arXiv subjects

Aaron M. Lindenberg

Publications and source records attributed to Aaron M. Lindenberg.

At least 19 recordsLinked to original sources

arXiv2026

Symmetry-selective nonrelativistic spin splitting in antiferromagnets driven by coherent phonons

Nonrelativistic spin splitting (NRSS) in antiferromagnets (AFMs) enables magnetization-free spin polarization for ultrafast spintronics. Here, we demonstrate that coherent phonons can dynamically induce and control NRSS in collinear AFMs. Excitation of $Γ$-point infrared-active phonons lifts the spin degeneracy of the ground state, while the residual sublattice-connecting symmetries determine the momentum-space form of the induced splitting. Because the relevant infrared modes couple to orthogonal in-plane light polarizations, distinct spin-split phases can be selectively activated by the polarization of the driving field. Using first-principles calculations for MnPS$_3$, we show that a mode that breaks all sublattice-connecting symmetries induces an $s$-wave spin-split state with $Δ(Γ)\neq0$, whereas a symmetry-distinct mode that preserves a sublattice-connecting mirror symmetry generates a $d$-wave altermagnetic state with $Δ(Γ)=0$. In both cases, the spin splitting grows linearly with the phonon amplitude and reverses the induced spin polarization when the displacement is reversed. Our results establish coherent lattice driving as a direct, polarization- and mode-selective route to dynamically induce distinct NRSS phases in AFMs.

cond-mat.mtrl-sci↗

arXiv2026

Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics↗

arXiv2026

Monolithic integration of optically anisotropic GeSe-based films on GaAs by templated solid-phase epitaxy

Layered IV-VI semiconductors such as GeSe exhibit strong in-plane optical anisotropy, making them promising candidates for polarization-sensitive photonic devices. However, realizing these properties in scalable platforms requires heteroepitaxial integration on technologically relevant substrates like GaAs. Direct growth of GeSe is complicated by its glass formation at low temperatures and high vapor pressure at elevated temperatures. To overcome this, we develop a method for ex-situ solid-phase epitaxy utilizing a SnSe buffer and offcut GaAs substrate to enable single-orientation crystalline GeSe films. Using polarized reflection measurements, we find that stabilizing a single-in-plane-orientation results in a 2x increase in anisotropic response between the armchair and zigzag directions. This work provides a new integration route to harness the anisotropic optical properties of GeSe and its alloys for polarization-sensitive technologies.

cond-mat.mtrl-sci↗

arXiv2026

Photoinduced orbital polarization and Jahn-Teller effect in RNiO$_3$

The orbital degree of freedom in rare-earth nickelates is typically inactive across the temperature-driven metal-insulator transition, where the system develops two inequivalent Ni sites associated with Ni-O bond disproportionation and breathing-mode distortions of NiO$_6$ octahedra. Here, we show that orbital polarization can be induced by optical excitation with linearly polarized light. Using an interacting multiband tight-binding model combined with real-time simulations of coupled electron-ion-spin dynamics, we find that photoinduced $d$-$d$ transitions reduce the local magnetic moments at Ni sites and effectively suppress Hund's coupling $J$ in the excited state. Importantly, these transitions can be made strongly orbital-selective by tuning the light polarization, leading to an imbalance in $e_g$ orbital occupancies. The resulting nonequilibrium state, characterized by reduced effective $J$ and unequal orbital populations, becomes unstable toward Jahn-Teller (JT) distortions, driving structural relaxation along coherently excited JT modes. Our results demonstrate that polarization-controlled optical excitation provides a pathway to access hidden nonthermal phases with emergent orbital order, enabling coherent control of coupled charge, spin, and lattice degrees of freedom on ultrafast timescales.

cond-mat.str-el↗

arXiv2026

Alkaline-Earth Rare-Earth Fluoride Nanoparticle Superlattices for Ultrafast, Radiation Stable Scintillators

Radioluminescent nanostructures provide a pathway to the fabrication of next-generation scintillators with tunability in composition, size, and morphology, and spectral and temporal properties, as well as scalable processing. Here we create a 3D millimeter-scale solid-state scintillators from SrLuF Ce3+, Pr3+ (SrLuF) core-shell nanostructures, integrating nanoscale building blocks into self-assembled macroscopic crystals. These scintillators exhibit single-digit nanosecond decay times, linear response, resistance to radiation-induced degradation, and optical emission yields within an order of magnitude of YAG Ce3+. We select a SrLuF host lattice owing to its high effective atomic number, wide band gap, and low phonon energy, which together support efficient 4f-5d radiative transitions from Ce3+ and Pr3+ activators while suppressing afterglow. We create a library of core-shell nanoscintillators with undoped SrLuF shells and cores spanning compositions from undoped SrLuF to fully doped SrCeF or SrPrF. Time-resolved and steady-state X-ray excited optical luminescence (XEOL) reveal broadband emission at 310 nm (Ce3+) and 335 nm (Pr3+) with biexponential decays in the sub-nanosecond (100-500 ps) and sub-15 ns (4-13 ns) regimes, demonstrating tunable radiative efficiency and ultrafast dynamics. Ensemble performance of the mm-scale superlattices is characterized under both continuous-wave and femtosecond high-intensity excitation, revealing high light yield, linear response, and radiation hardness under extreme irradiation of ultrafast 50fs X-ray pulses up to 5mJ per mm2 corresponding to a peak intensity of 1013 W per cm2. Together, these results establish a design framework for stable, bright, and tunable scintillation platforms with applications in precision health, space exploration and hard X-ray imaging at next-generation free-electron laser facilities.

cond-mat.mtrl-sci↗

arXiv2026

Dynamical diffraction formalism for imaging time-dependent diffuse scattering from coherent phonons with Dark-Field X-ray Microscopy

Coherent acoustic phonons, whose damping sets the upper bound of quality factors in acoustic resonators, play a critical role in advanced telecommunication and quantum information technologies. Yet, probing their decay in the GHz regime remains challenging using conventional surface-based techniques. Dark-field X-ray microscopy (DFXM) offers a solution by enabling through-depth, non-destructive and full-field imaging of strain fields and dislocations inside bulk materials with high spatial and angular resolution. We previously used kinematic diffraction theory to describe DFXM signals based on how the Bragg peak shifts due to the strain wave, allowing us to reconstruct the frequency spectrum of coherent phonons as a function of depth through the sample. The approach of tracking the Bragg peak shifts to study phonon dynamics, however, places an upper-bound to the highest phonon frequency that can be studied, determined by the spatial resolution of the measurement. In this work, we discuss how coherent phonon dynamics can be studied with DFXM from time-dependent intensity oscillation sidebands. This approach simultaneously allows studying coherent phonon dynamics in real and reciprocal space, overcoming frequency resolution limits imposed by the real-space resolution of Bragg-peak tracking. Using Takagi-Taupin dynamical diffraction formalism, we establish the spatial and reciprocal space resolution achievable for studying the coherent phonon dynamics and evaluate conditions for observing long-lived intensity oscillations. We close by proposing experimental strategies to optimize excitation bandwidths and reciprocal-space selectivity. The formalism in the paper enables the design of DFXM experiments for quantitative, frequency-resolved measurements of acoustic phonon decay and phonon-defect interactions in bulk crystalline materials.

cond-mat.mes-hall↗

arXiv2025

Quantifying and minimizing dissipation in a non-equilibrium phase transition

In a finite-time continuous phase transition, topological defects emerge as the system undergoes spontaneous symmetry breaking. The Kibble-Zurek mechanism predicts how the defect density scales with the quench rate. During such processes, dissipation also arises as the system fails to adiabatically follow the control protocol near the critical point. Quantifying and minimizing this dissipation is fundamentally relevant to nonequilibrium thermodynamics and practically important for energy-efficient computing and devices. However, there are no prior experimental measurements of dissipation, or the optimization of control protocols to reduce it in many-body systems. In addition, it is an open question to what extent dissipation is correlated with the formation of defects. Here, we directly measure the dissipation generated during the voltage-driven Freedericksz transition of a liquid crystal with a sensitivity equivalent to a ~10 nanokelvin temperature rise. We observe Kibble-Zurek scaling of dissipation and its breakdown, both in quantitative agreement with existing theoretical works. We further implement a fully automated in-situ optimization approach that discovers more optimal driving protocols, reducing dissipation by a factor of three relative to a simple linear protocol.

cond-mat.stat-mech↗

arXiv2025

Terahertz field-induced giant symmetry modulations in a van der Waals antiferromagnet

Strong-field terahertz (THz) excitations enable dynamic control over electronic, lattice and symmetry degrees of freedom in quantum materials. Here, we uncover pronounced terahertz-induced symmetry modulations and coherent phonon dynamics in the van der Waals antiferromagnet MnPS3, in which inversion symmetry is broken by its antiferromagnetic spin configuration. Time-resolved second harmonic generation measurements reveal long-lived giant oscillations in the antiferromagnetic phase, with amplitudes comparable to the equilibrium signal, driven by phonons involving percent-level atomic displacements relative to the equilibrium bond lengths. The temporal evolution of the rotational anisotropy patterns indicate a dynamic breaking of mirror symmetry, modulated by two vibrational modes at 1.7 THz and 4.5 THz, with the former corresponding to a hidden mode not observed in equilibrium spectroscopy. We show that these effects arise in part from a field-induced charge rearrangement mechanism that lowers the local crystal symmetry, and couples to the phonon modes. A long-lived field-driven response was uncovered with a complex THz polarization dependence which, in comparison to theory, indicates evidence for an antiferromagnetic-to-ferrimagnetic transition. Our results establish an effective field-tunable pathway for driving excitations otherwise weak in equilibrium, and for manipulating magnetism in low-dimensional materials via dynamical modulation of symmetry.

cond-mat.str-el↗

arXiv2025

Nonresonant Raman control of ferroelectric polarization

Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

physics.optics↗

arXiv2025

Terahertz-field activation of polar skyrons

Unraveling collective modes arising from coupled degrees of freedom is crucial for understanding complex interactions in solids and developing new functionalities. Unique collective behaviors emerge when two degrees of freedom, ordered on distinct length scales, interact. Polar skyrmions, three-dimensional electric polarization textures in ferroelectric superlattices, disrupt the lattice continuity at the nanometer scale with nontrivial topology, leading to previously unexplored collective modes. Here, using terahertz-field excitation and femtosecond x-ray diffraction, we discovered subterahertz collective modes, dubbed 'skyrons', which appear as swirling patterns of atomic displacements functioning as atomic-scale gearsets. Momentum-resolved time-domain measurements of diffuse scattering revealed an avoided crossing in the dispersion relation of skyrons. We further demonstrated that the amplitude and dispersion of skyrons can be controlled by sample temperature and electric-field bias. Atomistic simulations and dynamical phase-field modeling provided microscopic insights into the three-dimensional crystallographic and polarization dynamics. The discovery of skyrons and their coupling with terahertz fields opens avenues for ultrafast control of topological polar structures.

cond-mat.mtrl-sci↗

arXiv2025

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. We investigate the frequency domain representation of the photoemission intensity and \tred{the first moment of the energy distribution curves}. Both quantities provide complimentary 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.

cond-mat.mtrl-sci↗

arXiv2024

Phase Segregation Dynamics in Mixed-Halide Perovskites Revealed by Plunge-Freeze Cryogenic Electron Microscopy

Mixed-halide lead perovskites, with photoexcited charge-carrier properties suitable for high-efficiency photovoltaics, hold significant promise for high-efficiency tandem solar cells. However, phase segregation under illumination, where an iodide-rich phase forms carrier trap states, remains a barrier to applications. This study employs plunge-freeze cryogenic electron microscopy to visualize nanoscale phase segregation dynamics in CsPb(Br,I) films. By rapidly freezing the illuminated samples, we preserve transient photoexcited ion distributions for high-resolution structural and compositional analysis at the nanoscale. Cryogenic scanning transmission electron microscopy techniques (EELS, 4D-STEM) captured the dynamics of photo-induced iodine migration from grain boundaries to centers, identified the buildup of anisotropic strain, and captured the heterogeneous evolution of this process within a single grain. These findings provide new insights into microscopic phase segregation mechanisms and their dynamics, enhancing our understanding of mixed-halide perovskite photostability.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast symmetry control in photoexcited quantum dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, we unveil reversible symmetry changes in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, we reveal that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties as shown by transient optical measurements. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

cond-mat.mes-hall↗

arXiv2024

Non-equilibrium pathways to emergent polar supertextures

Ultrafast stimuli can stabilize metastable states of matter inaccessible by equilibrium means. Establishing the spatiotemporal link between ultrafast excitation and metastability is crucial to understanding these phenomena. Here, we use single-shot optical-pump, X-ray-probe measurements to provide snapshots of the emergence of a persistent polar vortex supercrystal in a heterostructure that hosts a fine balance between built-in electrostatic and elastic frustrations by design. By perturbing this balance with photoinduced charges, a starting heterogenous mixture of polar phases disorders within a few picoseconds, resulting in a soup state composed of disordered ferroelectric and suppressed vortex orders. On the pico-to-nanosecond timescales, transient labyrinthine fluctuations form in this soup along with a recovering vortex order. On longer timescales, these fluctuations are progressively quenched by dynamical strain modulations, which drive the collective emergence of a single supercrystal phase. Our results, corroborated by dynamical phase-field modeling, reveal how ultrafast excitation of designer systems generates pathways for persistent metastability.

cond-mat.mtrl-sci↗

arXiv2023

Solution-phase single-particle spectroscopy for probing multi-polaronic dynamics in quantum emitters at femtosecond resolution

The development of many optical quantum technologies depends on the availability of solid-state single quantum emitters with near-perfect optical coherence. However, a standing issue that limits systematic improvement is the significant sample heterogeneity and lack of mechanistic understanding of microscopic energy flow at the single emitter level and ultrafast timescales. Here we develop solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. We apply this technique to single quantum emitters in two-dimensional hexagonal boron nitride, which suffers from significant heterogeneity and low quantum efficiency. From millisecond to nanosecond timescales, the translation diffusion, metastable-state-related bunching shoulders, rotational dynamics, and antibunching features are disentangled by their distinct photon-correlation timescales, which collectively quantify the normalized two-photon emission quantum yield. Leveraging its femtosecond resolution, spectral selectivity and ultralow noise (two orders of magnitude improvement over solid-state methods), we visualize electron-phonon coupling in the time domain at the single defect level, and discover the acceleration of polaronic formation driven by multi-electron excitation. Corroborated with results from a theoretical polaron model, we show how this translates to sample-averaged photon fidelity characterization of cascaded emission efficiency and optical decoherence time. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.

cond-mat.mes-hall↗

arXiv2023

Giant room-temperature nonlinearities from a monolayer Janus topological semiconductor

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and topological properties, such as Berry curvature and the quantum metric tensor, have stimulated great interest. Here, we report giant room-temperature nonlinearities in an emergent non-centrosymmetric two-dimensional topological material, the Janus transition metal dichalcogenides in the 1T' phase, which are synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently reveal orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities of 1T' MoSSe (e.g., > 50 times higher than 2H MoS$_2$ for 18th order harmonic generation; > 20 times higher than 2H MoS$_2$ for terahertz emission). It is elucidated that such colossal nonlinear optical responses come from topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and preludes the applications of topological materials in optoelectronics down to the monolayer limit. This two-dimensional form of topological materials also constitute a unique platform for examining origin of the anomalous high-harmonic generation, with potential applications as building blocks for scalable attosecond sources.

cond-mat.mes-hall↗

arXiv2023

Determination of nonthermal bonding origin of a novel photoexcited lattice instability in SnSe

Interatomic forces that bind materials are largely determined by an often complex interplay between the electronic band-structure and the atomic arrangements to form its equilibrium structure and dynamics. As these forces also determine the phonon dispersion, lattice dynamics measurements are often crucial tools for understanding how materials transform between different structures. This is the case for the mono-chalcogenides which feature a number of lattice instabilities associated with their network of resonant bonds and a large tunability in their functional properties. SnSe hosts a novel lattice instability upon above-bandgap photoexcitation that is distinct from the distortions associated with its high temperature phase transition, demonstrating that photoexcitation can alter the interatomic forces significantly different than thermal excitation. Here we report decisive time-resolved X-ray scattering-based measurements of the nonequlibrium lattice dynamics in SnSe. By fitting interatomic force models to the excited-state dispersion, we determine this instability as being primarily due to changes in the fourth-nearest neighbor bonds that connect bilayers, with relatively little change to the intralayer resonant bonds. In addition to providing critical insight into the nonthermal bonding origin of the instability in SnSe, such measurements will be crucial for understanding and controlling materials properties under non-equilibrium conditions.

cond-mat.mtrl-sci↗

arXiv2022

Accelerating quantum materials development with advances in transmission electron microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, quantum dots, color center hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the materials detailed atomic scale structure, including atomic defects, dopants, and lattice stacking. In this review, after introduction of different classes of quantum materials and quantum excitations, we describe how progress in the field of electron microscopy, including in situ and in operando EM, can accelerate advances in quantum materials. Our review describes EM methods including: i) principles and operation modes of EM, ii) EM spectroscopies, such as electron energy loss spectroscopy, cathodoluminescence, and electron energy gain spectroscopy, iii) 4D scanning transmission electron microscopy, iv) dynamic and ultrafast EM, v) complimentary ultrafast spectroscopies, and vi) atomic electron tomography. We discuss how these methods inform structure function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable high resolution manipulation of quantum materials. Among numerous results, our review highlights how EM has enabled identification of the 3D structure of quantum defects, measuring reversible and metastable dynamics of quantum excitations, mapping exciton states and single photon emission, measuring nanoscale thermal transport and coupled excitation dynamics, and measuring the internal electric field of quantum heterointerfaces, all at the quantum materials intrinsic atomic and near atomic-length scale.

cond-mat.mtrl-sci↗