The Key Role of Non-Local Screening in the Environment-Insensitive Exciton Fine Structures of Transition-Metal Dichalcogenide Monolayers.

In this work, we present a comprehensive theoretical and computational investigation of exciton fine structures of WSe2-monolayers, one of the best-known two-dimensional (2D) transition-metal dichalcogenides (TMDs), in various dielectric-layered environments by solving the first-principles-based Bethe-Salpeter equation. While the physical and electronic properties of atomically thin nanomaterials are normally sensitive to the variation of the surrounding environment, our studies reveal that the influence of the dielectric environment on the exciton fine structures of TMD-MLs is surprisingly limited. We point out that the non-locality of Coulomb screening plays a key role in suppressing the dielectric environment factor and drastically shrinking the fine structure splittings between bright exciton (BX) states and various dark-exciton (DX) states of TMD-MLs. The intriguing non-locality of screening in 2D materials can be manifested by the measurable non-linear correlation between the BX-DX splittings and exciton-binding energies by varying the surrounding dielectric environments. The revealed environment-insensitive exciton fine structures of TMD-ML suggest the robustness of prospective dark-exciton-based optoelectronics against the inevitable variation of the inhomogeneous dielectric environment.

Precession-induced nonclassicality of the free induction decay of NV centers by a dynamical polarized nuclear spin bath.

The ongoing exploration of the ambiguous boundary between the quantum and the classical worlds has spurred substantial developments in quantum science and technology. Recently, the nonclassicality of dynamical processes has been proposed from a quantum-information-theoretic perspective, in terms of witnessing nonclassical correlations with Hamiltonian ensemble simulations. To acquire insights into the quantum-dynamical mechanism of the process nonclassicality, here we propose to investigate the nonclassicality of the electron spin free-induction-decay process associated with an NV-center. By controlling the nuclear spin precession dynamics via an external magnetic field and nuclear spin polarization, it is possible to manipulate the dynamical behavior of the electron spin, showing a transition between classicality and nonclassicality. We propose an explanation of the classicality-nonclassicality transition in terms of the nuclear spin precession axis orientation and dynamics. We have also performed a series of numerical simulations supporting our findings. Consequently, we can attribute the nonclassical trait of the electron spin dynamics to the behavior of nuclear spin precession dynamics.

Quantifying the nonclassicality of pure dephasing.

One of the central problems in quantum theory is to characterize, detect, and quantify quantumness in terms of classical strategies. Dephasing processes, caused by non-dissipative information exchange between quantum systems and environments, provides a natural platform for this purpose, as they control the quantum-to-classical transition. Recently, it has been shown that dephasing dynamics itself can exhibit (non)classical traits, depending on the nature of the system-environment correlations and the related (im)possibility to simulate these dynamics with Hamiltonian ensembles-the classical strategy. Here we establish the framework of detecting and quantifying the nonclassicality for pure dephasing dynamics. The uniqueness of the canonical representation of Hamiltonian ensembles is shown, and a constructive method to determine the latter is presented. We illustrate our method for qubit, qutrit, and qubit-pair pure dephasing and describe how to implement our approach with quantum process tomography experiments. Our work is readily applicable to present-day quantum experiments.

Distinctive Signatures of the Spin- and Momentum-Forbidden Dark Exciton States in the Photoluminescence of Strained WSe2 Monolayers under Thermalization.

With both spin and valley degrees of freedom, the low-lying excitonic spectra of photoexcited transition-metal dichalcogenide monolayers (TMDC-MLs) are featured by rich fine structures, comprising the intravalley bright exciton states as well as various intra- and intervalley dark ones. The latter states can be classified as those of the spin- and momentum-forbidden dark excitons according to the violated optical selection rules. Because of their optical invisibility, these two types of the dark states are in principle hardly observed and even distinguished in conventional spectroscopies although their impacts on the optical and dynamical properties of TMDC-MLs have been well noticed. In this Letter, we present a theoretical and computational investigation of the exciton fine structures and the temperature-dependent photoluminescence spectra of strained tungsten diselenide monolayers (WSe2-MLs) where the intravalley spin-forbidden dark exciton lies in the lowest exciton states and other momentum-forbidden states are in the higher energies that are tunable by external stress. The numerical computations are carried out by solving the Bethe-Salpeter equation for an exciton in a WSe2-ML under the stress-control in the tight-binding scheme established from the first principle computation in the density functional theory. According to the numerical computation and supportive model analysis, we reveal the distinctive signatures of the spin- and momentum-forbidden exciton states of strained WSe2-MLs in the temperature-dependent photoluminescences and present the guiding principle to infer the relative energetic locations of the two types of dark excitons.

Simulating Open Quantum Systems with Hamiltonian Ensembles and the Nonclassicality of the Dynamics.

The incoherent dynamical properties of open quantum systems are generically attributed to an ongoing correlation between the system and its environment. Here, we propose a novel way to assess the nature of these system-environment correlations by examining the system dynamics alone. Our approach is based on the possibility or impossibility to simulate open-system dynamics with Hamiltonian ensembles. As we show, such (im)possibility to simulate is closely linked to the system-environment correlations. We thus define the nonclassicality of open-system dynamics in terms of the nonexistence of a Hamiltonian-ensemble simulation. This classifies any nonunital open-system dynamics as nonclassical. We give examples for open-system dynamics that are unital and classical, as well as unital and nonclassical.

Erratum: General Non-Markovian Dynamics of Open Quantum Systems [Phys. Rev. Lett. 109, 170402 (2012)].

This corrects the article DOI: 10.1103/PhysRevLett.109.170402.

Non-Markovian Complexity in the Quantum-to-Classical Transition.

The quantum-to-classical transition is due to environment-induced decoherence, and it depicts how classical dynamics emerges from quantum systems. Previously, the quantum-to-classical transition has mainly been described with memory-less (Markovian) quantum processes. Here we study the complexity of the quantum-to-classical transition through general non-Markovian memory processes. That is, the influence of various reservoirs results in a given initial quantum state evolving into one of the following four scenarios: thermal state, thermal-like state, quantum steady state, or oscillating quantum nonstationary state. In the latter two scenarios, the system maintains partial or full quantum coherence due to the strong non-Markovian memory effect, so that in these cases, the quantum-to-classical transition never occurs. This unexpected new feature provides a new avenue for the development of future quantum technologies because the remaining quantum oscillations in steady states are decoherence-free.

Breakdown of Bose-Einstein distribution in photonic crystals.

In the last two decades, considerable advances have been made in the investigation of nano-photonics in photonic crystals. Previous theoretical investigations of photon dynamics were carried out at zero temperature. Here, we investigate micro/nano cavity photonics in photonic crystals at finite temperature. Due to photonic-band-gap-induced localized long-lived photon dynamics, we discover that cavity photons in photonic crystals do not obey Bose-Einstein statistical distribution. Within the photonic band gap and in the vicinity of the band edge, cavity photons combine the long-lived non-Markovain dynamics with thermal fluctuations together to form photon states that memorize the initial cavity state information. As a result, Bose-Einstein distribution is completely broken down in these regimes, even if the thermal energy is larger or much larger than the cavity detuning energy. In this investigation, a crossover phenomenon from equilibrium to nonequilibrium steady states is also revealed.

General non-Markovian dynamics of open quantum systems.

We present a general theory of non-Markovian dynamics for open systems of noninteracting fermions (bosons) linearly coupled to thermal environments of noninteracting fermions (bosons). We explore the non-Markovian dynamics by connecting the exact master equations with the nonequilibirum Green's functions. Environmental backactions are fully taken into account. The non-Markovian dynamics consists of nonexponential decays and dissipationless oscillations. Nonexponential decays are induced by the discontinuity in the imaginary part of the self-energy corrections. Dissipationless oscillations arise from band gaps or the finite band structure of spectral densities. The exact analytic solutions for various non-Markovian thermal environments show that non-Markovian dynamics can be largely understood from the environmental-modified spectra of open systems.