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DOE OSTI2025

Catastrophic Cooling Instability in Optically Thin Plasmas

The solar corona is the prototypical example of a low-density environment heated to high temperatures by external sources. The plasma cools radiatively, and because it is optically thin to this radiation, it becomes possible to model the density, velocity, and temperature structure of the system by modifying the MHD equations to include an energy source term that approximates the local heating and cooling rates. The solutions can be highly inhomogeneous and even multiphase because the well-known linear instability associated with this source term, thermal instability, leads to a catastrophic heating and cooling of the plasma in the nonlinear regime. Here we show that there is a separate, much simpler linear instability accompanying this source term that can rival thermal instability in dynamical importance. The stability criterion is the isochoric one identified by Parker (1953), and we demonstrate that cooling functions derived from collisional ionization equilibrium are highly prone to violating this criterion. If catastrophic cooling instability can act locally in global simulations, then it is an alternative mechanism for forming condensations, and due to its nonequilibrium character, it may be relevant to explaining a host of phenomena associated with the production of cooler gas in hot, low density plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Polariton relaxation under vibrational strong coupling: Comparing cavity molecular dynamics simulations against Fermi’s golden rule rate

Under vibrational strong coupling (VSC), the formation of molecular polaritons may significantly modify the photo-induced or thermal properties of molecules. In an effort to understand these intriguing modifications, both experimental and theoretical studies have focused on the ultrafast dynamics of vibrational polaritons. Here, following our recent work [Li et al., J. Chem. Phys. 154, 094124 (2021)], we systematically study the mechanism of polariton relaxation for liquid CO 2 under a weak external pumping. Classical cavity molecular dynamics (CavMD) simulations confirm that polariton relaxation results from the combined effects of (i) cavity loss through the photonic component and (ii) dephasing of the bright-mode component to vibrational dark modes as mediated by intermolecular interactions. The latter polaritonic dephasing rate is proportional to the product of the weight of the bright mode in the polariton wave function and the spectral overlap between the polariton and dark modes. Both these factors are sensitive to parameters such as the Rabi splitting and cavity mode detuning. Compared to a Fermi’s golden rule calculation based on a tight-binding harmonic model, CavMD yields a similar parameter dependence for the upper polariton relaxation lifetime but sometimes a modest disagreement for the lower polariton. We suggest that this disagreement results from polariton-enhanced molecular nonlinear absorption due to molecular anharmonicity, which is not included in our analytical model. Finally, we also summarize recent progress on probing nonreactive VSC dynamics with CavMD.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Nonlinear Optics Measurements in IOTA

Nonlinear integrable optics is a recently proposed accelerator lattice design approach which allows to generate an amplitude dependent tune shift which is needed in high brightness accelerators to mitigate fast coherent instabilities. Whereas usually octupoles are used to achieve this task, this concept allows doing so without exciting any resonances, in turn preventing any particle loss. The concept is based around a special magnet design, together with specific constraints on the optics of the accelerator. To study such a system, the Integrable Optics Test Accelerator (IOTA) was recently constructed and commissioned at Fermilab. For the assessment of the performance of this concept, good knowledge of the optics and the (non-)linear dynamics without the special magnet is of key importance. As such, measurements were conducted in the IOTA ring, using the captured turn-by-turn data by the beam position monitors after excitation to infer quantities such as amplitude detuning and resonance driving terms. In this note, first results of these measurements are presented.

43 PARTICLE ACCELERATORS↗

DOE OSTI2022

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Ultrafast nonlinear absorption of Haldane model quantum dots

We study theoretically the nonlinear absorbance of Haldane model quantum dots (QDs) placed in the field of an ultrashort and strong optical pulse. The absorbance strongly depends on the frequency of the pulse. When the frequency of the pulse is much less than the QD bandgap, the absorbance shows strong dependence on the pulse amplitude and, as a function of an internal phase of the Haldane model, the absorbance has maxima at intermediate values of the phase. When the frequency of the pulse becomes closer to, but still less than, the bandgap, the absorbance has a weak dependence on the pulse amplitude and, as a function of the internal phase, it has a maximum at the phase of 900 when the QD bandgap also has the smallest value. Furthermore, nonlinear electron dynamics in such QD systems changes from almost reversible one at small pulse frequencies to highly irreversible dynamics at large frequencies of the pulse.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Kirigami-Inspired Self-Assembly of 3D Structures

Self-assembly of 3D structures introduce an attractive and scalable route to realize reconfigurable and functionally capable mesoscale devices without human intervention. A common approach for achieving this is to utilize stimuli-responsive folding of hinged structures, which requires the integration of different materials and/or geometric arrangements along the hinges. It is also demonstrated that the inclusion of Kirigami cuts in planar, hingeless bilayer thin sheets can be used to produce complex 3D shapes in an on-demand manner. Nonlinear finite element models are developed to elucidate the mechanics of shape morphing in bilayer thin sheets and verify the predictions through swelling experiments of planar, millimeter-scaled PDMS (polydimethylsiloxane) bilayers in organic solvents. Building upon the mechanistic understandings, The transformation of Kirigami-cut simple bilayers into 3D shapes such as letters from the Roman alphabet (to make “ADVANCED FUNCTIONAL MATERIALS”) and open/closed polyhedral architectures is experimentally demonstrated. A possible application of the bilayers as tether-less optical metamaterials with dynamically tunable light transmission and reflection behaviors is also shown. As the proposed mechanistic design principles could be applied to a variety of materials, this research broadly contributes toward the development of smart, tetherless, and reconfigurable multifunctional systems.

36 MATERIALS SCIENCE↗

DOE OSTI2025

When do molecular polaritons behave like optical filters?

This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light–matter coupling regime. Under weak laser irradiation and when the single-molecule light–matter coupling can be neglected (often in the limit when the number of molecules per photon mode is large), we show that the excited-state molecular dynamics under collective strong coupling can be exactly replicated without the cavity using a shaped (or “filtered”) laser, whose field amplitude is enhanced by the cavity quality factor, shining on the bare molecules. As a consequence, the absorption within a cavity can be understood as the overlap between the polariton transmission and the bare molecular absorption, suggesting that polaritons act in part as optical filters. This framework demystifies and provides a straightforward explanation for a large class of experiments and theoretical models in molecular polaritonics, highlighting that the same effects can be achieved without the cavity with shaped laser pulses. With a few modifications, this simple conceptual picture can also be adapted to understand the incoherent nonlinear response of polaritonic systems. This review establishes a clear distinction between polaritonic phenomena that can be fully explained through classical linear optics and those that require a quantum electrodynamics approach. It also highlights the need to differentiate between effects that necessitate polaritons (i.e., hybrid light–matter states) and those that can occur in the weak coupling regime. Here, we further discuss that certain quantum optical effects like fluorescence can be partially described as optical filtering, whereas some others like cavity-induced Raman scattering go beyond this. Further exploration in these areas is needed to uncover novel polaritonic phenomena beyond optical filtering.

Schwennicke, Kai [University of California, San Di↗

DOE OSTI2023

Photoconversion in Disordered Semiconductors: Spatial, Spectral, and Temporal Insights through Nonlinear Microscopy (Final Technical Report)

Conversion of solar photons to useable energy requires two processes to occur successfully in a light-harvesting material: 1) the initial photoexcited state must efficiently produce excited states that are free to move, and 2) those states must be transported to a new location where they can do useful work before any potential is lost as heat. The core focus of this project examined the spatial and energetic dynamics of these two primary events of photoconversion in solution-processed semiconducting materials. The electronic properties of these systems are complex and strongly influenced by the cumulative interaction of local morphology and composition, along with defects, interfaces, and trap sites. It is therefore important to interrogate these systems at the local level, where structural and compositional heterogeneity can be precisely correlated to variation in functionality. Utilizing ultrafast laser spectroscopy coupled together with optical microscopy, this project examined how excited states and free charges spatially and energetically evolve on length scales between 10 nanometers and 10 microns and on timescales from 50 femtoseconds to 1 nanosecond. Insights gained from measurements made on these characteristic length and time scales provided new insight into how macroscopic functionality in disordered photovoltaic materials emerges from the interplay of nanoscale and mesoscale interactions.

14 SOLAR ENERGY↗

DOE OSTI2023

Hard x-ray – optical four-wave mixing using a split-and-delay line

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray, x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Signatures of Multiband Effects in High-Harmonic Generation in Monolayer MoS 2

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS 2 , as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. Further, this observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multiband recombination dipoles.

2-dimensional systems↗

DOE OSTI2022

Ultrafast nonlinear absorption of TMDC quantum dots

Here, we study theoretically absorption properties of MoS 2 quantum dots placed in an ultrashort and strong optical pulse with the duration of a few femtoseconds and the amplitude up to 1.5 V/Å. While the monolayer of MoS 2 has a bandgap of ≈ 1.8 eV, the quantum dots of MoS 2 have in-gap edge states, which open additional absorption channels. The absorbance of the system strongly depends on the amplitude of the pulse. At small amplitude, less than 0.5 V/Å, the absorbance varies by more than 20% with the frequency of the pulse. The system shows saturable absorption if the frequency of the pulse is larger than the bulk bandgap and reverse saturable absorption if the frequency of the pulse is in the bandgap. At large amplitudes, > 0.5 V/Å, of the pulse, the ultrafast absorbance of a quantum dot has a weak dependence on the pulse frequency. If the frequency of the pulse is less than the corresponding bulk bandgap, the absorbance has a nonmonotonic dependence on the pulse amplitude with the maximum at ≈ 0.5 V/Å. We also present the results for QDs of different TMDC materials, which show that at large field amplitude, > 0.5 V/Å, the absorbance is universal and has weak dependence on the type of TMDC.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Exciton dressing by extreme nonlinear magnons in a layered semiconductor

Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency mixing processes are central to communication, sensing, wavelength conversion, and attosecond physics. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear opto-magnonic coupling by presenting exciton states dressed by up to 20 harmonics of magnons, resulting from their nonlinearities, in the layered antiferromagnetic semiconductor CrSBr. We also create tunable optical side bands from sum- and difference-frequency generation between two optically bright magnon modes under symmetry breaking magnetic fields. Moreover, the observed difference-frequency generation mode can be continuously tuned into resonance with one of the fundamental magnons, resulting in parametric amplification of magnons. These findings realize the modulation of the optical frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide new avenues for implementing opto-magnonic devices.

Diederich, Geoffrey M.↗

DOE OSTI2024

Lightwave-electronic harmonic frequency mixing

Electronic frequency mixers are fundamental building blocks of electronic systems. Harmonic frequency mixing in particular enables broadband electromagnetic signal analysis across octaves of spectrum using a single local oscillator. However, conventional harmonic frequency mixers do not operate beyond hundreds of gigahertz to a few terahertz. If extended to the petahertz scale in a compact and scalable form, harmonic mixers would enable field-resolved optical signal analysis spanning octaves of spectra in a monolithic device without the need for frequency conversion using nonlinear crystals. Here, we demonstrate lightwave-electronic harmonic frequency mixing beyond 0.350 PHz using plasmonic nanoantennas. We demonstrate that the mixing process enables complete, field-resolved detection of spectral content far outside that of the local oscillator, greatly extending the range of detectable frequencies compared to conventional heterodyning techniques. Our work has important implications for applications where optical signals of interest exhibit coherent femtosecond-scale dynamics spanning multiple harmonics.

Science & Technology - Other Topics↗

DOE OSTI2025

Geometric control of hyperbolic exciton-polariton condensate dimers

Coupled many-body quantum systems exhibit rich emergent physics with diverse stationary and dynamical behaviours. By engineering platforms with tunable and distinct coupling mechanisms, new insights emerge into the collective behaviour of coupled many body systems. Particles can be exchanged via evanescent or ballistic coupling: the former, based on proximity, yields large spectral splitting, while the latter requires strict phase-matching, analogous to phase-coupled harmonic oscillators and has a smaller impact on the energy landscape. We demonstrate an all-optically tunable quantum fluid dimer based on exciton-polariton condensates in a photonic crystal waveguide with hyperbolic (saddle-like) dispersion. Varying the dimer’s angle relative to the grating tunes the coupling from evanescent to ballistic. We directly observe spectral features and mass flow shaped by the saddle dispersion. This work highlights photonic crystals as powerful platforms to explore condensed matter phenomena lying at the interface between delay-coupled nonlinear oscillators and tight binding physics.

Georgakilas, Ioannis [IBM Research-Zurich, Rüschli↗

DOE OSTI2026

Nonlinear reversal of photoexcitation on the attosecond time scale improves ultrafast X-ray diffraction images

The complex refractive index of a material governs its light-matter interactions, with intense light fields enabling tailored nonlinear optical responses. In the X-ray regime, rapid photoionization limits the potential of nonlinear techniques by inducing irreversible electronic damage. Here we demonstrate that intense, sub-femtosecond X-ray pulses, shorter than typical Auger decay times, can partially reverse photoexcitation via stimulated emission near atomic resonances. By analyzing thousands of coherent diffraction patterns and ion spectra from neon nanoparticles exposed to sub-fs and 15-fs pulses, we observe enhanced X-ray diffraction alongside reduced energy absorption for sub-fs pulses. Theoretical modeling attributes this to dynamics akin to Rabi flopping that prolong the lifetime of resonant states and suppress electronic bleaching. These findings suggest that ultrashort, intense X-ray pulses enable active control of X-ray refractive index and damage pathways, opening avenues for improved high-resolution imaging and nonlinear spectroscopy in complex nanoscale systems.

Ulmer, Anatoli [Universität Hamburg (Germany)] (OR↗

DOE OSTI2024

Nanoscale polarization transient gratings

Light manipulation at the nanoscale is essential both for fundamental science and modern technology. The quest to shorter lengthscales, however, requires the use of light wavelengths beyond the visible. In particular, in the extreme ultraviolet regime these manipulation capabilities are hampered by the lack of efficient optics, especially for polarization control. Here, we present a method to create periodic, polarization modulations at the nanoscale using a tailored configuration of the FERMI free electron laser and demonstrate its capabilities by comparing the dynamics induced by this polarization transient grating with those driven by a conventional intensity grating on a thin ferrimagnetic alloy. While the intensity grating signal is dominated by the thermoelastic response, the polarization grating excitation minimizes it, uncovering helicity-dependent responses previously undetected. We anticipate nanoscale polarization transient gratings to become useful for the study of physical, chemical and biological systems possessing chiral symmetry.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Spatially Resolved Near Field Spectroscopy of Vibrational Polaritons at the Small N Limit

Vibrational polaritons, which have been primarily studied in Fabry–Pérot cavities with a large number of molecules (N ~ 10 6 –10 10 ) coupled to the resonator mode, exhibit various experimentally observed effects on chemical reactions. However, the exact mechanism is elusively understood from the theoretical side, as the large number of molecules involved in an experimental strong coupling condition cannot be represented completely in simulations. This discrepancy between theory and experiment arises from computational descriptions of polariton systems typically being limited to only a few molecules, thus failing to represent the experimental conditions adequately. To address this mismatch, we used surface phonon polariton (SPhP) resonators as an alternative platform for vibrational strong coupling. SPhPs exhibit strong electromagnetic confinement on the surface and thus allow for coupling to a small number of molecules. As a result, this platform can enhance nonlinearity and slow down relaxation to the dark modes. In this study, we fabricated a pillar-shaped quartz resonator and then coated it with a thin layer of cobalt phthalocyanine (CoPc). By employing scattering-type scanning near-field optical microscopy (s-SNOM), we spatially investigated the dependency of vibrational strong coupling on the spatially varying electromagnetic field strength and demonstrated strong coupling with 38,000 molecules only–reaching to the small N limit. Through s-SNOM analysis, we found that strong coupling was observed primarily on the edge of the quartz pillar and the apex of the s-SNOM tip, where the maximum field enhancement occurs. In contrast, a weak resonance signal and lack of coupling were observed closer to the center of the pillar. This work demonstrates the importance of spatially resolved polariton systems in nanophotonic platforms and lays a foundation to explore polariton chemistry and chemical dynamics at the small N limit–one step closer to reconcile with high-level quantum calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Many-Exciton Quantum Dynamics in a Ruddlesden–Popper Tin Iodide

We present a study on the many-body exciton interactions in a Ruddlesden–Popper tin halide, namely, (PEA) 2 SnI 4 (PEA = phenylethylammonium), using coherent two-dimensional electronic spectroscopy. The optical dephasing times of the third-order polarization observed in these systems are determined by exciton many-body interactions and lattice fluctuations. We investigate the excitation-induced dephasing (EID) and observe a significant reduction of the dephasing time with increasing excitation density as compared to its lead counterpart (PEA) 2 PbI 4 , which we have previously reported in a separate publication [J. Chem. Phys. 2020, 153, 164706]. Surprisingly, we find that the EID interaction parameter is four orders of magnitude higher in (PEA) 2 SnI 4 than that in (PEA) 2 PbI 4 . This increase in the EID rate may be due to exciton localization arising from a more statically disordered lattice in the tin derivative. This is supported by the observation of multiple closely spaced exciton states and the broadening of the linewidth with increasing population time (spectral diffusion), which suggests a static disordered structure relative to the highly dynamic lead-halide. Additionally, we find that the exciton nonlinear coherent lineshape shows evidence of a biexcitonic state with low binding energy (<10 meV) not observed in the lead system. We model the lineshapes based on a stochastic scattering theory that accounts for the interaction with a nonstationary population of dark background excitations. Our study provides evidence of differences in the exciton quantum dynamics between tin- and lead-based Ruddlesden–Popper metal halides (RPMHs) and links them to the exciton–exciton interaction strength and the static disorder aspect of the crystalline structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗