Simulation of emission spectra of transition-metal dichalcogenide monolayers with the multimode Brownian oscillator model

The multimode Brownian oscillator model is employed to simulate the emission spectra of transition metal dichalcogenide monolayers. Good agreement is obtained between measured and simulated photoluminescence spectra of WSe2, WS2, MoSe2 and MoS2 at various temperatures. The Huang-Rhys factor extracted from the model can be associated with that from the modified semi-empirical Varshni equation at high temperatures. Individual mechanisms leading to the unique temperature-dependent emission spectra of those TMDs are validated by the MBO fitting, while it is in turn confirmed that the MBO analysis is an effective method for studying the optical properties of TMD monolayers. Parameters extractd from the MBO fitting can be used to explore exciton-photon-phonon dynamics of TMDs in a more comprehensive model

Photon-assisted Landau-Zener transitions in a periodically driven Rabi dimer coupled to a dissipative mode

We investigate multiple photon-assisted Landau-Zener (LZ) transitions in a hybrid circuit quantum electrodynamics device in which each of two interacting transmission-line resonators is coupled to a qubit, and the qubits are driven by periodic driving fields and also coupled to a common phonon mode. The quantum state of the entire composite system is modeled using the multi-$\rm D_2$ Ansatz in combination with the time-dependent Dirac-Frenkel variational principle. Applying a sinusoidal driving field to one of the qubits, this device is an ideal platform to study the photon-assisted LZ transitions by comparing the dynamics of the two qubits. A series of interfering photon-assisted LZ transitions take place if the photon frequency is much smaller than the driving amplitude. Once the two energy scales are comparable, independent LZ transitions arise and a transition pathway is revealed using an energy diagram. It is found that both adiabatic and nonadiabatic transitions are involved in the dynamics. Used to model environmental effects on the LZ transitions, the common phonon mode coupled to the qubits allows for more available states to facilitate the LZ transitions. An analytical formula is obtained to estimate the short-time phonon population and produces results in reasonable agreement with numerical calculations. Equipped with the knowledge of the photon-assisted LZ transitions in the system, we can precisely manipulate the qubit state and successfully generate the qubit dynamics with a square-wave pattern by applying driving fields to both qubits, opening up new venues to manipulate the states of qubits and photons in quantum information devices and quantum computer

Optical-Cavity Manipulation Strategies of Conical Intersections Mediated Singlet Fission Systems

We offer a theoretical perspective on simulation and engineering of polaritonic conical-intersection-driven singlet-fission (SF) materials. Using rubrene as an example and applying the numerically accurate Davydov-Ansatz methodology, we derive dynamic and spectroscopic responses of the system and demonstrate key mechanisms capable of SF manipulation, viz. cavity-induced enhancement/weakening/suppression of SF, population localization on the singlet state via engineering of the cavity-mode excitation, polaron/polariton decoupling, collective enhancement of SF. We outline unsolved problems and challenges in the field, and share our views on the development of the future lines of research. We emphasize the significance of careful modeling of cascades of polaritonic conical intersections in high excitation manifolds and envisage that collective geometric phase effects may remarkably affect the SF dynamics and yield. We argue that microscopic interpretation of the main regulatory mechanisms of the polaritonic conical-intersection-driven SF can substantially deepen our understanding of this process, thereby providing novel ideas and solutions for improving conversion efficiency in photovoltaics.Comment: 14 pages, 6 figure

A Deep‐Learning Approach to the Dynamics of Landau–Zenner Transitions

Traditional approaches to the dynamics of the open quantum systems with high precision are often resource intensive. How to improve computation accuracy and efficiency for target systems is an extremely difficult challenge. In this work, combining unsupervised and supervised learning algorithms, a deep-learning approach is introduced to simulate and predict Landau–Zenner dynamics. Data obtained from multiple Davydov (Formula presented.) Ansatz with a low multiplicity of four are used for training, while the data from the trial state with a high multiplicity of ten are adopted as target data to assess the accuracy of prediction. After proper training, our method can successfully predict and simulate Landau–Zenner dynamics using only random noise and two adjustable model parameters. Compared to the high-precision dynamics data from multiple Davydov (Formula presented.) Ansatz with a multiplicity of ten, the error rate falls below 0.6%.Ministry of Education (MOE)Accepted versionThe authors gratefully acknowledge the support of the Singapore Ministry of Education Academic Research Fund (Grant Nos. 2018-T1-002-175 and 2020-T1-002- 075)). K. Sun would also like to thank the Natural Science Foundation of Zhejiang Province (Grant No. LY18A040005) for partial support. L.L. Gao acknowledges the support of the Graduate Scientific Research Foundation of Hangzhou Dianzi University

Quantifying non-Markovianity for a chromophore-qubit pair in a super-Ohmic bath

An approach based on a non-Markovian time-convolutionless polaron master equation is used to probe the quantum dynamics of a chromophore-qubit in a super-Ohmic bath. Utilizing a measure of non-Markovianity based on dynamical fixed points, we study the effects of the environment temperature and the coupling strength on the non-Markovian behavior of the chromophore in a super-Ohmic bath. It is found that an increase in the temperature results in a reduction in the backflow information from the environment to the chromophore, and therefore, a suppression of non-Markovianity. In the weak coupling regime, increasing coupling strength will enhance the non- Markovianity, while the effect is reversed in the strong coupling regime.Comment: 10 pages, 9 figure

Exciton Dynamics and Time-Resolved Fluorescence in Nanocavity-Integrated Monolayers of Transition-Metal Dichalcogenides

We have developed an ab-initio-based fully-quantum numerically-accurate methodology for the simulation of the exciton dynamics and time- and frequency-resolved fluorescence spectra of the cavity-controlled two-dimensional materials at finite temperature and applied this methodology to the single-layer WSe2 system. This allowed us to establish dynamical and spectroscopic signatures of the polaronic and polaritonic effects as well as uncover their characteristic timescales in the relevant range of temperatures

Excitonic energy transfer in light-harvesting complexes in purple bacteria

Two distinct approaches, the Frenkel-Dirac time-dependent variation and the Haken-Strobl model, are adopted to study energy transfer dynamics in single-ring and double-ring light-harvesting systems in purple bacteria. It is found that inclusion of long-range dipolar interactions in the two methods results in significant increases in intra- or inter-ring exciton transfer efficiency. The dependence of exciton transfer efficiency on trapping positions on single rings of LH2 (B850) and LH1 is similar to that in toy models with nearest-neighbor coupling only. However, owing to the symmetry breaking caused by the dimerization of BChls and dipolar couplings, such dependence has been largely suppressed. In the studies of coupled-ring systems, both methods reveal interesting role of dipolar interaction in increasing energy transfer efficiency by introducing multiple intra/inter-ring transfer paths. Importantly, the time scale (~4ps) of inter-ring exciton transfer obtained from polaron dynamics is in good agreement with previous studies. In a double-ring LH2 system, dipole-induced symmetry breaking leads to global minima and local minima of the average trapping time when there is a finite value of non-zero dephasing rate, suggesting that environment plays a role in preserving quantum coherent energy transfer. In contrast, dephasing comes into play only when the perfect cylindrical symmetry in the hypothetic system is broken. This study has revealed that dipolar interaction between chromophores may play an important part in the high energy transfer efficiency in the LH2 system and many other natural photosynthetic systems.Comment: 14 pages 9 figure