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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Applications of ultrafast nano-spectroscopy and nano-imaging with tip-based microscopy

Innovation in microscopy has often been critical in advancing both fundamental science and technological progress. Notably, the evolution of ultrafast near-field optical nano-spectroscopy and nano-imaging has unlocked the ability to image at spatial scales from nanometers to ångströms and temporal scales from nanoseconds to femtoseconds. This approach revealed a plethora of fascinating light-matter states and quantum phenomena, including various species of polaritons, quantum phases, and complex many-body effects. This review focuses on the working principles and state-of-the-art development of ultrafast tip-enhanced and near-field microscopy, integrating diverse optical pump-probe methods across the terahertz (THz) to ultraviolet (UV) spectral ranges. It highlights their utility in examining a broad range of materials, including two-dimensional (2D), organic molecular, and hybrid materials. The review concludes with a spatio-spectral-temporal comparison of ultrafast nano-imaging techniques, both within already well-defined domains, and offering an outlook on future developments of ultrafast tip-based microscopy and their potential to address a wider range of materials.

Zhao, Zhichen [Tongji University, Shanghai (China)↗
NASA NTRS1992

Quantum spatial propagation of squeezed light in a degenerate parametric amplifier

Differential equations which describe the steady state spatial evolution of nonclassical light are established using standard quantum field theoretic techniques. A Schroedinger equation for the state vector of the optical field is derived using the quantum analog of the slowly varying envelope approximation (SVEA). The steady state solutions are those that satisfy the time independent Schroedinger equation. The resulting eigenvalue problem then leads to the spatial propagation equations. For the degenerate parametric amplifier this method shows that the squeezing parameter obey nonlinear differential equations coupled by the amplifier gain and phase mismatch. The solution to these differential equations is equivalent to one obtained from the classical three wave mixing steady state solution to the parametric amplifier with a nondepleted pump.

Deutsch, Ivan H.↗
DOE OSTI2025

Cooperative effects in thin dielectric layers: Long-range Dicke superradiance

The realization and control of collective quantum effects so far have predominantly focused on cold atomic ensembles. Quantum photonic platforms, with their engineered Green's functions and integration capability of advanced solid-state quantum emitters, provide opportunities to explore regimes of light-matter interaction beyond the scope of atomic systems. In this work, we demonstrate that embedding quantum emitters within a thin dielectric layer fundamentally alters their collective radiative behavior. The optical modes in the dielectric layer mediate long-range dipole-dipole interactions between emitters, enabling both total and directional superradiance between emitters separated by several wavelengths. Crucially, this mechanism supports Dicke superradiance even in parameter regimes where standard settings fail to support an interaction, unveiling a dimensionality-driven enhancement of cooperative effects. By bridging many-body quantum optics and photonic engineering, our work reveals a distinct interplay between surrounding dimensionality and collective quantum dynamics. Experimental realization of these predictions, readily achievable in solid-state quantum optics platforms, paves the way for scalable, directional quantum light sources and frontiers in many-body quantum optics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Modeling Strong Light-Matter Coupling in Correlated Systems: State-Averaged Cavity Quantum Electrodynamics Complete Active Space Self-Consistent Field Theory

The description of strongly correlated systems interacting with quantized cavity modes poses significant theoretical challenges due to the combinatorial scaling of electronic and photonic degrees of freedom. Recent advances addressing this complexity include cavity quantum electrodynamics (QED) generalizations of complete active space configuration interaction and density matrix renormalization group methods. In this work, we introduce a QED extension of state-averaged complete active space self-consistent field theory, which incorporates cavity-induced correlations through a second-order orbital optimization framework with robust convergence properties. The method is implemented using both photon number state and coherent state representations, with the latter showing robust origin invariance in the energies regardless of the completeness of the photonic Fock space. The implementation enables symmetry-free orbital relaxations to account for photon-mediated symmetry breaking in polaritonic systems. Numerical validation on lithium hydride, hydroxide anion, and magnesium hydride cation demonstrates that this method achieves significantly improved accuracy in modeling ground-state and polariton potential energy surfaces compared to QED-CASCI in a fixed orbital basis. In these studies, we reach sub-kcal/mol accuracy in potential energy surface in much smaller active spaces than are required for QED-CASCI. This advancement provides a more robust approach for studying cavity-altered chemical landscapes for ground and exited strongly coupled systems.

CASSCF↗
DOE OSTI2025

Bringing weak transitions to light

Abstract Weak transitions between quantum states are of fundamental importance for a broad range of phenomena from analytical biochemistry to precision physics, but generally challenge experimental detection. Due to their small cross sections scaling with the absolute square of their transition matrix elements, spectroscopic measurements often fail in particular in the presence of competing background processes. Here we introduce a general concept to break this scaling law and enhance the transition probability by exploiting a stronger laser-coupled pathway to the same excited state. We demonstrate the concept experimentally by attosecond transient absorption spectroscopy in helium atoms. The quasi-forbidden transitions from the ground state 1s 2 to the weakly coupled doubly excited 2p3dandsp 2,4− states are boosted by an order of magnitude. Enhancing single-photon-suppressed transitions can find widespread applicability, from spectral diagnostics of complex molecules in life and chemical sciences to precision spectroscopy of weak transitions in metastable atomic nuclei in the search for new physics.

Science & Technology - Other Topics↗
DOE OSTI2026

Zero-added-loss entanglement multiplexing using time-bin spectral shearing

High-quality quantum communications that enable important capabilities, such as distributed quantum computing and sensing, will require quantum repeaters for providing high-quality entanglement. To realize high-rate heralded entanglement for quantum repeaters, Chen et al . [Phys. Rev. Appl. 19 , 054029 (2023)] proposed a scheme for heralded-multiplexed generation of quasideterministic entangled photon pairs, called zero-added-loss multiplexing (ZALM). Here, we propose a design of the ZALM source using time-bin entanglement and spectral shearing. Additionally, we provide an analysis of experimentally relevant spectral-shearing parameters to optimize the spectral multiplexing. Moreover, we experimentally verify the compatibility of time-bin pulses and spectral shearing, as supported by observation of no appreciable phase shift when the same shearing is applied to both time bins. These results expand the benefits of applying a ZALM source to time-bin entanglement use cases. Moreover, more fully demonstrating time-bin and spectral shearing compatibility clears a path toward a broader use of spectral shearing that provides a deterministic frequency shift of high utility.

entanglement production↗
DOE OSTI2024

Symmetry Protected Two-Photon Coherence Time

We report the observation of symmetry protected two-photon coherence time of biphotons generated from backward spontaneous four-wave mixing in laser-cooled 87 Rb atoms. When biphotons are nondegenerate, nonsymmetric photonic absorption loss results in exponential decay of the temporal waveform of the two-photon joint probability amplitude, leading to shortened coherence time. In contrast, in the case of degenerate biphotons, when both paired photons propagate with the same group velocity and absorption coefficient, the two-photon coherence time, protected by space-time symmetry, remains unaffected by medium absorptive losses. Furthermore, our experimental results validate these theoretical predictions. This outcome highlights the pivotal role of symmetry in manipulating and controlling photonic quantum states.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Polaritonic quantum matter

Polaritons are quantum mechanical superpositions of photon states with elementary excitations in molecules and solids. The light–matter admixture causes a characteristic frequency-momentum dispersion shared by all polaritons irrespective of the microscopic nature of material excitations that could entail charge, spin, lattice or orbital effects. Polaritons retain the strong nonlinearities of their matter component and simultaneously inherit ray-like propagation of light. Polaritons prompt new properties, enable new opportunities for spectroscopy/imaging, empower quantum simulations and give rise to new forms of synthetic quantum matter. Here, we review the emergent effects rooted in polaritonic quasiparticles in a wide variety of their physical implementations. We present a broad portfolio of the physical platforms and phenomena of what we term polaritonic quantum matter. We discuss the unifying aspects of polaritons across different platforms and physical implementations and focus on recent developments in: polaritonic imaging, cavity electrodynamics and cavity materials engineering, topology and nonlinearities, as well as quantum polaritonics.

light–matter interaction↗
NASA NTRS2011

Phase-Sensitive Coherence and the Classical-Quantum Boundary in Ghost Imaging

The theory of partial coherence has a long and storied history in classical statistical optics. the vast majority of this work addresses fields that are statistically stationary in time, hence their complex envelopes only have phase-insensitive correlations. The quantum optics of squeezed-state generation, however, depends on nonlinear interactions producing baseband field operators with phase-insensitive and phase-sensitive correlations. Utilizing quantum light to enhance imaging has been a topic of considerable current interest, much of it involving biphotons, i.e., streams of entangled-photon pairs. Biphotons have been employed for quantum versions of optical coherence tomography, ghost imaging, holography, and lithography. However, their seemingly quantum features have been mimicked with classical-sate light, questioning wherein lies the classical-quantum boundary. We have shown, for the case of Gaussian-state light, that this boundary is intimately connected to the theory of phase-sensitive partial coherence. Here we present that theory, contrasting it with the familiar case of phase-insensitive partial coherence, and use it to elucidate the classical-quantum boundary of ghost imaging. We show, both theoretically and experimentally, that classical phase-sensitive light produces ghost imaging most closely mimicking those obtained in biphotons, and we derived the spatial resolution, image contrast, and signal-to-noise ratio of a standoff-sensing ghost imager, taking into account target-induced speckle.

coherence theory↗
DOE OSTI2026

Proposed framework for applying squeezed light to multi-photon absorption plasma diagnostics

We propose a quantum-enhanced plasma diagnostic based on squeezed states of light. Squeezed light can exhibit super-Poissonian photon statistics, leading to enhanced multiphoton absorption cross-sections compared to classical light. This effect enables improved sensitivity for two-photon excitation of high-energy atomic transitions such as ground-state excitation, and results in increased absorbed power and fluorescence in a plasma. We consider two methods of generating squeezed states and evaluate their advantages and limitations in the context of plasma absorption diagnostics. By comparing with and extending previous theoretical work, we predict an enhancement of the absorption signal by up to seven orders of magnitude at low intensities (10 1 W/m 2 ), with diminishing enhancement persisting up to high intensities (10 10 W/m 2 ). These results suggest that squeezed-light sources offer a viable pathway toward quantum-enhanced plasma diagnostics.

imaging↗
DOE OSTI2026

Scattering theory of frequency-entangled biphoton states facilitated by cavity polaritons

The use of quantum light to probe exciton properties in semiconductor and molecular nanostructures typically occurs in the low-intensity regime. A substantial enhancement of exciton-photon coupling can be achieved with photonic cavities, where excitons hybridize with cavity modes to form polariton states. Here, to provide a theoretical framework for interpreting emerging experimental efforts in this direction, we develop a scattering theory describing the interaction of frequency-entangled photon pairs with cavity polariton and bipolariton states under various coupling regimes. Employing the Tavis-Cummings model in combination with our scattering approach, we present a quantitative analysis of how the interaction of the entangled photon pair with the polariton or bipolariton modifies its joint spectral amplitude (JSA). Specifically, we examine the effects of the cavity-mode steady-state population, exciton-cavity coupling strength, and different forms of the input photon JSA. Our results show that the entanglement entropy of the scattered photons is highly sensitive to the interplay between the input JSA and the spectral line shapes of the polariton resonances, emphasizing the cavity filtering effects. We suggest that biphoton-scattering quantum light spectroscopy best serves as a sensitive probe of polariton and bipolariton states in the photon-vacuum cavity state. Our approach is not only robust to various regimes of cavity-exciton coupling, but also amenable to extensions beyond the Tavis-Cummings model, enabling the representation of a broad class of molecular systems and solid state quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Coherent anti-Stokes Raman scattering with squeezed light: CARS for quantum-enhanced spectroscopy and imaging

We theoretically investigate quantum-enhanced coherent anti-Stokes Raman scattering (CARS) using squeezed light to amplify vibrational transition rates at low photon flux. Quantum sensing approaches are needed for nondestructive nanometrology such as in bioimaging where reduced photodamage is desired while retaining resolution and sensitivity. We analyze both single-mode squeezing applied to the pump field and two-mode squeezing between the pump and Stokes fields. We also show that the ordering of displacement and squeezing operations—whether displacement precedes squeezing or squeezing precedes displacement—has an impact on the resulting CARS transition amplitudes due to a difference in the photon number and the quantum-enhancement coefficients, with the latter offering a stronger enhancement in the case of two modes squeezing of the pump and Stokes under experimentally accessible conditions. Furthermore, our calculations capture these quantum enhancements through the intrinsic photon-number correlations of squeezed light, eliminating the need for interferometric detection or higher pump powers that are otherwise required to reach comparable sensitivities in classical CARS. Finally, we outline a quantum plasmonic extension of our model in which local field enhancements caused by surface plasmon excitation in metallic nanoparticles can be incorporated via mode-selective field amplification factors, offering a pathway toward combining squeezed-light quantum optics with surface-enhanced nanoscale spectroscopy and imaging.

Atomic & molecular structure↗
NASA NTRS2020

On Perspectives of Generating Quasi-Fock State via Resonant Self-Phase-Modulation

Optical resonators with cubic nonlinearity were among the ?rst simplest physical systems proposed for generation of squeezed states of light as well as for veri?cation of quantum nondemolition measurement concept. These conventional squeezed states are characterized with Gaussian statistics and positive Wigner function and are frequently treated as semiclassical. In contrast, it is known that the quantum states resulting from the higher order self-phase modulation are characterized with negative Wigner function. Such states can be transformed to an imperfect Fock state via classical biasing. Using these known features, we have developed an experiment strategy for observation and characterization of the nonclassical state in a system based on a high-Q nonlinear optical microcavity. We discuss technical limitations for the state observation associated with the losses in the system and technical noise of the classical optical sources involved in the measurement.

Bilenko, I. A.↗
NASA NTRS2005

Magnetometer Based on Optoelectronic Microwave Oscillator

proposed instrument, intended mainly for use as a magnetometer, would include an optoelectronic oscillator (OEO) stabilized by an atomic cell that could play the role of a magnetically tunable microwave filter. The microwave frequency would vary with the magnetic field in the cell, thereby providing an indication of the magnetic field. The proposed magnetometer would offer a combination of high accuracy and high sensitivity, characterized by flux densities of less than a picotesla. In comparison with prior magnetometers, the proposed magnetometer could, in principle, be constructed as a compact, lightweight instrument: It could fit into a package of about 10 by 10 by 10 cm and would have a mass <0.5 kg. As described in several prior NASA Tech Briefs articles, an OEO is a hybrid of photonic and electronic components that generates highly spectrally pure microwave radiation, and optical radiation modulated by the microwave radiation, through direct conversion between laser light and microwave radiation in an optoelectronic feedback loop. As used here, "atomic cell" signifies a cell containing a vapor, the constituent atoms of which can be made to undergo transitions between quantum states, denoted hyperfine levels, when excited by light in a suitable wavelength range. The laser light must be in this range. The energy difference between the hyperfine levels defines the microwave frequency. In the proposed instrument (see figure), light from a laser would be introduced into an electro-optical modulator (EOM). Amplitude-modulated light from the exit port of the EOM would pass through a fiber-optic splitter having two output branches. The light in one branch would be sent through an atomic cell to a photodiode. The light in the other branch would constitute the microwave-modulated optical output. Part of the light leaving the atomic cell could also be used to stabilize the laser at a frequency in the vicinity of the desired hyperfine or other quantum transition. The microwave signal from the output of the photodiode would be amplified (if necessary, as explained below) and fed back into the EOM. This system would oscillate if the amplification in the closed loop exceeded the linear absorption of the loop. The microwave amplifier may be unnecessary to sustain stable oscillations, depending on the power of the laser radiation at the photodetector and on particular features of the modulator and optical delay line.

Maleki, Lute↗
NASA NTRS1994

Multimode squeezing, biphotons and uncertainty relations in polarization quantum optics

The concept of squeezing and uncertainty relations are discussed for multimode quantum light with the consideration of polarization. Using the polarization gauge SU(2) invariance of free electromagnetic fields, we separate the polarization and biphoton degrees of freedom from other ones, and consider uncertainty relations characterizing polarization and biphoton observables. As a consequence, we obtain a new classification of states of unpolarized (and partially polarized) light within quantum optics. We also discuss briefly some interrelations of our analysis with experiments connected with solving some fundamental problems of physics.

Karassiov, V. P.↗
DOE OSTI2025

Twisted Nonlinear Optics in Monolayer van der Waals Crystals

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications in optical communications and quantum information science. Multibeam nonlinear optical processes, augmented by optical vortices, are essential in this context, providing robust access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting multipulse difference frequency, sum frequency, and four-wave mixing in monolayer quantum materials, we demonstrate their ability to independently control the orbital angular momentum and radial distribution of vortex light-fields in addition to their wavelength. Due to the atomically thin nature of the host crystal, this control spans a broad spectral bandwidth in a highly integrable platform that is unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds an innovative path for ultracompact and scalable hybrid nanophotonic technologies empowered by twisted nonlinear light–matter interactions in van der Waals nanomaterials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Spatiotemporal quenches for efficient critical ground state preparation in the two-dimensional transverse field Ising model

Quantum simulators have the potential to shed light on the study of quantum many-body systems and materials, offering unique insights into various quantum phenomena. Although adiabatic evolution has been conventionally employed for state preparation, it faces challenges when the system evolves too quickly or the coherence time is limited. In such cases, shortcuts to adiabaticity, such as spatiotemporal quenches, provide a promising alternative. This paper numerically investigates the application of spatiotemporal quenches in the two-dimensional transverse field Ising model with ferromagnetic interactions, focusing on the emergence of the ground state and its correlation properties at criticality when the gap vanishes. We demonstrate the effectiveness of these quenches in rapidly preparing ground states in critical systems. Our simulations reveal the existence of an optimal quench front velocity at the emergent speed of light, leading to minimal excitation energy density and correlation lengths of the order of finite system sizes we can simulate. These findings emphasize the potential of spatiotemporal quenches for efficient ground state preparation in quantum systems, with implications for the exploration of strongly correlated phases and programmable quantum computing.

2-dimensional systems↗
NASA NTRS2000

Sixth International Conference on Squeezed States and Uncertainty Relations

These proceedings contain contributions from about 200 participants to the 6th International Conference on Squeezed States and Uncertainty Relations (ICSSUR'99) held in Naples May 24-29, 1999, and organized jointly by the University of Naples "Federico II," the University of Maryland at College Park, and the Lebedev Institute, Moscow. This was the sixth of a series of very successful meetings started in 1990 at the College Park Campus of the University of Maryland. The other meetings in the series were held in Moscow (1992), Baltimore (1993), Taiyuan P.R.C. (1995) and Balatonfuered, Hungary (1997). The present one was held at the campus Monte Sant'Angelo of the University "Federico II" of Naples. The meeting sought to provide a forum for updating and reviewing a wide range of quantum optics disciplines, including device developments and applications, and related areas of quantum measurements and quantum noise. Over the years, the ICSSUR Conference evolved from a meeting on quantum measurement sector of quantum optics, to a wide range of quantum optics themes, including multifacet aspects of generation, measurement, and applications of nonclassical light (squeezed and Schrodinger cat radiation fields, etc.), and encompassing several related areas, ranging from quantum measurement to quantum noise. ICSSUR'99 brought together about 250 people active in the field of quantum optics, with special emphasis on nonclassical light sources and related areas. The Conference was organized in 8 Sections: Squeezed states and uncertainty relations; Harmonic oscillators and squeeze transformations; Methods of quantum interference and correlations; Quantum measurements; Generation and characterisation of non-classical light; Quantum noise; Quantum communication and information; and Quantum-like systems.

Han, D.↗