Phonon Environment Research Articles

Optimal tree tensor network operators for tensor network simulations: Applications to open quantum systems.

Tree tensor network states (TTNS) decompose the system wavefunction to the product of low-rank tensors based on the tree topology, serving as the foundation of the multi-layer multi-configuration time-dependent Hartree method. In this work, we present an algorithm that automatically constructs the optimal and exact tree tensor network operators (TTNO) for any sum-of-product symbolic quantum operator. The construction is based on the minimum vertex cover of a bipartite graph. With the optimal TTNO, we simulate open quantum systems, such as spin relaxation dynamics in the spin-boson model and charge transport in molecular junctions. In these simulations, the environment is treated as discrete modes and its wavefunction is evolved on equal footing with the system. We employ the Cole-Davidson spectral density to model the glassy phonon environment and incorporate temperature effects via thermo-field dynamics. Our results show that the computational cost scales linearly with the number of discretized modes, demonstrating the efficiency of our approach.

The Rotating Excitons in 2D Materials: Valley Zeeman Effect and Chirality

The rotational dynamics of the intralayer and interlayer excitons with their inherent momenta of inertia in the monolayer and bilayer transition metal dichalcogenides, respectively, where the new chirality of exciton is endowed by the rotational angular momentum, namely, the formations of left‐ and right‐handed excitons at the +K and −K valleys, respectively, is proposed. It is found that angular momenta exchange between excitons and its surrounding phononic bath result in the large fluctuation of the effective g‐factor and the asymmetry of valley Zeeman splitting observed in most recently experiments, both of which sensitively depend on the magnetic moments provided by the phononic environment. This rotating exciton model not only proposes a new controllable knob in valleytronics, but opens the door to explore the angular momentum exchange of the chiral quasiparticles with the many‐body environment.

A quantum trajectory picture of single photon absorption and energy transport in photosystem II.

We use quantum trajectory theory to study the dynamics of the first step in photosynthesis for a single photon interacting with photosystem II (PSII). By considering individual trajectories we are able to look beyond the ensemble average dynamics to compute the PSII system evolution conditioned upon individual photon counting measurements. Measurements of the transmitted photon beam strongly affects the system state, since detection of an outgoing photon confirms that the PSII must be in the electronic ground state, while a null measurement implies it is in an excited electronic state. We show that under ideal conditions, observing the null result transforms a state with a low excited state population to a state with nearly all population contained in the excited states. We study the PSII dynamics conditioned on such photon counting for both a pure excitonic model of PSII and a more realistic model with exciton-phonon coupling to a dissipative phononic environment. In the absence of such coupling, we show that the measured fluorescence rates show oscillations constituting a photon-counting witness of excitonic coherence. Excitonic coupling to the phonon environment has a strong effect on the observed rates of fluorescence, damping the oscillations. Addition of non-radiative decay and incoherent transitions to radical pair states in the reaction center to the phononic model allows extraction of a quantum efficiency of 92.5% from the long-time evolution, consistent with bulk experimental measurements.

Relaxation dynamics of nonresonant excitation transfer processes assisted by coherent phonon environment

In this study, the steepest-entropy-ascent quantum thermodynamics (SEAQT) framework is used to investigate the excitation transfer (ET) dynamics of two-level nanosystems (TLSs), focusing on non-resonant processes that involve a dynamic local phonon system. In contrast to other methods based on Markovian or non-Markovian quantum master equations, SEAQT analysis always guarantees the positivity of the density operators, thus enabling the discussion of both transient and long-term dynamics of nanosystems. The findings of this study demonstrate that the relaxation time of coherent phonons, relative to the Rabi oscillation period in two TLSs, significantly affects the relaxation process of non-resonant ETs. Moreover, the degree of mutual synchronization between ET dynamics of TLSs and local (coherent) phonons can either prolong or shorten the decoherence time, presenting a way to control the coherence in nanosystems and stimulate quantum device applications.

Impact of the phonon environment on the nonlinear quantum-dot–cavity QED: Path-integral approach

Impact of the phonon environment on the nonlinear quantum-dot–cavity QED: Path-integral approach

Theory of all-coupling angulon for molecules rotating in many-body environment.

The formation of angulon, stemming from the rotor (molecule or impurity), rotating in the quantum many-body field, adds a new member to the quasi-particles' family and has aroused intense interest in multiple research fields. However, the analysis of the coupling strength between the rotor and its hosting environment remains a challenging task, both in theory and experiment. Here, we develop the all-coupling theory of the angulon by introducing a unitary transformation, where the renormalization of the rotational constants for different molecules in the helium nanodroplets is reproduced, getting excellent agreement with the experimental data collected during the past decades. Moreover, the strength of molecule-helium coupling and the effective radius of the solvation shell co-rotating along with the molecular rotor could be estimated qualitatively. This model not only provides significant enlightenment for analyzing the rotational spectroscopy of molecules in the phononic environment, but also provides a new method to study the transfer of the phonon angular momentum in the angulon frame.

Phonon coupling versus pure dephasing in the photon statistics of cooperative emitters

Realizing scalable quantum networks requires a meticulous level of understanding and mitigating the deleterious effects of decoherence. Many quantum device platforms feature multiple decoherence mechanisms, often with a dominant mechanism seemingly fully masking others. In this paper, we show how access to weaker dephasing mechanisms can nevertheless be obtained for optically active qubits by performing two-photon coincidence measurements. To this end we theoretically investigate the impact of different decoherence mechanisms on cooperatively emitting quantum dots. Focusing on the typically dominant deformation-potential coupling to longitudinal acoustic phonons and typically much less severe additional sources of pure dephasing, we employ a numerically exact method to show that these mechanisms lead to very different two-photon coincidence signals. Moreover, surprisingly, the impact of the strongly coupled phonon environment is weak and leads to long-lived coherences. We trace this back to the superohmic nature of the deformation-potential coupling causing interemitter coherences to converge to a nonzero value on a short timescale, whereas pure dephasing contributions cause a complete decay of coherence over longer times. Our approach provides a practical means of investigating decoherence processes on different timescales in solid-state emitters, and thus contributes to understanding and possibly eliminating their detrimental influences.

The impact of stacking and phonon environment on energy transfer in organic chromophores: computational insights

Energy transfer in organic materials is extensively studied due to many applications in optoelectronics.

Real-Time Observation of Charge-Spin Cooperative Dynamics Driven by a Nonequilibrium Phonon Environment.

We report on experimental observations of charge-spin cooperative dynamics of two-electron states in a GaAs double quantum dot located in a nonequilibrium phonon environment. When the phonon energy exceeds the lowest excitation energy in the quantum dot, the spin-flip rate of a single electron strongly enhances. In addition, originated from the spatial gradient of phonon density between the dots, the parallel spin states become more probable than the antiparallel ones. These results indicate that spin is essential for further demonstrations of single-electron thermodynamic systems driven by phonons, which will greatly contribute to understanding of the fundamental physics of thermoelectric devices.

Coupling function from bath density of states

Modelling of an open quantum system requires knowledge of parameters that specify how it couples to its environment. However, beyond relaxation rates, realistic parameters for specific environments and materials are rarely known. Here we present a method of inferring the coupling between a generic system and its bosonic (e.g., phononic) environment from the experimentally measurable density of states (DOS). With it we confirm that the DOS of the well-known Debye model for three-dimensional solids is physically equivalent to choosing an Ohmic bath. We further match a real phonon DOS to a series of Lorentzian coupling functions, allowing us to determine coupling parameters for gold, yttrium iron garnet (YIG) and iron as examples. The results illustrate how to obtain material-specific dynamical properties, such as memory kernels. The proposed method opens the door to more accurate modelling of relaxation dynamics, for example for phonon-dominated spin damping in magnetic materials.

Local Phonon Environment as a Design Element for Long-Lived Excitonic Coherence: Dithia-anthracenophane Revisited

The purpose of this study is to investigate the role of a structured immediate phonon environment in determining the exciton dynamics and the possibility of using it as an optimal design element. Through the case study of dithia-anthracenophane, a bichromophore using the Hierarchical Equations Of Motion formalism, we show that the experimentally observed coherent exciton dynamics can be reproduced only by considering the actual structure of the phonon environment. While the slow dephasing of quantum coherence in dithia-anthracenophane can be attributed to strong vibronic coupling to high-frequency modes, vibronic quenching is the source of long oscillation periods in population transfer. This study sheds light on the crucial role of the structure of the immediate phonon environment in determining the exciton dynamics. We conclude by proposing some design principles for sustaining long-lived coherence in molecular systems.

Phonon-assisted entanglement between two quantum dots coupled to a plasmonic nanocavity

We theoretically investigate the influence of a phonon bath on entangled generation between two semiconductor quantum dots coupled to a plasmonic nanocavity and coherently driven by an external optical field. Our study reveals that phonons could be useful in a certain range of system parameters where a subradian state preparation is possible. We point out that this behavior is due to the fact that phonon environment modify the radiative properties of the two-qubit inducing different decay rates between the collective states of the system. The influence of the factors characteristic of quantum dot systems and plasmonic nanocavity such as energy mismatch in different dots, different plasmonic cavity losses as well as coupling to phonons is analyzed. The entanglement can be controlled via different external parameters such as the cavity detuning, the Rabi frequency of the driving field and the resonance frequency of the QDs.

Molecule-photon interactions in phononic environments

Molecules constitute compact hybrid quantum optical systems that can interface photons, electronic degrees of freedom, localized mechanical vibrations and phonons. In particular, the strong vibronic interaction between electrons and nuclear motion in a molecule resembles the optomechanical radiation pressure Hamiltonian. While molecular vibrations are often in the ground state even at elevated temperatures, one still needs to get a handle on decoherence channels associated with phonons before an efficient quantum optical network based on opto-vibrational interactions in solid-state molecular systems could be realized. As a step towards a better understanding of decoherence in phononic environments, we take here an open quantum system approach to the non-equilibrium dynamics of guest molecules embedded in a crystal, identifying regimes of Markovian versus non-Markovian vibrational relaxation. A stochastic treatment based on quantum Langevin equations predicts collective vibron-vibron dynamics that resembles processes of sub- and superradiance for radiative transitions. This in turn leads to the possibility of decoupling intramolecular vibrations from the phononic bath, allowing for enhanced coherence times of collective vibrations. For molecular polaritonics in strongly confined geometries, we also show that the imprint of opto-vibrational couplings onto the emerging output field results in effective polariton cross-talk rates for finite bath occupancies.

Generalized input-output method to quantum transport junctions. I. General formulation

In this work, we put forward a generalized input-output method (GIOM) for studying charge transport in molecular junctions accounting for strong electron-vibration interactions and including electronic and phononic environments. The method radically expands the scope of the input-output theory, which was originally proposed to treat quantum optic problems. Based on the GIOM we derive a Langevin-type equation of motion for molecular operators, which posses a great generality and accuracy, and permits the derivation of a stationary charge current expression involving only two types of transfer rates. Furthermore, we devise the so-called "Polaron Transport in Electronic Resonance" (PoTER) approximation, which allows to feasibly simulate electron dynamics in generic tight-binding models with strong electron-vibration interactions. For short chains, the charge current reduces to known limits and reasonably agrees with exact numerical simulations. For extended junctions the current displays a turnover from phonon-assisted to phonon-suppressed transport. Nevertheless, the onset of ohmic behavior requires extensions beyond the PoTER approximation. As an additional application, we consider a cavity-coupled molecule junction. Here we identify a cavity-induced suppression of charge current in the single-site case, and observe signatures of polariton formation in the current-voltage characteristics in the strong light-matter coupling regime. A critical understanding gained from the GIOM-PoTER scheme is that the single-site vibrationally-coupled model is deceptively simpler, and amenable to approximations than multi-site models. Therefore, benchmarking of methods should not be concluded with the single-site case. The work manifests that the input-output framework, which is normally employed in quantum optics, can serve as a powerful and feasible tool in the realm of electron transport junctions.

Quantum control of excitons for reversible heat transfer

Lasers, photovoltaics, and thermoelectrically-pumped light emitting diodes are thermodynamic machines which use excitons (electron-hole pairs) as the working medium. The heat transfers in such devices are highly irreversible, leading to low efficiencies. Here we predict that reversible heat transfers between a quantum-dot exciton and its phonon environment can be induced by laser pulses. We calculate the heat transfer when a quantum-dot exciton is driven by a chirped laser pulse. The reversibility of this heat transfer is quantified by the efficiency of a heat engine in which it forms the hot stroke, which we predict to reach 95% of the Carnot limit. This performance is achieved by using the time-dependent laser-dressing of the exciton to control the heat current and exciton temperature. We conclude that reversible heat transfers can be achieved in excitonic thermal machines, allowing substantial improvements in their efficiency.

All-optical generation and ultrafast tuning of non-linear spin Hall current

Spin Hall effect, one of the cornerstones in spintronics refers to the emergence of an imbalance in the spin density transverse to a charge flow in a sample under voltage bias. This study points to a novel way for an ultrafast generation and tuning of a unidirectional nonlinear spin Hall current by means of subpicosecond laser pulses of optical vortices. When interacting with matter, the optical orbital angular momentum (OAM) carried by the vortex and quantified by its topological charge is transferred to the charge carriers. The residual spin-orbital coupling in the sample together with confinement effects allow exploiting the absorbed optical OAM for spatio-temporally controlling the spin channels. Both the non-linear spin Hall current and the dynamical spin Hall angle increase for a higher optical topological charge. The reason is the transfer of a higher amount of OAM and the enhancement of the effective spin-orbit interaction strength. No bias voltage is needed. We demonstrate that the spin Hall current can be all-optically generated in an open circuit geometry for ring-structured samples. These results follow from a full-fledged propagation of the spin-dependent quantum dynamics on a time-space grid coupled to the phononic environment. The findings point to a versatile and controllable tool for the ultrafast generation of spin accumulations with a variety of applications such as a source for ultrafast spin transfer torque and charge and spin current pulse emitter.

New One‐Dimensional Material Nb2Se9: Theoretical Prediction of Indirect to Direct Band Gap Transition due to Dimensional Reduction

Layered two‐dimensional (2D) transition metal dichalcogenides (TMDCs) often form 2D sheets and some of these show an indirect to direct band gap transition as the number of layers decreases from that of the bulk structure. Recently, a new one‐dimensional (1D) material of Nb2Se9 is successfully prepared by solid state reaction. This material is semiconducting and composed of periodically stacked single‐chain atomic crystals (SCAC) where the SCACs form inorganic bulk crystals due to strong bonds within the chain but with weak inter‐chain interactions. To determine the potential applications of our newly developed 1D nanowire, theoretical prediction of its material properties is performed. As a first step, the band structures of bundles of Nb2Se9 SCACs, which are composed of 1–7 single chains, are calculated by using density functional theory. Unlike the bulk structure of Nb2Se9, the chain bundles composed of up to 21 single SCACs would have a direct band gap. Accordingly, it is expected that an Nb2Se9 bundle SCAC with a diameter of 3.6 nm can cause the electronic transition without being disturbed by the phononic environment due to the direct band gap, and can therefore be used in photoluminescence applications.

Tensor network simulation of polaron-polaritons in organic microcavities

In the regime of strong coupling between molecular excitons and confined optical modes, the intramolecular degrees of freedom are profoundly affected, leading to a reduced vibrational dressing of polaritons compared to bare electronically excited states. However, existing models only describe a single vibrational mode in each molecule, while actual molecules possess a large number of vibrational degrees of freedom and additionally interact with a continuous bath of phononic modes in the host medium in typical experiments. In this work, we investigate a small ensemble of molecules with an arbitrary number of vibrational degrees of freedom under strong coupling to a microcavity mode. We demonstrate that reduced vibrational dressing is still present in this case, and show that the influence of the phononic environment on most electronic and photonic observables in the lowest excited state can be predicted from just two collective parameters of the vibrational modes. Besides, we explore vibrational features that can be addressed exclusively by our extended model and could be experimentally tested. Our findings indicate that vibronic coupling is more efficiently suppressed for environments characterized by low-frequency (sub-Ohmic) modes.

Entanglement of a laser-driven pair of two-level qubits via its phonon environment

The entanglement dynamics of a laser-pumped two-level quantum dot pair is investigated in the steady-state. The closely spaced two-level emitters, embedded in a semiconductor substrate, interact with both the environmental vacuum modes of the electromagnetic field reservoir as well as with the lattice vibrational phonon thermostat. We have found that the entanglement among the pair's components is substantially enhanced due to presence of the phonon subsystem. The reason is phonon induced decay among the symmetrical and antisymmetrical two-qubit collective states and, consequently, the population of the latter one. This also means that through thermal phonon bath engineering one can access the subradiant two-particle cooperative state.

Studying light-harvesting models with superconducting circuits

The process of photosynthesis, the main source of energy in the living world, converts sunlight into chemical energy. The high efficiency of this process is believed to be enabled by an interplay between the quantum nature of molecular structures in photosynthetic complexes and their interaction with the environment. Investigating these effects in biological samples is challenging due to their complex and disordered structure. Here we experimentally demonstrate a technique for studying photosynthetic models based on superconducting quantum circuits, which complements existing experimental, theoretical, and computational approaches. We demonstrate a high degree of freedom in design and experimental control of our approach based on a simplified three-site model of a pigment protein complex with realistic parameters scaled down in energy by a factor of 105. We show that the excitation transport between quantum-coherent sites disordered in energy can be enabled through the interaction with environmental noise. We also show that the efficiency of the process is maximized for structured noise resembling intramolecular phononic environments found in photosynthetic complexes.