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Terahertz 2D coherent spectroscopy for probing and controlling multicorrelations in quantum matter

Terahertz 2D coherent spectroscopy (THz-2DCS) is an emerging technique that brings multidimensional resolution to the ultrafast spectral–temporal dynamics of non-equilibrium quantum phases of matter, enabling new capabilities for precise coherent control in many-body dynamics and multiorder correlations. Here, by mapping and disentangling complex excitation and detection pathways across distinct time and frequency dimensions, THz-2DCS provides a form of coherence tomography of light-induced quantum matter — revealing multiquantum coherences, separating nonlinear response functions and capturing collective modes and quantum kinetics on ultrafast THz timescales. This Perspective discusses the technical capabilities of THz-2DCS, provides a comparison to other multidimensional and coherent transient spectroscopies and looks ahead towards opportunities for advancing THz-2DCS instrumentation and experimental strategies towards new frontier discoveries.

Huang, Chuankun [Ames Laboratory (AMES), Ames, IA ↗

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump–probe experiments on condensed matter samples. Electron–phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron–phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. Here, we investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe 2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

47 OTHER INSTRUMENTATION↗

Rotational coherence dominates early-time dynamics and produces long-time revivals in the S 2 state of azulene

Here, the ultrafast dynamics of azulene have been debated for decades, with reported picosecond decay constants variously attributed to intramolecular vibrational redistribution (IVR), internal conversion, or rotational dephasing. Using polarization- and femtosecond time-resolved resonance-enhanced multiphoton ionization spectroscopy with a nanosecond delay window, we disentangle this long-standing inconsistency and show that the early 2–5 ps decay component arises entirely from the rotational dephasing of an excited-state wavepacket. Identical time constants extracted from the decay of the parallel signal and the rise of the perpendicular signal across multiple vibronic origins provide an unambiguous rotational anisotropy signature, eliminating the need for IVR-based interpretations. Extending the measurement window to 1.3 ns reveals well-structured J-type and C-type rotational coherence revivals in S 2 azulene on top of the well-documented fluorescence decay, demonstrating that both the short- and long-time dynamics contain information about the coherent rotational dynamics. These results show that azulene, and by extension polycyclic aromatic hydrocarbons, can sustain structured rotational coherence deep into the nanosecond regime, positioning PAHs as model systems for quantum-coherent wavepacket dynamics and providing a framework for probing coherence, decoherence, and rotational control in electronically rich molecular systems.

Zhan, Jie [University of Georgia, Athens, GA (Unit↗

Revealing Defect-Seeded and Interfacial Generation Mechanisms of Photoinduced Coherent Phonons with 4D Ultrafast Electron Microscopy

Ultrafast photoexcitation of coherent phonons is driven by an impulsive, collective displacement of constituent atoms from their average equilibrium lattice positions [1]. Models describing the generation of coherent acoustic modes typically invoke the creation of an anisotropic strain profile arising from the relatively instantaneous absorption of an ultrafast laser pulse [2]. If the skin depth is shallow relative to the specimen thickness, a steep tensile strain gradient perpendicular to the surface ($\frac{∂ε}{∂z}$) results. Initial relaxation occurs via rapid contraction of the surface layers followed by subsequent coherent oscillations of the lattice and launch of a train of coherent elastic strain waves [i.e., coherent acoustic phonons (CAPs)]. Macroscopically, responses are generally well-described by constitutive relations as gleaned from data gathered using ultrasonic methods or ultrafast spectroscopies. Furthermore, at the atomic to nanoscale level, individual lattice discontinuities and their impact on CAP behaviors can be modeled using multiscale methods [3,4]. Further, average unit-cell level responses on ultrafast timescales can be probed using femtosecond electron and X-ray scattering [5,6].

Flannigan, David J. [University of Minnesota, Minn↗

Out-of-Distribution Generalization for Learning Quantum Channels with Low-Energy Coherent States

When experimentally learning the action of a continuous-variable quantum process by probing it with inputs, there will often be some restriction on the input states used. One experimentally simple way to probe a quantum channel is to use low-energy coherent states. Learning a quantum channel in this way presents difficulties, due to the fact that two channels may act similarly on low-energy inputs but very differently for high-energy inputs. They may also act similarly on coherent-state inputs but differently on nonclassical inputs. Extrapolating the behavior of a channel for more general input states from its action on the far more limited set of low-energy coherent states is a case of out-of-distribution generalization. To be sure that such generalization gives meaningful results, one needs to relate error bounds for the training set to bounds that are valid for all inputs. We show that for any pair of channels that act sufficiently similarly on low-energy coherent-state inputs, one can bound how different the input-output relations are for any (high-energy or highly nonclassical) input. This proves that out-of-distribution generalization is always possible for learning quantum channels using low-energy coherent states, as long as enough samples are used.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Coherently coupled carrier and phonon dynamics in elemental tellurium probed by extreme ultraviolet transient absorption

The narrow band-gap semiconductor elemental tellurium (Te) has a unique electronic structure due to strong spin-orbit splitting and a lack of inversion symmetry of its helical lattice. Using broadband extreme ultraviolet core-level transient absorption, we simultaneously measure the coherently coupled photoinduced carrier and lattice dynamics at the Te N4,5 edge initiated by a few-cycle NIR pulse. Ultrafast excitation of carriers leads to a coherently excited A1 phonon oscillation and the generation of a hot carrier population distribution that oscillates in temperature, and the phonon excursion and hot carrier temperature are π out of phase with respect to each other. The depths of modulation suggest a significant coupling between the electronic and lattice degrees of freedom in Te. A long-lived shift of the absorption edge suggests an excited state of Te in another equilibrium potential energy surface that lives on the order of the carrier recombination timescale. The observed phonon-induced oscillations of the hot carriers are supportive of a change in the metallicity, whereby Te becomes more metallic with increasing phonon-induced displacement. Additionally, near the Fermi level we observe an energy-dependent phase of the displacive excitation of the A1 phonon mode. The discovery of coherent coupling between the lattice and hot carriers in Te provides the basis to investigate coherent interactions between spin and orbital degrees of freedom. The results spectrally and temporally resolve the correlation between photoexcited hot carriers and coherent lattice excitations, providing insight on the optical manipulation of the Te electronic structure at high carrier densities exceeding 1021cm−3.

Adelman, Jonah R↗

Pushing the Boundaries of Coherence in Superconducting Quantum Systems at the SQMS Center for Computing, Sensing, and Metrology

This talk will highlight recent advances at the SQMS Center in understanding and mitigating decoherence in superconducting quantum systems, focusing on both transmon qubits and 3D superconducting cavities. I will present results from systematic studies of materials and devices, aimed at identifying key sources of loss: including two-level systems (TLS), quasiparticles, and other noise mechanisms. These studies span microwave loss characterization in materials such as niobium, tantalum, aluminum, and their native oxides, as well as substrate losses in silicon and sapphire. Using both qubits and cavities, we disentangle subsystem contributions to loss and develop a hierarchy of mitigation strategies. Through these efforts, we have achieved transmon coherence times exceeding one millisecond. I will also present investigations into quasiparticle dynamics, including bursts observed in qubits located above ground and in the Gran Sasso underground laboratory. Additional studies explore temperature dependence to distinguish between TLS and quasiparticle losses, and reveal that applying a magnetic field can reduce temporal T1 fluctuations in transmons. Building on these results, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. By leveraging sideband interactions and error-resilient protocols including measurement-based correction and post-selection, we achieve high-fidelity quantum state control. This includes preparation of Fock states up to N = 20 with fidelities over 95%, and two-mode entanglement with coherence-limited fidelities reaching 99.9% after post-selection. These achievements position the SQMS platform as a powerful foundation for scalable quantum information processing and high-dimensional qudit encodings. Finally, I will discuss how these ultra-coherent systems are being deployed in emerging quantum sensing applications, including dark matter searches and gravitational wave detection.

Roy, Tanay [Fermilab]↗

Enhancing Coherence Limits in Superconducting Quantum Systems for Computing and Sensing

This talk will highlight recent efforts at the SQMS Center to develop qudit-based quantum computing architectures using superconducting three-dimensional (3D) cavities, as well as the use of these ultra-coherent cavities for quantum sensing. I will present systematic studies of materials and devices aimed at identifying and mitigating the dominant sources of decoherence—including two-level systems (TLS), quasiparticles, and other noise mechanisms—in both transmons and 3D cavities. These investigations include microwave loss characterization of niobium, tantalum, aluminum, their native oxides, and substrate materials such as silicon and sapphire. By combining measurements on qubits and cavities, we disentangle subsystem-specific loss mechanisms and establish a hierarchy of mitigation strategies, leading to transmon coherence times exceeding one millisecond. I will also discuss studies of quasiparticle dynamics, including quasiparticle bursts observed in qubits operated both above ground and at the Gran Sasso underground laboratory, and the observation that applied magnetic fields can suppress temporal T₁ fluctuations. Building on these advances, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. Leveraging tunable sideband interactions together with error-resilient protocols, including measurement-based error correction and post-selection, we achieve high-fidelity quantum state control, including the preparation of Fock states up to N=20 with fidelities above 95% and the generation of high-fidelity two-mode entangled states. Finally, I will discuss how these ultra-coherent quantum systems are enabling emerging quantum sensing applications, including searches for dark matter and gravitational waves.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗

Coherence bandwidth loss in transionospheric radio propagation

In this report a theoretical model is developed that predicts the single-point, two-frequency coherence function for transionospheric radio waves. The theoretical model is compared to measured complex frequency correlation coefficients using data from the seven equispaced, phase-coherent UHF signals transmitted by the Wideband satellite. The theory and data are in excellent agreement. The theory is critically dependent upon the power-law index, and the frequency coherence data clearly favor the comparatively small spectral indices that have been consistently measured from the wideband satellite phase data. A model for estimating the pulse delay jitter induced by the coherence bandwidth loss is also developed and compared with the actual delay jitter observed on synthesized pulses obtained from the Wideband UFH comb. The results are in good agreement with the theory. The results presented in this report, which are based on an asymptotic theory, are compared with the more commonly used quadratic theory. The model developed and validated in this report can be used to predict the effects of coherence bandwidth loss in disturbed nuclear environments. Simple formulas for the resultant pulse delay jitter are derived that can be used in predictive codes.

Rino, C. L.↗

Conditioned pressure spectra and coherence measurements in the core of a turbofan engine

Multiple and partial coherence functions and the corresponding conditioned coherent output spectra are computed between fluctuating pressures measured at two locations within the tailpipe of a turbofan engine and far-field acoustic pressure. The results are compared with the ordinary coherent output spectrum as obtained between a single tailpipe pressure measurement and the far-field acoustic pressure. The comparison indicates apparent additional "coherent output" (i.e., core-noise) beyond that detectable with an ordinary coherent measurement, thus suggesting the tailpipe as a core-noise source region. Further evidence suggests, however, that these differences may be attributed to the presence of transverse acoustic modes in the tailpipe and that the tailpipe is not, in fact, a significant source region.

Karchmer, A.↗

Conditioned pressure spectra and coherence measurements in the core of a turbofan engine

Multiple and partial coherence functions and the corresponding conditioned coherent output spectra are computed between fluctuating pressures measured at two locations within the tailpipe of a turbofan engine and far-field acoustic pressure. The results are compared with the ordinary coherent output spectrum as obtained between a single tailpipe pressure measurement and the far-field acoustic pressure. The comparison indicates apparent additional 'coherent output' (i.e., core-noise) beyond that detectable with an ordinary coherence measurement, thus suggesting the tailpipe as a core-noise source region. Further evidence suggests, however, that these differences may be attributed to the presence of transverse acoustic modes in the tailpipe and that the tailpipe is not, in fact, a significant source region.

Karchmer, A.↗

Progress in coherent laser radar

Considerable progress with coherent laser radar has been made over the last few years, most notably perhaps in the available range of high performance devices and components and the confidence with which systems may now be taken into the field for prolonged periods of operation. Some of this increasing maturity was evident at the 3rd Topical Meeting on Coherent Laser Radar: Technology and Applications. Topics included in discussions were: mesoscale wind fields, nocturnal valley drainage and clear air down bursts; airborne Doppler lidar studies and comparison of ground and airborne wind measurement; wind measurement over the sea for comparison with satellite borne microwave sensors; transport of wake vortices at airfield; coherent DIAL methods; a newly assembled Nd-YAG coherent lidar system; backscatter profiles in the atmosphere and wavelength dependence over the 9 to 11 micrometer region; beam propagation; rock and soil classification with an airborne 4-laser system; technology of a global wind profiling system; target calibration; ranging and imaging with coherent pulsed and CW system; signal fluctuations and speckle. Some of these activities are briefly reviewed.

Vaughan, J. M.↗

Determining the coherence of micropulses

A technique based on analysis of the cross spectra of single-use data from pulsars is described which can be used to measure the coherence properties of, and search for coherent periodicities in, pulsar signals. Several simulated pulsar models are constructed and analyzed to test the technique. From an analysis of 2000 consecutive pulses from PSR 2016 + 28 it is concluded that the micropulse coherence time of 430 MHz is less than the spin period for this object. This could could be consistent with a coherent model if the random phase jitter in such a model is 35 percent or more of the micropulse quasi-periodicity. The subpulse separation of roughly 10 ms is coherent across 4-5 pulse periods and is reasonably consistent with a model of subpulse drift that allows for variation about some mean drift rate. A two-component shot-noise model can reproduce much of the structure seen in the individual pulses as well as the spectra of PSR 2016 + 28.

Strohmayer, T. E.↗

Multiple symbol partially coherent detection of MPSK

It is shown that by using the known (or estimated) value of carrier tracking loop signal to noise ratio (SNR) in the decision metric, it is possible to improve the error probability performance of a partially coherent multiple phase-shift-keying (MPSK) system relative to that corresponding to the commonly used ideal coherent decision rule. Using a maximum-likeihood approach, an optimum decision metric is derived and shown to take the form of a weighted sum of the ideal coherent decision metric (i.e., correlation) and the noncoherent decision metric which is optimum for differential detection of MPSK. The performance of a receiver based on this optimum decision rule is derived and shown to provide continued improvement with increasing length of observation interval (data symbol sequence length). Unfortunately, increasing the observation length does not eliminate the error floor associated with the finite loop SNR. Nevertheless, in the limit of infinite observation length, the average error probability performance approaches the algebraic sum of the error floor and the performance of ideal coherent detection, i.e., at any error probability above the error floor, there is no degradation due to the partial coherence. It is shown that this limiting behavior is virtually achievable with practical size observation lengths. Furthermore, the performance is quite insensitive to mismatch between the estimate of loop SNR (e.g., obtained from measurement) fed to the decision metric and its true value. These results may be of use in low-cost Earth-orbiting or deep-space missions employing coded modulations.

Simon, M. K.↗

Software Coherence in Multiprocessor Memory Systems

Processors are becoming faster and multiprocessor memory interconnection systems are not keeping up. Therefore, it is necessary to have threads and the memory they access as near one another as possible. Typically, this involves putting memory or caches with the processors, which gives rise to the problem of coherence: if one processor writes an address, any other processor reading that address must see the new value. This coherence can be maintained by the hardware or with software intervention. Systems of both types have been built in the past; the hardware-based systems tended to outperform the software ones. However, the ratio of processor to interconnect speed is now so high that the extra overhead of the software systems may no longer be significant. This issue is explored both by implementing a software maintained system and by introducing and using the technique of offline optimal analysis of memory reference traces. It finds that in properly built systems, software maintained coherence can perform comparably to or even better than hardware maintained coherence. The architectural features necessary for efficient software coherence to be profitable include a small page size, a fast trap mechanism, and the ability to execute instructions while remote memory references are outstanding.

Bolosky, William Joseph↗

Analysis of Technology for Compact Coherent Lidar

In view of the recent advances in the area of solid state and semiconductor lasers has created new possibilities for the development of compact and reliable coherent lidars for a wide range of applications. These applications include: Automated Rendezvous and Capture, wind shear and clear air turbulence detection, aircraft wake vortex detection, and automobile collision avoidance. The work performed by the UAH personnel under this Delivery Order, concentrated on design and analyses of a compact coherent lidar system capable of measuring range and velocity of hard targets, and providing air mass velocity data. The following is the scope of this work. a. Investigate various laser sources and optical signal detection configurations in support of a compact and lightweight coherent laser radar to be developed for precision range and velocity measurements of hard and fuzzy targets. Through interaction with MSFC engineers, the most suitable laser source and signal detection technique that can provide a reliable compact and lightweight laser radar design will be selected. b. Analyze and specify the coherent laser radar system configuration and assist with its optical and electronic design efforts. Develop a system design including its optical layout design. Specify all optical components and provide the general requirements of the electronic subsystems including laser beam modulator and demodulator drivers, detector electronic interface, and the signal processor. c. Perform a thorough performance analysis to predict the system measurement range and accuracy. This analysis will utilize various coherent laser radar sensitivity formulations and different target models.

Amzajerdian, Farzin↗

Stability and Interaction of Coherent Structure in Supersonic Reactive Wakes

A theoretical formulation and analysis is presented for a study of the stability and interaction of coherent structure in reacting free shear layers. The physical problem under investigation is a premixed hydrogen-oxygen reacting shear layer in the wake of a thin flat plate. The coherent structure is modeled as a periodic disturbance and its stability is determined by the application of linearized hydrodynamic stability theory which results in a generalized eigenvalue problem for reactive flows. Detailed stability analysis of the reactive wake for neutral, symmetrical and antisymmetrical disturbance is presented. Reactive stability criteria is shown to be quite different from classical non-reactive stability. The interaction between the mean flow, coherent structure and fine-scale turbulence is theoretically formulated using the von-Kaman integral technique. Both time-averaging and conditional phase averaging are necessary to separate the three types of motion. The resulting integro-differential equations can then be solved subject to initial conditions with appropriate shape functions. In the laminar flow transition region of interest, the spatial interaction between the mean motion and coherent structure is calculated for both non-reactive and reactive conditions and compared with experimental data wherever available. The fine-scale turbulent motion determined by the application of integral analysis to the fluctuation equations. Since at present this turbulence model is still untested, turbulence is modeled in the interaction problem by a simple algebraic eddy viscosity model. The applicability of the integral turbulence model formulated here is studied parametrically by integrating these equations for the simple case of self-similar mean motion with assumed shape functions. The effect of the motion of the coherent structure is studied and very good agreement is obtained with previous experimental and theoretical works for non-reactive flow. For the reactive case, lack of experimental data made direct comparison difficult. It was determined that the growth rate of the disturbance amplitude is lower for reactive case. The results indicate that the reactive flow stability is in qualitative agreement with experimental observation.

Menon, Suresh↗

The Multi-Center Airborne Coherent Atmospheric Wind Sensor: Recent Measurements and Future Applications

The coherent Doppler lidar, when operated from an airborne platform, offers a unique measurement capability for study of atmospheric dynamical and physical properties. This is especially true for scientific objectives requiring measurements in optically-clear air, where other remote sensing technologies such as Doppler radar are at a disadvantage in terms of spatial resolution and coverage. Recent experience suggests airborne coherent Doppler lidar can yield unique wind measurements of--and during operation within--extreme weather phenomena. This paper presents the first airborne coherent Doppler lidar measurements of hurricane wind fields. The lidar atmospheric remote sensing groups of National Aeronautics and Space Administration (NASA) Marshall Space Flight Center, National Oceanic and Atmospheric Administration (NOAA) Environmental Technology Laboratory, and Jet Propulsion Laboratory jointly developed an airborne lidar system, the Multi-center Airborne Coherent Atmospheric Wind Sensor (MACAWS). The centerpiece of MACAWS is the lidar transmitter from the highly successful NOAA Windvan. Other field-tested lidar components have also been used, when feasible, to reduce costs and development time. The methodology for remotely sensing atmospheric wind fields with scanning coherent Doppler lidar was demonstrated in 1981; enhancements were made and the system was reflown in 1984. MACAWS has potentially greater scientific utility, compared to the original airborne scanning lidar system, owing to a factor of approx. 60 greater energy-per-pulse from the NOAA transmitter. MACAWS development was completed and the system was first flown in 1995. Following enhancements to improve performance, the system was re-flown in 1996 and 1998. The scientific motivation for MACAWS is three-fold: obtain fundamental measurements of subgrid scale (i.e., approx. 2-200 km) processes and features which may be used to improve parameterizations in hydrological, climate, and general/regional circulation models; obtain similar datasets to improve understanding and predictive capabilities for similarly-scaled processes and features; and simulate and validate the performance of prospective satellite Doppler lidars for global tropospheric wind measurement.

Rothermel, Jeffry↗