Quantum Coherence Of Electrons Research Articles

Universal Conductance Fluctuations in a MnBi2Te4 Thin Film.

Quantum coherence of electrons can produce striking behaviors in mesoscopic conductors. Although magnetic order can also strongly affect transport, the combination of coherence and magnetic order has been largely unexplored. Here, we examine quantum coherence-driven universal conductance fluctuations in the antiferromagnetic, canted antiferromagnetic, and ferromagnetic phases of a thin film of the topological material MnBi2Te4. In each magnetic phase, we extract a charge carrier phase coherence length of about 100 nm. The conductance magnetofingerprint is repeatable when sweeping applied magnetic field within one magnetic phase. Surprisingly, in the antiferromagnetic and canted antiferromagnetic phases, but not in the ferromagnetic phase, the magnetofingerprint depends on the direction of the field sweep. To explain our observations, we suggest that conductance fluctuation measurements are sensitive to the motion and nucleation of magnetic domain walls in MnBi2Te4.

Mapping electronic decoherence pathways in molecules.

Establishing the fundamental chemical principles that govern molecular electronic quantum decoherence has remained an outstanding challenge. Fundamental questions such as how solvent and intramolecular vibrations or chemical functionalization contribute to the decoherence remain unanswered and are beyond the reach of state-of-the-art theoretical and experimental approaches. Here we address this challenge by developing a strategy to isolate electronic decoherence pathways for molecular chromophores immersed in condensed phase environments that enables elucidating how electronic quantum coherence is lost. For this, we first identify resonance Raman spectroscopy as a general experimental method to reconstruct molecular spectral densities with full chemical complexity at room temperature, in solvent, and for fluorescent and non-fluorescent molecules. We then show how to quantitatively capture the decoherence dynamics from the spectral density and identify decoherence pathways by decomposing the overall coherence loss into contributions due to individual molecular vibrations and solvent modes. We illustrate the utility of the strategy by analyzing the electronic decoherence pathways of the DNA base thymine in water. Its electronic coherences decay in [Formula: see text]30 fs. The early-time decoherence is determined by intramolecular vibrations while the overall decay by solvent. Chemical substitution of thymine modulates the decoherence with hydrogen-bond interactions of the thymine ring with water leading to the fastest decoherence. Increasing temperature leads to faster decoherence as it enhances the importance of solvent contributions but leaves the early-time decoherence dynamics intact. The developed strategy opens key opportunities to establish the connection between molecular structure and quantum decoherence as needed to develop chemical strategies to rationally modulate it.

Dephasing effect promotes the appearance of quantized Hall plateaus

The quantum Hall effect (QHE) is a topologically protected phenomenon which has been observed in various systems. In experiments, the size of Hall bar device to realize the QHE is generally much larger than the phase coherence length, in which the quantum coherence of electrons is destroyed. Here, we theoretically study the influence of dephasing effect on the quantized Hall (QH) plateaus. We find that the QH plateaus disappear in perfectly quantum coherent systems if the coupling between leads and central region is imperfect. The Hall resistance is very large and strongly oscillates instead of presenting the QH plateaus in this case. However, by introducing the dephasing, Hall resistance decreases and the QH plateaus appear gradually. Similar results can also be observed for the quantum anomalous Hall effect. Our results propose that dephasing effect promotes the appearance of QH plateaus, which opens a new topic of the dephasing effect on topological systems.

Imaginary-time open-chain path-integral approach for two-state time correlation functions and applications in charge transfer.

Quantum time correlation functions (TCFs) involving two states are important for describing nonadiabatic dynamical processes such as charge transfer (CT). Based on a previous single-state method, we propose an imaginary-time open-chain path-integral (OCPI) approach for evaluating the two-state symmetrized TCFs. Expressing the forward and backward propagation on different electronic potential energy surfaces as a complex-time path integral, we then transform the path variables to average and difference variables such that the integration over the difference variables up to the second order can be performed analytically. The resulting expression for the symmetrized TCF is equivalent to sampling the open-chain configurations in an effective potential that corresponds to the average surface. Using importance sampling over the extended OCPI space via open path-integral molecular dynamics, we tested the resulting path-integral approximation by calculating the Fermi's golden rule CT rate constant within a widely used spin-boson model. Comparing with the real-time linearized semiclassical method and analytical result, we show that the imaginary-time OCPI provides an accurate two-state symmetrized TCF and rate constant in the typical turnover region. It is shown that the first bead of the open chain corresponds to physical zero-time and that the endpoint bead corresponds to final time t; oscillations of the end-to-end distance perfectly match the nuclear mode frequency. The two-state OCPI scheme is seen to capture the tested model's electronic quantum coherence and nuclear quantum effects accurately.

Electronic quantum coherence in glycine molecules probed with ultrashort x-ray pulses in real time

Here, we use x-rays to create and probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay and by photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times (0 to 25 fs) is observed in both measurements. Advanced ab initio many-electron simulations allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence. In the kinematically complete x-ray absorption measurement, we monitor its dynamics for a period of 175 fs and observe an evolving modulation that may implicate the coupling of electronic to vibronic coherence at longer time scales. Our experiment provides a direct support for the existence of long-lived electronic coherence in photoionized biomolecules.

Investigation of Electronic Quantum Coherence in Semiconductor Materials using Time-resolved Non-Linear Optical Microscopy at Nanoscale Level

Investigation of Electronic Quantum Coherence in Semiconductor Materials using Time-resolved Non-Linear Optical Microscopy at Nanoscale Level

Anyons in quantum Hall interferometry

The quantum Hall (QH) effect represents a unique playground where quantum coherence of electrons can be exploited for various applications, from metrology to quantum computation. In the fractional regime it also hosts anyons, emergent quasiparticles that are neither bosons nor fermions and possess fractional statistics. Their detection and manipulation represent key milestones in view of topologically protected quantum computation schemes. Exploiting the high degree of phase coherence, edge states in the QH regime have been investigated by designing and constructing electronic interferometers, able to reveal the coherence and statistical properties of the interfering constituents. Here, we review the two main geometries developed in the QH regime, the Mach-Zehnder and the Fabry-Perot interferometers. We present their basic working principles, fabrication methods, and the main results obtained both in the integer and fractional QH regime. We will also show how recent technological advances led to the direct experimental demonstration of fractional statistics for Laughlin quasiparticles in a Fabry-Perot interferometric setup.

In vacuo atomic layer deposition and electron tunneling characterization of ultrathin dielectric films for metal/insulator/metal tunnel junctions

Metal-insulator-metal tunnel junctions (MIMTJs) are an enabling technology for future electronics including advanced computing, data storage, sensors, etc. MIMTJs are formed by inserting an ultrathin insulating layer, known as the tunnel barrier (TB), between metal electrodes. Devices based on MIMTJs have advantages of enhanced quantum coherent transport, fast speed, small size, and energy efficiency. The performance of MIMTJs depends critically on the thickness and quality of the tunnel barrier. Specifically, the tunneling current, for example, the superconducting critical current in superconductor-insulator-superconductor Josephson junctions (JJs) or the spin tunneling current in ferromagnetic-insulator-ferromagnetic magnetic tunnel junctions (MTJs), decreases exponentially with the TB thickness. This means thinner TBs would enable stronger coherent tunneling in MIMTJs. In addition, the defects in the TBs can degrade the quantum coherence of electrons (spins) of JJs and MTJs, respectively, resulting in decoherence and degraded performance of the MIMTJs. This justifies the urgent need in research and development of ultrathin (subnanometers to 1 nm) pinhole-free and defect-free TBs beyond the current state-of-the-art TBs of larger thickness (>1–2 nm) and high defect concentration made using thermal diffusion of oxygen or physical vapor deposition (PVD) including magnetron sputtering and molecular beam epitaxy. Atomic layer deposition (ALD) can provide a unique resolution to achieving ultrathin and defect-free dielectric TBs for high-performance MIMTJs for future electronics. In this article, a review on their recent effort in the development of in vacuo ALD for the fabrication of ultrathin TBs for JJs and MTJs is presented. A custom-designed system that integrates high-vacuum/ultrahigh-vacuum PVD, ALD, and scanning probe microscopy was established for in vacuo fabrication of MIMTJs and characterization of the electronic properties of ALD TBs including Al2O3, MgO, and Al2MgO4 on both superconductor metals (Al) and ferromagnetic metals (Fe and FeCoB). Capacitors with ALD dielectric of thickness in the range of 1–5 nm were also constructed for the characterization of the dielectric properties of the ALD TBs. The authors have found that the metal-insulator interface plays a critical role in controlling the quality of the ALD TBs including the tunnel barrier height, dielectric constant, electric breakdown, and uniformity. They have shown that JJs and MTJs with 0.1–1.0 nm thick ALD Al2O3 TBs can be obtained with highly promising performance. The result obtained suggests that the in vacuo ALD may provide a unique approach toward MIMTJs with an atomic-scale control of the device structure required for high-performance future electronics.

Does electronic coherence enhance anticorrelated pigment vibrations under realistic conditions?

The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom. Here, we reexamine two recently formulated concepts that a coherent vibronic coupling between molecular states would either extend the electronic coherence lifetime or enhance the amplitude of the anticorrelated vibrational mode at longer times. For this, we study a vibronically coupled dimer and calculate the nonlinear two-dimensional (2D) electronic spectra that directly reveal electronic coherence. The time scale of electronic coherence is initially extracted by measuring the antidiagonal bandwidth of the central peak in the 2D spectrum at zero waiting time. Based on the residual analysis, we identify small-amplitude long-lived oscillations in the cross-peaks, which, however, are solely due to groundstate vibrational coherence, regardless of having resonant or off-resonant conditions. Our studies neither show an enhancement of the electronic quantum coherence nor an enhancement of the anticorrelated vibrational mode by the vibronic coupling under ambient conditions.

Interplay between Josephson and Aharonov-Bohm effects in Andreev interferometers

Proximity induced quantum coherence of electrons in multi-terminal voltage-driven hybrid normal-superconducting nanostructures may result in a non-trivial interplay between topology-dependent Josephson and Aharonov-Bohm effects. We elucidate a trade-off between stimulation of the voltage-dependent Josephson current due to non-equilibrium effects and quantum dephasing of quasiparticles causing reduction of both Josephson and Aharonov-Bohm currents. We also predict phase-shifted quantum coherent oscillations of the induced electrostatic potential as a function of the externally applied magnetic flux. Our results may be employed for engineering superconducting nanocircuits with controlled quantum properties.

Correlated Disorder in YBCO and Composite YBCO Films Revealed by Means of Synchrotron X-Ray Diffraction

The presence of lattice correlated disorder in real materials places further demands on the understanding of the structure-function relationship. The study of this disorder is quite challenging, since it can be due to various and interconnected reasons. This requires advanced probes able to measure weak structural features. Thanks to synchrotron radiation features, nowadays, it is possible to visualize structural disorder alongside its spatial distribution and time dynamics. In this context, we aim to characterize thin-film superconducting YBa 2 Cu 3 O 7-x , whose structure is particularly rich. Indeed, here, the nanogranularity related to superlattices, distribution of dopants, and strain-induced stoichiometry inhomogeneity are coupled with the intrinsic granularity arising from the material island growth mode, which leads to small grains (~200 nm) and a large network of grain boundaries. X-ray Grazing incidence diffraction has been used to visualize low-dimensional lattice disorder in optimally doped YBa 2 Cu 3 O 7-x with inclusion of BaZrO 3 nanodefects grown on SrTiO 3 single crystals. The results are expected to shade light on interplay of lattice disorder and the electronic quantum coherence in the superconducting state.

Substantially Enhancing Quantum Coherence of Electrons in Graphene via Electron-Plasmon Coupling.

The interplays between different quasiparticles in solids lay the foundation for a wide spectrum of intriguing quantum effects, yet how the collective plasmon excitations affect the quantum transport of electrons remains largely unexplored. Here we provide the first demonstration that when the electron-plasmon coupling is introduced, the quantum coherence of electrons in graphene is substantially enhanced with the quantum coherence length almost tripled. We further develop a microscopic model to interpret the striking observations, emphasizing the vital role of the graphene plasmons in suppressing electron-electron dephasing. The novel and transformative concept of plasmon-enhanced quantum coherence sheds new insight into interquasiparticle interactions, and further extends a new dimension to exploit nontrivial quantum phenomena and devices in solid systems.

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is commonly rationalized in terms of excitons moving on a grid of biomolecular chromophores on typical timescales [Formula: see text]100 fs. Today's understanding of the energy transfer includes the fact that the excitons are delocalized over a few neighboring sites, but the role of quantum coherence is considered as irrelevant for the transfer dynamics because it typically decays within a few tens of femtoseconds. This orthodox picture of incoherent energy transfer between clusters of a few pigments sharing delocalized excitons has been challenged by ultrafast optical spectroscopy experiments with the Fenna-Matthews-Olson protein, in which interference oscillatory signals up to 1.5 ps were reported and interpreted as direct evidence of exceptionally long-lived electronic quantum coherence. Here, we show that the optical 2D photon echo spectra of this complex at ambient temperature in aqueous solution do not provide evidence of any long-lived electronic quantum coherence, but confirm the orthodox view of rapidly decaying electronic quantum coherence on a timescale of 60 fs. Our results can be considered as generic and give no hint that electronic quantum coherence plays any biofunctional role in real photoactive biomolecular complexes. Because in this structurally well-defined protein the distances between bacteriochlorophylls are comparable to those of other light-harvesting complexes, we anticipate that this finding is general and directly applies to even larger photoactive biomolecular complexes.

Attosecond Dynamics of Molecular Electronic Ring Currents.

Ultrafast charge migration is of fundamental importance to photoinduced chemical reactions. However, exploring such a quantum dynamical process requires demanding spatial and temporal resolutions. We show how electronic coherence dynamics induced in molecules by a circularly polarized UV pulse can be tracked by using a time-delayed circularly polarized attosecond X-ray pulse. The X-ray probe spectra retrieve an image at different time delays, encoding instantaneous pump-induced circular charge migration information on an attosecond time scale. A time-dependent ultrafast electronic coherence associated with the periodical circular ring currents shows a strong dependence on the helicity of the UV pulse, which may provide a direct approach to access and control the electronic quantum coherence dynamics in photophysical and photochemical reactions in real time.

Mesoscopic transport and quantum chaos

The field of Quantum Chaos, addressing the quantum manifestations of an underlying classically chaotic dynamics, was developed in the early eighties, mainly from a theoretical perspective. Few experimental systems were initially recognized to exhibit the versatility of being sensitive, at the same time, to their classical and quantum dynamics. Rydberg atoms provided the main testing ground of Quantum Chaos concepts until the early nineties, marked by the development of microwave billiards, ultra-cold atoms in optical lattices, and low-temperature transport in mesoscopic semiconductor structures. The mesoscopic regime is attained in small condensed matter systems at sufficiently low temperatures for the electrons to propagate coherently across the sample. The quantum coherence of electrons, together with the ballistic motion characteristic of ultra-clean microstructures, motivated the proposal of mesocopic systems as a very special laboratory for performing measurements and testing the theoretical ideas of Quantum Chaos. Experimental realizations and many important developments, reviewed in this article, followed from such a connection.

Quantum coherence of electrons in random networks of c-axis oriented wedge-shaped GaN nanowalls grown by molecular beam epitaxy

The depth distribution of the transport properties as well as the temperature dependence of the low field magneto-conductance for -axis oriented GaN nanowall network samples grown with different average wall-widths () are investigated. Magneto-conductance recorded at low temperatures shows clear signature of weak localization effect in all samples studied here. The scattering mean free path and the phase coherence time , are extracted from the magneto-conductance profile. Electron mobility estimated from is found to be comparable with those estimated previously from room temperature conductivity data for these samples, confirming independently the substantial mobility enhancement in these nanowalls as compared to bulk. Our study furthermore reveals that the high electron mobility region extends down to several hundreds of nanometer below the tip of the walls. Like mobility, phase coherence length () is found to increase with the reduction of the average wall width. Interestingly, for samples with lower values of the average wall width, is estimated to be as high as 60 μm, which is much larger than those reported for GaN/AlGaN heterostructure based two-dimensional electron gas (2DEG) systems.

Wigner function approach to single electron coherence in quantum Hall edge channels

Recent electron quantum optics experiments performed with on-demand single electron sources call for a mixed time/frequency approach to electronic quantum coherence. Here, we present a Wigner function representation of first-order electronic coherence and show that it provides a natural visualization of the excitations emitted by recently demonstrated single electron sources. It also gives a unified perspective on single particle and two particle interferometry experiments. In particular, we introduce a nonclassicality criterion for single electron coherence and discuss it in the context of Mach-Zehnder interferometry. Finally, the electronic Hanbury Brown and Twiss and the Hong-Ou-Mandel experiments are interpreted in terms of overlap of Wigner function, thus connecting them to signal processing.

Quantum-coherent energy transfer: implications for biology and new energy technologies

The important thing in science is not so much to obtain new facts as to discover new ways of thinking about them. Sir William Henry Bragg Nobel Prize For Physics, 1915 There is a growing body of scientific evidence that light-initiated reactions in the molecular components of photosynthetic

On the Interpretation of Quantum Coherent Beats Observed in Two-Dimensional Electronic Spectra of Photosynthetic Light Harvesting Complexes

The observation of long-lived electronic quantum coherence in a photosynthetic light harvesting system [Engel et al. Nature 2007, 446, 782] has led to much effort being devoted to elucidation of the quantum mechanisms of the photosynthetic excitation energy transfer. In this paper we examine the question of whether the decay of the coherent beating signal is due to quantum mechanical decoherence or ensemble dephasing (also called "fake decoherence"). We compare results based on the quantum master equation description of the time-evolution of the reduced density matrix with a mixed quantum/classical approach where the ensemble average is calculated after the dynamics. The two methods show good agreement with results from the quantum master equation in terms of the decay of quantum coherent oscillations when ensemble average is considered for the mixed quantum/classical approach. However, the results also demonstrate it remains possible that the quantum coherent motion is robust under individual realizations of the environment-induced fluctuations contrary to intuition obtained from the reduced density matrices, indicating that the decay of the observed quantum coherence should be understood as ensemble dephasing. Our calculations imply that coherence is a property of the pigment-protein system, not simply the preparation method of the electronic excitation.

Mixed Quantum-Classical Description of Excitation Energy Transfer in a Model Fenna−Matthews−Olsen Complex

The Fenna−Matthews−Olsen (FMO) complex has recently become a paradigmatic model system in terms of understanding the long-lived electronic quantum coherence that has been experimentally observed in photosynthetic systems. In this article we investigate the quantum dynamics of an FMO model within a mixed quantum-classical dynamics approach known as the Poisson bracket mapping equation (PBME), and explore the consequences of adopting this approximate description by simulating population transfer and electronic coherence. The results obtained via the Poisson bracket mapping formalism are explicitly compared with a selection of recent results on the FMO complex. The PBME is shown to be in excellent agreement with benchmark computational results at physiological temperature, and thus provides a computationally efficient and physically consistent algorithm that may be easily integrated in all-atom molecular dynamics simulations.