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Multidimensional spectroscopy suggests that perovskite nanocrystals have a dark state interleaved with the triplet states.
Investigating light emission by free charged particles through the prism of quantum optics can unveil the emitter wave function.
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Word-error probability versus signal-to-noise ratio evaluation for five communications systems
A method, apparatus, and article of manufacture provide the ability to generate a damage proxy map. A master coherence map and a slave coherence map, for an area prior and subsequent to (including) a damage event are obtained. The slave coherence map is registered to the master coherence map. Pixel values of the slave coherence map are modified using histogram matching to provide a first histogram of the master coherence map that exactly matches a second histogram of the slave coherence map. A coherence difference between the slave coherence map and the master coherence map is computed to produce a damage proxy map. The damage proxy map is displayed with the coherence difference displayed in a visually distinguishable manner.
The current accepted approach to modeling launch vehicle transonic buffet environments is to acquire time-correlated unsteady pressure measurements at discrete locations on a model-scale wind-tunnel model and use these measurements to develop buffet forcing functions (BFFs).Part of the BFF development process is the application of coherence factors to account for the discrete nature of the pressure measurement used in the development of the BFFs. Presently, the Space Launch System (SLS) program divides the launch vehicle into distinct aerodynamic regions, within which, the coherence lengths are assumed to be constant. The coherence factors are computed by averaging the coherence function between sensors within the region over a specified frequency range. The present work validates and examines the impact of two proposed changes to the development of longitudinal coherence factors used in the development of launch vehicle BFFs. One change is to employ frequency-dependent coherence factors instead of coherence factors based on the mean of the coherence function. The second proposed change replaces the aerodynamic regions with a moving-segment approach that varies the calculated coherence lengths as a function of longitudinal location of the transducers. The impact of these approaches is examined using data from two rigid buffet model wind-tunnel tests: (1)a notional launch vehicle geometry through the comparison of discrete measurement-basedBFFs to loads developed by continuous integration of unsteady pressure sensitive paint data and (2) the SLS Block 1 Cargo vehicle configuration for which BFFs have been previously developed using less-mature methods. The trends from this examination of updated coherence factor approaches ultimately result in more intuitive results than currently-accepted coherence methods.
The current accepted approach to modeling launch vehicle transonic buffet environments is to acquire time-correlated unsteady pressure measurements at discrete locations on a model-scale wind-tunnel model and use these measurements to develop buffet forcing functions (BFFs). Part of the BFF development process is the application of coherence factors to account for the discrete nature of the pressure measurement used in the development of the BFFs. Presently, the Space Launch System (SLS) program divides the launch vehicle into distinct aerodynamic regions, within which, the coherence lengths are assumed to be constant. The coherence factors are computed by averaging the coherence function between sensors within the region over a specified frequency range. The present work validates and examines the impact of two proposed changes to the development of longitudinal coherence factors used in the development of launch vehicle BFFs. One change is to employ frequency-dependent coherence factors instead of coherence factors based on the mean of the coherence function. The second proposed change replaces the aerodynamic regions with a moving-segment approach that varies the calculated coherence lengths as a function of longitudinal location of the transducers. The impact of these approaches is examined using data from two rigid buffet model wind-tunnel tests: (1) a notional launch vehicle geometry through the comparison of discrete measurement-based BFFs to loads developed by continuous integration of unsteady pressure sensitive paint data and (2) the SLS Block 1 Cargo vehicle configuration for which BFFs have been previously developed using less-mature methods. The trends from this examination of updated coherence factor approaches ultimately result in more intuitive results than currently-accepted coherence methods.
Various papers on coherent lightwave communications are presented. Individual topics addressed include: overview of coherent light wave communications, frequency stabilization techniques for coherent lightwave systems, characterization of laser diode intensity noise at microwave frequencies with high sensitivity, FP and DFB semiconductor lasers with arbitrary external optical feedback, birefringence-controlled phase-shifter, polarization diversity and scrambling techniques for coherent systems, polarization control scheme for coherent optical systems, simulation of IF filtering effects on the performance of coherent optical receivers. Also discussed are: performance of optical DPSK receivers in the presence of optical channel noise, optical heterodyne communications with polarization modulation, coherent fiber optical subcarrier multiplexed system, engineered rack-mounted coherent transmission system, technology aspects of a coherent optical MAN, broadband exchange by coherent multicarrier switching, generalized temporal CDMA for optical communications. Overviews are given of recent progress at individual companies.
Coherence refers to correlations in waves. Because matter has a wave-particle nature, it is unsurprising that coherence has deep connections with the most contemporary issues in chemistry research (e.g., energy harvesting, femtosecond spectroscopy, molecular qubits and more). But what does the word "coherence" really mean in the context of molecules and other quantum systems? We provide a review of key concepts, definitions, and methodologies, surrounding coherence phenomena in chemistry, and we describe how the terms "coherence" and "quantum coherence" refer to many different phenomena in chemistry. Moreover, we show how these notions are related to the concept of an interference pattern. Coherence phenomena are indeed complex, and ambiguous definitions may spawn confusion. By describing the many definitions and contexts for coherence in the molecular sciences, we aim to enhance understanding and communication in this broad and active area of chemistry.
Characteristics of coherent and incoherent lidars are described. The carrier-to-noise ratio (CNR), SNR relationship, coherence diameter, speckle averaging, multiple pulse averaging, and the possibility of single-frequency pulse generation from the laser transmitter for the two lidar types are compared. Diagrams of the incoherent lidar's direct detection system and the coherent lidar's heterodyne detection system are presented. The transverse coherence diameter is discussed and equations for backscatter from a distributed medium, transverse coherence length, and return path refractive index variations are provided. The importance of transverse coherence length in the coherence lidar system design is considered. The effectiveness of the lidar systems is evaluated in terms of CNR and SNR. The differences in generation of noise-equivalent power are studied and it is observed that the coherent lidar system achieves higher CNR values. The relation between signal fluctuation due to speckle effects and SNR is analyzed; equations for SNR in coherent and incoherent lidar systems are given.
Combustion noise from turbofan engines has become important, as the noise from sources like the fan and jet are reduced. An aligned and un-aligned coherence technique has been developed to determine a threshold level for the coherence and thereby help to separate the coherent combustion noise source from other noise sources measured with far-field microphones. This method is compared with a statistics based coherence threshold estimation method. In addition, the un-aligned coherence procedure at the same time also reveals periodicities, spectral lines, and undamped sinusoids hidden by broadband turbofan engine noise. In calculating the coherence threshold using a statistical method, one may use either the number of independent records or a larger number corresponding to the number of overlapped records used to create the average. Using data from a turbofan engine and a simulation this paper shows that applying the Fisher z-transform to the un-aligned coherence can aid in making the proper selection of samples and produce a reasonable statistics based coherence threshold. Examples are presented showing that the underlying tonal and coherent broad band structure which is buried under random broadband noise and jet noise can be determined. The method also shows the possible presence of indirect combustion noise. Copyright 2011 Acoustical Society of America. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the Acoustical Society of America.
Electronic coherence is central to numerous areas of science, from quantum biology to quantum materials. In quantum materials, lead-halide perovskite (LHP) quantum dots (QDs) have been shown to support electronic coherence through observation of coherent single-photon emission and superfluorescence arising from spatial coherence at low temperatures. In contrast, direct measurement of temporal coherence between exciton states has been lacking. Here, we employ coherent multi-dimensional spectroscopy to observe an electronic coherence between exciton states in CsPbBr 3 QDs that is long-lived at room temperature, surviving nearly three times longer than the electronic dephasing time. This observation of a long-lived electronic coherence at room temperature points to nearly perfectly correlated lattice fluctuations for each excitonic state in the superposition. In conclusion, these experiments reveal that the properties of LHP QDs extend to lattice dynamics that give rise to correlated fluctuations in the basis exciton states, a process that may next be optimized by design.
A reaction center is a unique biological system that performs the initial charge separation within a Photosystem II (PSII) multiunit enzyme, which eventually drives the catalytic water-splitting in plants and algae. The possible role of quantum coherences coinciding with the energy and charge transfer processes in PSII reaction center is one of the active areas of research. Here, we study these quantum coherences by using a numerically exact method on an excitonic dimer model, including linear vibronic coupling and employing optimal parameters from experimental two-dimensional coherent spectroscopic measurements. This enables us to precisely capture the excitonic interaction between pigments and the dissipation of the energy from electronic and charge-transfer (CT) states to the protein environment. We employ the time nonlocal (TNL) quantum master equation to calculate the population dynamics, which yields numerically reliable results. The calculated results show that, due to the strong dissipation, the lifetime of electronic coherence is too short to have direct participation in the charge transfer processes. However, there are long-lived vibrational coherences present in the system at frequencies close to the excitionic energy gap. These are strongly coupled with the electronic coherences, which makes the detection of the electronic coherences with conventional techniques very challenging. Additionally, we unravel the strong excitonic interaction of radical pair (PD1 and PD2) in the reaction center, which results in a long-lived electronic coherence of >100 fs, even at room temperature. Our work provide important physical insight to the charge separation process in PSII reaction center, which may be helpful for better understanding of photophysical processes in other natural and artificial light-harvesting systems.
In the primary step of natural light harvesting, the solar photon energy is captured in a photoexcited electron–hole pair, or an exciton, in chlorophyll. Its conversion to chemical potential occurs in the special pair reaction center, which is reached by downhill ultrafast excited-state energy transport through a network of chromophores. Being inherently quantum, transport could in principle occur via a matter wave, with vast implications for efficiency. How long a matter wave remains coherent is determined by the intensity by which the exciton is disturbed by the noisy biological environment. The stronger this is, the stronger the electronic coupling between chromophores must be to overcome the fluctuations and phase shifts. The current consensus is that under physiological conditions, quantum coherence vanishes on the 10-fs time scale, rendering it irrelevant for the observed picosecond transfer. Yet, at low-enough temperature, quantum coherence should in principle be present. Here, we reveal the onset of longer-lived electronic coherence at extremely low temperatures of ∼20 K. Using two-dimensional electronic spectroscopy, we determine the exciton coherence times in the Fenna–Matthew–Olson complex over an extensive temperature range. At 20 K, coherence persists out to 200 fs (close to the antenna) and marginally up to 500 fs at the reaction center. It decays markedly faster with modest increases in temperature to become irrelevant above 150 K. At low temperature, the fragile electronic coherence can be separated from the robust vibrational coherence, using a rigorous theoretical analysis. We believe that by this generic principle, light harvesting becomes robust against otherwise fragile quantum effects.
Intensities in high-resolution phase-contrast images from electron microscopes build up discretely in time by detecting single electrons. A wave description of pulse-like coherent-inelastic interaction of an electron with matter implies a time-dependent coexistence of coherent partial waves. Their superposition forms a wave package by phase decoherence of 0.5 - 1 radian with Heisenbergs energy uncertainty ΔE H = $\hbar$/2 Δt -1 matching the energy loss ΔE of a coherent-inelastic interaction and sets the interaction time Δt. In these circumstances, the product of Planck's constant and the speed of light hc is given by the product of the expression for temporal coherence λ 2 /Δλ and the energy loss ΔE. Experimentally, the self-coherence length was measured by detecting the energy-dependent localization of scattered, plane matter waves in surface proximity exploiting the Goos–Hänchen shift. Chromatic-aberration Cc-corrected electron microscopy on boron nitride (BN) proves that the coherent crystal illumination and phase contrast are lost if the self-coherence length shrinks below the size of the crystal unit cell at ΔE > 200 eV. Finally, in perspective, the interaction time of any matter wave compares with the lifetime of a virtual particle of any elemental interaction, suggesting the present concept of coherent-inelastic interactions of matter waves might be generalizable.
In situ irradiations with 1 MeV Kr ions at 50~613 K up to a fluence of 6.25 × 10 14 ions/cm 2 (~1.25 displacements per atom, dpa) have been performed on pre-aged dilute Cu-0.9%Co, Cu-0.9%Fe and Cu-0.8%Cr alloys containing uniform matrix dispersions of coherent precipitates in order to study the effects of initial precipitate sink strength, damage dose and irradiation temperature on radiation-induced coherency loss of precipitates. Coherent precipitates with different point defect sink strengths (2πNd, where N and d are the precipitate density and diameter) were used in this work to examine potential differences in atomic relaxation during absorption of point defects. In all cases, irradiation to low doses (<~1 dpa) was very effective at inducing loss of precipitate coherency. At low sink strengths (~10 13 m -2 ), loss of precipitate coherency could be induced for doses ~0.01 dpa. This suggests there might be an efficient preferential medium-range strain-induced bias for absorption of interstitial defects due to tensile strains emanating from the undersized precipitates, which induces relatively rapid loss of coherency at low precipitate sink strengths. High precipitate sink strength (~10 14 m -2 ) conditions were relatively resistant to the radiation-induced loss of coherency (requiring higher doses approaching ~1 dpa) and this might be due to nearly equal numbers of interstitial and vacancy defects arriving at the precipitate interface for such high sink strength conditions. The precipitate coherency loss was observed to have a weak dependence on irradiation temperature. Molecular dynamics simulations confirm a strong effect of precipitate sink strength on the probability of interstitial absorption at precipitates.
The role of quantum mechanical coherences or coherent superposition states in excited state processes has received considerable attention in the last two decades largely due to advancements in ultrafast laser spectroscopy. These coherence effects hold promise for enhancing the efficiency and robustness of functionally relevant processes, even when confronted with energy disorder and environmental fluctuations. Understanding coherence deeply drives us to unravel mechanisms and dynamics controlled by order and synchronization at a quantum mechanical level, envisioning optical control of coherence to enhance functions or create new ones in molecular and material systems. In this frontier, the interplay between electronic and vibrational dynamics, specifically the influence of vibrations in directing electronic dynamics, has emerged as the leading principle. Here, two energetically disparate quantum degrees of freedom work in-sync to dictate the trajectory of an excited state reaction. Moreover, with the vibrational degree being directly related to the structural composition of molecular or material systems, new molecular designs could be inspired by tailoring certain structural elements. In the realm of chemical kinetics, our understanding of the dynamics of chemical transformations is underpinned by fundamental theories, such as transition state theory, activated rate theory, and Marcus theory. These theories elucidate reaction rates by considering the energy barriers that must be overcome for reactants to transform into products. Those barriers are surmounted by the stochastic nature of energy gap fluctuations within reacting systems, emphasizing that the reaction coordinate, the pathway from reactants to products, is not rigidly defined by a specific vibrational motion but encompasses a diverse array of molecular motions. While less is known about the involvement of specific intramolecular vibrational modes, their significance in certain cases cannot be overlooked. In this Account, we summarize key experimental findings that offer deeper insights into the complex electronic–vibrational trajectories encompassing excited states afforded from state-of-the-art ultrafast laser spectroscopy in three exemplary processes: photoinduced electron transfer, singlet–triplet intersystem crossing, and intramolecular vibrational energy flow in molecular systems. We delve into the rapid decoherence, or loss of phase and amplitude correlations, of vibrational coherences along promoter vibrations during subpicosecond intersystem crossing dynamics in a series of binuclear platinum complexes. This rapid decoherence illustrates the vibration-driven reactive pathways from the Franck–Condon state to the curve crossing region. We also explore the generation of new vibrational coherences induced by impulsive reaction dynamics rather than by the laser pulse in these systems, which sheds light on specific energy dissipation pathways and thereby on the progression of the reaction trajectory in the vicinity of the curve crossing on the product side. Another property of vibrational coherences, amplitude, reveals how energy can flow from one vibration to another in the electronic excited state of a terpyridine–molybdenum complex hosting a nonreactive dinitrogen substrate. In conclusion, a slight change in vibrational energy triggers a quasi-resonant interaction, leading to constructive wavepacket interference and ultimately intramolecular vibrational redistribution from a Franck–Condon active terpyridine vibration to a dinitrogen stretching vibration, energizing the dinitrogen bond.