Coherent Dynamics Research Articles

Bell Test of Quantum Entanglement in Attosecond Photoionization

Attosecond physics enables the study of ultrafast coherent electron dynamics in matter upon photoexcitation and photoionization, revealing spectacular effects such as hole migration and coherent Auger dynamics in molecules. In the photoionization scenario, there has been a strong focus on probing the physical manifestations of internal quantum coherence within the individual parent ion and photoelectron systems. However, quantum correlations between these two subsystems emerging from attosecond photoionization events have thus far remained much more elusive. In this work, we design theoretically and model numerically a direct probe of quantum entanglement in attosecond photoionization in the form of a Bell test. We simulate from first principles a Bell test protocol for the case of noble gas atoms photoionized by ultrashort, circularly polarized infrared laser pulses in the strong-field regime predicting robust violation of the Bell inequality. This theoretical result paves the way for the direct observation of entanglement in the context of ultrafast photoionization of many-electron systems. Our work provides a novel perspective on attosecond physics directed toward the detection of quantum correlations between systems born during attosecond photoionization and unraveling the signatures of entanglement in ultrafast coherent molecular dynamics, including in the chemical decomposition pathways of molecular ions. Published by the American Physical Society 2024

Retraction Note: Quantum memory and coherence dynamics of two qubits interacting with a coherent cavity under intrinsic decoherence

Retraction Note: Quantum memory and coherence dynamics of two qubits interacting with a coherent cavity under intrinsic decoherence

Coherent dynamics in an optical quantum dot with phonons and photons

Genuine quantum-mechanical effects are readily observable in modern optomechanical systems comprising “classical” (bosonic) optical resonators. Unique features and advantages of optical two-level systems (qubits) for optomechanics, however, have not been so thoroughly explored. We experimentally demonstrate these advantages using charge-controlled InAs quantum dots (QDs) in surface-acoustic-wave resonators. We coherently control QD population dynamics using engineered optical pulses and mechanical motion, i.e., using both phonons and photons. As a first example, at moderate acoustic drive strengths, we demonstrate the potential of this technique to maximize fidelity in quantum microwave-to-optical transduction. Specifically, the scheme is tailored to enhance mechanically assisted photon scattering over the direct detuned photon scattering from the QD. Spectral analysis reveals distinct scattering channels related to Rayleigh scattering and luminescence in our pulsed excitation measurements, which lead to time-dependent scattering spectra. Quantum-mechanical calculations show good agreement with our experimental results, together providing a comprehensive description of excitation, scattering, and emission in a coupled QD-phonon system. These results highlight unique opportunities to expand the functionality of quantum optomechanical systems.

Control of coherent phonon dynamics in CoFeB/heavy metal heterojunction structures for future hybrid phononic and spintronic devices

Abstract The heterojunction structure of CoFeB/heavy metal has shown significant potential for spintronics, where both electrons and magnons potentially can serve as information carriers. However, another promising information carrier, coherent phonons, has not been fully explored for hybrid phononic and spintronic devices. In this study, we used time-resolved pump-probe spectroscopy to investigate the dynamic behavior of coherent phonons. We observed variations in reflectivity spectra, corresponding to changes in phonon frequency and relaxation times, with different thicknesses of the heavy metal and CoFeB layers. The experimental results demonstrated a decrease in coherent phonon oscillation frequency as the thickness of the CoFeB and heavy metal layers increased. These findings were further supported by first-principles calculations, which showed that the frequency of the optical modes is suppressed due to interface relaxation between the magnetic and heavy metal layers.

Signatures of coherent vibrational dynamics in ethylene carbonate.

Despite having practical applications in battery technology and serving as a model system for Fermi resonance coupling, ethylene carbonate (EC) receives little direct attention as a vibrational probe in nonlinear vibrational spectroscopy experiments. EC contains a Fermi resonance that is well-characterized in the linear spectrum, and the environmental sensitivity of its Fermi resonance peaks could make it a good molecular probe for two-dimensional infrared spectroscopy (2DIR) experiments. As a model system, we investigate the linear and 2DIR vibrational spectrum of the carbonyl stretching region of ethylene carbonate in tetrahydrofuran. The 2DIR spectrum reveals peak dynamics that evolve coherently. We characterize these dynamics in the context of Redfield theory and find evidence that EC dynamics proceed through coherent pathways, including singular coherence transfer pathways that have not been widely observed in other studies. We find that coherent contributions play a significant role in the observed dynamics of cross-peaks in the 2DIR spectrum, which must be accounted for to extract accurate measurements of early waiting time dynamics.

Community structure of tropics emerging from spatio-temporal variations in the Intertropical Convergence Zone dynamics

The Intertropical Convergence Zone (ITCZ) is a narrow tropical belt of deep convective clouds, intense precipitation, and monsoon circulations encircling the Earth. Complex interactions between the ITCZ and local geophysical dynamics result in high climate variability, making weather forecasting and prediction of extreme rainfall or drought events challenging. We unravel the complex spatio-temporal dynamics of the ITCZ and the resulting teleconnection patterns via a novel tropical climate classification achieved using complex network analysis and community detection. We reduce the high-dimensional complex ITCZ dynamics into a simple yet insightful community structure that classifies the tropics into seven regions representing distinct ITCZ dynamics. The two largest communities, encompassing landmasses over the Northern and Southern hemispheres, are associated with coherent seasonal ITCZ dynamics and have significant long-range connections. Temporal analysis of the community structure highlights that the tropical Pacific and Atlantic Oceans communities exhibit substantial variation on multidecadal scales. Further, these communities exhibit incoherent dynamics due to atmosphere-ocean interactions driven by equatorial and coastal oceanic upwelling.

Time Delays as Attosecond Probe of Interelectronic Coherence and Entanglement.

Attosecond chronoscopy enables the exploration of correlated electron dynamics in real time. One key observable of attosecond physics is the determination of "time zero" of photoionization, the time delay with which the wave packet of the ionized electron departs from the ionic core. This observable has become accessible by experimental advances in attosecond streaking and reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) techniques. In this Letter, we explore photoionization time delays by strong extreme ultraviolet fields beyond the linear-response limit. We identify novel signatures in time delays signifying strong coupling between atoms and light fields and the light-field dressing of the ion. As a prototypical case, we study the interelectronic coherence and entanglement in helium driven by a strong extreme ultraviolet field. By the numerical solution of the time-dependent Schrödinger equation in its full dimensionality, we show that the time delay of the photoionized electron allows one to monitor the ultrafast variations of coherence dynamics and entanglement in real time.

Attosecond Probing of Coherent Vibrational Dynamics in CBr4.

A coherent vibrational wavepacket is launched and manipulated in the symmetric stretch (a1) mode of CBr4, by impulsive stimulated Raman scattering (ISRS) from nonresonant 400 nm laser pump pulses with various peak intensities on the order of tens of 1012 W/cm2. Extreme ultraviolet (XUV) attosecond transient absorption spectroscopy (ATAS) records the wavepacket dynamics as temporal oscillations in XUV absorption energy at the bromine M4,5 3d3/2,5/2 edges around 70 eV. The results are augmented by nuclear time-dependent Schrödinger equation simulations. Slopes of the (Br 3d3/2,5/2)-110a1* core-excited state potential energy surface (PES) along the a1 mode are calculated to be -9.4 eV/Å from restricted open-shell Kohn-Sham calculations. Using analytical relations derived for the small-displacement limit and the calculated slopes of the core-excited state PES, a deeper insight into the vibrational dynamics is obtained by retrieving the experimental excursion amplitude of the vibrational wavepacket and the amount of population transferred to the vibrational first-excited state as a function of pump-pulse peak intensity. Experimentally, the results show that XUV ATAS is capable of resolving oscillations in the XUV absorption energy on the order of a few to tens of meV with tens of femtosecond time precision. This corresponds to change in C-Br bond length on the order of 10-4 to 10-3 Å. The results and the analytic relationships offer a clear physical picture, on multiple levels of understanding, of how the pump-pulse peak intensity controls the vibrational dynamics launched by nonresonant ISRS in the small-displacement limit.

Optimization of Low-Pressure Turbine Blade by Means of Fine Inspection of Loss Production Mechanisms

Abstract In this study, Proper Orthogonal Decomposition (POD) was applied to Large Eddy Simulations (LES) of two high-loaded low-pressure turbine cascades under unsteady inflow conditions to investigate entropy production within different parts of the blade passage. The terms for Turbulent Kinetic Energy (TKE) production, diffusion, and dissipation from the stagnation pressure transport equation were integrated across the computational domain. The POD-based method enables the decomposition of contributions from various coherent flow dynamics to TKE production and dissipation, such as the migration, bowing, tilting, and reorientation of incoming wake filaments, as well as the breakdown of streaky structures in the blade boundary layer and the formation of Von Karman vortices in the blade wake. This approach helps designers identify the dominant POD modes (i.e., turbulent flow structures) responsible for loss generation, understand their dynamics and locate where they primarily act. Using this optimization strategy, a new low-pressure turbine profile was designed. LES calculations on the optimized geometry showed that it is possible to design a higher-loaded profile with a lower global loss coefficient. The new loading distribution, characterized by stronger acceleration in the early part of the blade passage, results in reduced upstream wake migration losses and lower TKE production in the trailing edge wake zone due to early suction side boundary layer transition.

Exploiting automatic differentiation for quantum optimal control of driven dissipative two-level systems

In principle one can use Pontryagin's minimum principle to treat an optimal control problem and derive the gradient for the cost functional. However, for the driven spin-boson model studied here, the response of the system to the variation of the control is determined by the master equation and the equation of motion for the propagator of the coherent system dynamics. As a result, the application of Pontryagin's minimum principle is less straightforward. An alternative to this approach is the technique of automatic differentiation which in principle amounts to doing calculus on the fully discretized form of the optimal control problem. Automatic differentiation tools can be viewed as black boxes taking as input a program computing the cost functional and giving as output another program computing its gradient. First we derive for the polaron transformed Hamiltonian a Born-Markov master equation using the Bloch-Redfield formalism. By combining the latter with automatic differentiation we are able to implement Z-gate and coherent destruction of tunnelling with high fidelity. Optimization of a dissipative quantum gate poses a more complex numerical problem, since it should occur independent of the input state. To overcome this difficulty, we apply optimal control to the concept of resolvent of the master equation which is the generalisation of quantum unitary evolution operator in the case of dissipative dynamics.

Quantumness of electron transport in quantum dot devices through Leggett–Garg inequalities: A non-equilibrium Green’s function approach

Although coherent manipulation of electronic states can be achieved in quantum dot (QD) devices by harnessing nanofabrication tools, it is often hard to fathom the extent to which these nanoelectronic devices can behave quantum mechanically. Witnessing their nonclassical nature would thus remain of paramount importance in the emerging world of quantum technologies, since the coherent dynamics of electronic states plays there a crucial role. Against this backdrop, we resort to the general framework of Leggett-Garg inequalities (LGI) as it allows for distinguishing the classical and quantum transport through nanostructures by way of various two-time correlation functions. Using the local charge detection at two different time, we investigate here theoretically whether any quantum violation of the original LGI exists with varying device configurations and parameters under both Markovian and non-Markovian dynamics. Two-time correlators within LGI are derived in terms of the non-equilibrium Green’s functions (NEGFs) by exactly solving the quantum Langevin equations. The present study of non-Markovian dynamics of quantum systems interacting with reservoirs is significant for understanding the relaxation phenomenon in the ultrafast transient regime to especially mimic what happens to high-speed quantum devices. We can potentially capture the effect of finite reservoir correlation time by accounting for level-broadening at the electrodes along with non-Markovian memory effects. Furthermore, the large bias restriction is no longer imposed in our calculations so that we can safely consider a finite bias between the electronic reservoirs. Our approach is likely to open up new possibilities of witnessing the quantumness for other quantum many-body systems as well that are driven out of the equilibrium.

What can we learn from the experiment of electrostatic conveyor belt for excitons?

Motivated by the experiment of electrostatic conveyor belt for indirect excitons (Winbowet al2011Phys. Rev. Lett.106196806), we studied the exciton patterns for understanding the exciton dynamics. By analyzing the exciton diffusion, we found that the patterns mainly came from the photoluminescence of two kinds of excitons. The patterns near the laser spot came from the hot excitons which can be regarded as the classical particles. However, the patterns far from the laser spot come from the cooled or coherent excitons. Considering the finite lifetime of Bosonic excitons and of the interactions between them, we built a time-dependent nonlinear Schrödinger equation including the non-Hermitian dissipation to describe the coherent exciton dynamics. The real-time and imaginary-time evolutions were used alternately to solve the Schrödinger equation to simulate the exciton diffusion accompanied by the exciton cooling in the moving lattices. By calculating the escape probability, we obtained the transport distances of the coherent excitons in the conveyor, consistent with the experimental data. The cooling speed of excitons was found to be important in coherent exciton transport. Moreover, the plateau in the average transport distance cannot be explained by the dynamical localization-delocalization transition induced by the disorders.

Stochastic Schrödinger equation for hot-carrier dynamics in plasmonic systems

We present a multiscale method coupling the theory of open quantum systems with real-time ab initio treatment of electronic structure to study hot-carrier dynamics in photoexcited plasmonic systems. We combine the Markovian Stochastic Schrödinger equation with an ab initio GW coupled to the Bethe–Salpeter (BSE) equation description of the electronic degrees of freedom, interacting with a metallic nanoparticle modeled classically according to the polarizable continuum model. We apply this methodology to study the effect of relaxation (T1) and pure dephasing (T2) times on the hot-carrier dynamics in a system composed of a quantum portion described at GW/BSE level, i.e., a CHO fragment adsorbed on a vertex of a rhodium nanocube, and of the rest of the nanocube, treated classically, when irradiated with a 2.7 eV light pulse, inspired by the experimental results on plasmon-driven CO2 photoreduction. A net hole injection from rhodium to CHO is observed, with and without the classical portion of the nanocube. The nanocube effect is to enhance the generated charge population by two orders of magnitude. The nonradiative decay, via a relaxation time T1 based on the energy-gap law, produces a rapid decrease of the charge population. Results with T2 only show that a charge injection retarded with respect to the pulse, which is present in the coherent dynamics, disappears when coherence is erased.

Many-Body Models for Chirality-Induced Spin Selectivity in Electron Transfer.

We present the first microscopic model for the chirality-induced spin selectivity effect in electron-transfer, in which the internal degrees of freedom of the chiral bridge are explicitly included. By exactly solving this model on short chiral chains we demonstrate that a sizable spin polarization on the acceptor arises from the interplay of coherent and incoherent dynamics, with strong electron-electron correlations yielding many-body states on the bridge as crucial ingredients. Moreover, we include the coherent and incoherent dynamics induced by interactions with vibrational modes and show that they can play an important role in determining the long-time polarized state probed in experiments.

Quantum Walks and Correlated Dynamics in an Interacting Synthetic Rydberg Lattice.

Coherent dynamics of interacting quantum particles plays a central role in the study of strongly correlated quantum matter and the pursuit of quantum information processors. Here, we present the state space of interacting Rydberg atoms as a synthetic landscape on which to control and observe coherent and correlated dynamics. With full control of the coupling strengths and energy offsets between the pairs of sites in a nine-site synthetic lattice, we realize quantum walks, Bloch oscillations, and dynamics in an Escher-type "continuous staircase." In the interacting regime, we observe correlated quantum walks, Bloch oscillations, and confinement of particle pairs. Additionally, we simultaneously tilt our lattice both up and down to achieve coherent pair oscillations. When combined with a few straightforward upgrades, this work establishes synthetic Rydberg lattices of interacting atom arrays as a promising platform for programmable quantum many-body dynamics with access to features that are difficult to realize in real-space lattices.

Non-classical correlations and coherence in a two-dimensional electron gas under the influence of Rashba spin–orbit coupling

This investigation delves into the dynamics of quantum correlations and coherence within a two-dimensional electron gas (2DEG) system, taking into account the influence of Rashba spin–orbit coupling (SOC). We utilize metrics such as logarithmic negativity ([Formula: see text]), local quantum uncertainty (LQU ([Formula: see text])), and relative entropy of coherence ([Formula: see text]) to specifically assess these quantum resources among electron spins within non-interacting electron gases. Our study investigates how the separation distance (R) between electrons and the intensity of Rashba SOC ([Formula: see text]), impact the behavior of quantum properties within the 2DEG system. We find that specific strengths of Rashba SOC can effectively regulate quantum correlations and coherence within this system. Particularly significant is our observation that optimal quantum indicators emerge when electron proximity is minimized, underscoring the substantial influence of electron distance on quantum characteristics. Conversely, as electron separation increases, these quantum metrics diminish. Therefore, by adjusting the Rashba parameter, we can enhance the resilience of these quantum measurements against increasing electron separations, providing valuable insights into the potential for controlling and manipulating quantum behavior in similar 2DEG systems.

Measurement of coherent vibrational dynamics with X-ray Transient Absorption Spectroscopy simultaneously at the Carbon K- and Chlorine L2,3- edges

X-ray Transient Absorption Spectroscopy (XTAS) is a powerful probe for ultrafast molecular dynamics. The evolution of XTAS signal is controlled by the shapes of potential energy surfaces of the associated core-excited states, which are difficult to directly measure. Here, we study the vibrational dynamics of Raman activated CCl4 with XTAS targeting the C 1s and Cl 2p electrons. The totally symmetric stretching mode leads to concerted elongation or contraction in bond lengths, which in turn induce an experimentally measurable red or blue shift in the X-ray absorption energies associated with inner-shell electron excitations to the valence antibonding levels. The ratios between slopes of different core-excited potential energy surfaces (CEPESs) thereby extracted agree very well with Restricted Open-Shell Kohn-Sham calculations. The other, asymmetric, modes do not measurably contribute to the XTAS signal. The results highlight the ability of XTAS to reveal coherent nuclear dynamics involving < 0.01 Å atomic displacements and also provide direct measurement of forces on CEPESs.

Coherent spin dynamics between electron and nucleus within a single atom

The nuclear spin, being much more isolated from the environment than its electronic counterpart, presents opportunities for quantum experiments with prolonged coherence times. Electron spin resonance (ESR) combined with scanning tunnelling microscopy (STM) provides a bottom-up platform to study the fundamental properties of nuclear spins of single atoms on a surface. However, access to the time evolution of nuclear spins remained a challenge. Here, we present an experiment resolving the nanosecond coherent dynamics of a hyperfine-driven flip-flop interaction between the spin of an individual nucleus and that of an orbiting electron. We use the unique local controllability of the magnetic field emanating from the STM probe tip to bring the electron and nuclear spins in tune, as evidenced by a set of avoided level crossings in ESR-STM. Subsequently, we polarize both spins through scattering of tunnelling electrons and measure the resulting free evolution of the coupled spin system using a DC pump-probe scheme. The latter reveals a complex pattern of multiple interfering coherent oscillations, providing unique insight into hyperfine physics on a single atom level.

Optical tomography and coherence of a cavity interacting with two time-dependent position qubits

Optical tomography is a widely used method for estimating complex information. It provides a monotonic relation between the coherent field states density and their corresponding probability distributions. This approach is critical for validating any quantum information processing system’s implementation. This paper explores the optical tomography and coherence dynamics for a cavity interacting with two two-level atoms having time-dependent locations. We analyze the dynamics of the photon-field states, as two moving atoms enter a cavity filled with two superposed coherent states. The von-Neumann entropy dynamics illustrates how interaction couplings between the two atoms and cavity can give rise to entangled states under the effects of the atom-field couplings and the time-dependent atomic location parameter. Aside from coherence, the interactions between the cavity and atoms are essential for producing nonclassical proprieties in optical tomography. Furthermore, we investigate the dynamics of optical tomography densities with respect to the couplings between atoms and photons for time-dependent atomic location. Our results show that the couplings between atoms and cavity not only accelerate but also improve the processes involved in generating nonclassical optical tomography and coherence dynamics.

Rossby waves with barotropic–baroclinic coherent structures and dynamics for the (2 + 1)-dimensional coupled cylindrical KP equations with variable coefficients

Starting from the classical quasi-geostrophic potential vorticity equation with equal depth two-layer fluid, the coupled cylindrical Kadomtsev–Petviashvili (KP) equations with variable coefficients for Rossby waves are studied. To be more general, the phase velocity is considered an indefinite integral about time and improves the analysis procedure. So the variable coefficients are obtained and some previous studies are reasonably explained. The cylindrical wave theory is therewith utilized to reduce the coupled cylindrical KP equations with variable coefficients, and based on the modified Hirota bilinear method, the lump solutions and interaction solutions are found. Through numerical simulations, the Rossby lump waves on both sides of the y axis move closer to the center, and their amplitude gradually decreases and tends to flatten with the generalized Rossby parameter growth. In the Rossby waves flow field, the dipole structures propagate to the east and lead to the appearance of the compress phenomenon during barotropic–baroclinic interaction. It is possibly useful for further theoretical research on atmospheric phenomena.