charged exciton. In the third and fourth work, we demonstrate interlayer charge transport from top few-layer graphene to bottom monolayer graphene, mediated by a coherently formed trion state using a few-layer graphene/monolayer WS2/monolayer graphene vertical het- erojunction. This is achieved by using a resonant excitation and varying the sample temperature. The resulting change in the WS2 bandgap allows us to scan the excitation around the exciton-trion spectral overlap with high spectral resolution. By correlating the vertical photocurrent and in situ photoluminescence features at the heterojunction as a function of the spectral position of the excitation, we show that (1) trions are anoma- lously stable at the junction even up to 463 K due to enhanced doping, and (2) the photocurrent results from the ultrafast formation of a trion through exciton-trion coher- ent coupling, followed by its fast interlayer transport. Further, the resonant photocurrent thus generated can be effectively controlled by a back gate voltage applied through the incomplete screening of the bottom monolayer graphene, and the photocurrent strongly correlates with the gate dependent trion intensity, while the non-resonant photocurrent exhibits only a weak gate dependence. We estimate a sub-100 fs switching time of the device. In the final work, we have used the pulsed laser excitation to create the quinton states in monolayer WS2 while resonantly exciting the exciton and trion states at low temperature. Strong light absorption by the charged biexciton under spectral resonance, coupled with its charged nature, makes it intriguing for photodetection - an area that is hitherto unexplored. Using the high built-in vertical electric eld in an asymmetrically designed few-layer graphene encapsulated 1L-WS2 heterostructure, here we report, for the rst time, a large, highly nonlinear photocurrent arising from the strong absorption by two charged biexciton species under zero external bias (self-powered mode). Time- resolved measurement reveals that the photoresponse is ultra-fast, on the order of sub-5 ps. By using single- and two-color photoluminescence excitation spectroscopy, we show that the two biexcitonic peaks originate from bright-dark and bright-bright exciton-trion combinations. The possibility of electrical manipulation and detection of a charged exciton (trion) before its radiative recombination makes it promising for excitonic devices. The demon- stration of coherent formation, high stabilization, vertical transportation, and electrical detection of trions marks a step toward room-temperature trionics. Following the same the ve-particle charged quinton can also be efficiently generated and electrically de- tected. They can be used in electrical detection of constituting bright and dark states and quantum manipulation of the coupled spin-valley physics. Such innate nonlinearity in the photocurrent due to its biexcitonic origin, coupled with the ultra-fast response due to swift inter-layer charge transfer exempli fies the promise of manipulating many- body effects in monolayers. Also, the findings are prospective toward highly tunable, atomically thin, compact, and light on chip, re-confi gurable components and promising for several applications such as higher harmonics generation of the modulating signal, receiver design in microwave photonics and visible light communication, square-law cir- cuits, and also in nonlinear next generation optoelectronics.