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At least 253 records · Page 14

Visible-to-THz near-field nanoscopy

Optical microscopy has a key role in research, development and quality control across a wide range of scientific, technological and medical fields. However, diffraction limits the spatial resolution of conventional optical instruments to about half the illumination wavelength. A technique that surpasses the diffraction limit in the wide spectral range between visible and terahertz frequencies is scattering-type scanning near-field optical microscopy (s-SNOM). The basis of s-SNOM is an atomic force microscope in which the tip is illuminated with light from the visible to the terahertz spectral range. By recording the elastically tip-scattered light while scanning the sample below the tip, s-SNOM yields near-field optical images with a remarkable resolution of 10 nm, simultaneously with the standard atomic force microscopic topography image. This resolution is independent of the illumination wavelength, rendering s-SNOM a versatile nanoimaging and nanospectroscopy technique for fundamental and applied studies of materials, structures and phenomena. This Review presents an overview of the fundamental principles governing the measurement and interpretation of near-field contrasts and discusses key applications of s-SNOM. We also showcase emerging developments that enable s-SNOM to operate under various environmental conditions, including cryogenic temperatures, electric and magnetic fields, electrical currents, strain and liquid environments. Furthermore, all these recent developments broaden the applicability of s-SNOMs for exploring fundamental solid-state and quantum phenomena, biological matter, catalytic reactions and more.

Hillenbrand, Rainer [CIC nanoGUNE BRTA and Departm↗

Mixed stochastic-deterministic density functional theoretic decomposition of Kubo–Greenwood conductivities in the projector augmented wave formalism

Pairing the accuracy of the Kohn–Sham density-functional framework with the efficiency of a stochastic algorithmic approach, mixed stochastic-deterministic density functional theory (mDFT) achieves a favorable computational scaling with system sizes and electronic temperatures. We employ the recently developed mDFT formalism to investigate the dynamic charge-transport properties of systems in the warm dense matter regime. The optical conductivity spectra are computed for single- and multi- component mixtures of carbon, hydrogen, and beryllium using two complementary approaches: Kubo–Greenwood in the mDFT picture and real-time time-dependent mDFT. We further devise a decomposition of the Onsager coefficients leading up to the Kubo–Greenwood spectra to exhibit contributions from the deterministic, stochastic, and mixed electronic state transitions at different incident photon energies.

36 MATERIALS SCIENCE↗

Purcell-Enhanced Emissions from Diamond Color Centers in Slow Light Photonic Crystal Waveguides

Diamond color centers are promising candidates for optically addressable quantum memories, which motivates the development of efficient photonic interfaces, often using nanophotonic cavities with narrow spectral line widths and small mode volumes. However, they require perfect spectral and spatial overlap between the cavity mode and quantum emitter, which is challenging. This is especially true for solid-state quantum emitters that are often randomly positioned and suffer from inhomogeneous broadening. Another approach to enhance light-matter interaction across large optical bandwidths and areas is using slow light waveguides. Here, in this study, we demonstrate diamond slow light photonic crystal (PhC) waveguides optically coupled to embedded silicon-vacancy (SiV) color centers. We use the recently developed thin-film diamond approach to fabricate fully suspended two-dimensional PhC waveguides. We demonstrate waveguide modes with high group indices up to 70 and observe Purcell-enhanced emissions of the SiVs. Our approach represents a practical diamond platform for robust spin-photon interfaces with color centers.

2D photonic crystal waveguide↗

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Extreme terahertz magnon multiplication induced by resonant magnetic pulse pairs

Nonlinear interactions of spin-waves and their quanta, magnons, have emerged as prominent candidates for interference-based technology, ranging from quantum transduction to antiferromagnetic spintronics. Yet magnon multiplication in the terahertz (THz) spectral region represents a major challenge. Intense, resonant magnetic fields from THz pulse-pairs with controllable phases and amplitudes enable high order THz magnon multiplication, distinct from non-resonant nonlinearities such as the high harmonic generation by below-band gap electric fields. Here, we demonstrate exceptionally high-order THz nonlinear magnonics. It manifests as 7th-order spin-wave-mixing and 6th harmonic magnon generation in an antiferromagnetic orthoferrite. We use THz two-dimensional coherent spectroscopy to achieve high-sensitivity detection of nonlinear magnon interactions up to six-magnon quanta in strongly-driven many-magnon correlated states. The high-order magnon multiplication, supported by classical and quantum spin simulations, elucidates the significance of four-fold magnetic anisotropy and Dzyaloshinskii-Moriya symmetry breaking. Moreover, our results shed light on the potential quantum fluctuation properties inherent in nonlinear magnons.

36 MATERIALS SCIENCE↗

Electronic Spin Relaxation and Clustering in High-Pressure High-Temperature Synthesized Microcrystalline Diamond Particles with Reduced Nitrogen Content

The negatively charged nitrogen-vacancy (NV – ) color center in diamonds is widely studied because of numerous applications of this unique quantum system in sensing and quantum information sciences. While substitutional nitrogen is required to form the NV – centers in diamond, it also yields other paramagnetic defects─primarily the neutrally charged substitutional nitrogen centers (P1)─that decrease NV – spin coherence, which in turn degrades performance in applications. Herein, we investigate high-pressure high-temperature synthesized diamond microparticles (ca. 140–185 μm) having lower─ranging from 3 to 38 ppm─than the typical nitrogen content of type 1b diamond ( ca. 100 ppm and higher) typically used for the production of fluorescent diamond particles with NV – centers. A suite of electron paramagnetic resonance, optically detected magnetic resonance, and nuclear magnetic resonance methods are used to characterize spin properties of P1 and NV – centers in the particles. Upon decreasing the nitrogen content from 29 to 3 ppm, the ensemble NV – T 2 relaxation time increased by about 3-fold as measured directly in the Hahn Echo experiment at magnetic field of 1.2 T. Analysis of electronic relaxation of P1 centers revealed the existence of at least two distinct populations of P1 centers, consisting of fast and slower relaxing spins and allowed for an estimation of local concentrations. Even with <10 ppm nitrogen contents, the analysis indicated a highly heterogeneous distribution of P1 centers, suggesting the possibility of P1 spin clustering even at low nitrogen concentrations. The combined data demonstrate that the particles prepared from HPHT diamond with a low nitrogen content offer improved spin properties that are beneficial for NV – sensing applications.

Carbon↗

Coherent phonon flatband generated in GaAs/AlAs superlattices via layer-selective optical pumping

Flatbands, characterized by their dispersionless energy levels in electronic, magnetic, and phononic systems, hold substantial potential for advancements in electronics and quantum information processing. Most flatbands exist in thermal equilibrium and cannot be easily created or annihilated externally, limiting their flexibility as switchable knobs for use in microelectronics and quantum applications. In our work, we demonstrate the generation of a coherent phonon flatband in a GaAs/AlAs superlattice using 800 nm femtosecond laser pulses. This coherent phonon flatband does not correspond to a phonon eigenmode at equilibrium and exhibits strong coupling with two branches of coherently excited longitudinal phonon modes. With molecular dynamics simulations, we show more generally that the coherent phonon flatband can be induced by coherently and spatially modulated optical excitations of superlattice structures. Our results highlight a pathway for coherent phonon flatband creation in the time domain that can be generalized to various superlattice systems, potentially inspiring the realization of coherent flatband generation of other quasiparticles.

Condensed-matter physics↗

Full complex amplitude control of second-harmonic generation via electrically tunable intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces based on coupling of the intersubband nonlinear optical response of quantum-engineered semiconductor heterostructures and electromagnetic modes of nanoresonators provide efficient frequency mixing with moderate pump intensities. The resonant nonlinear optical response, represented as a complex function, can be modulated via Stark tuning of intersubband transition energies under applied voltages. However, achieving full complex amplitude control (both phase and magnitude) remains challenging. In this work, we present and experimentally validate electrically tunable nonlinear intersubband polaritonic metasurfaces that achieve complete complex amplitude control for second-harmonic generation (SHG). Through a design featuring two in-plane flipped meta-atoms per unit cell, we achieve complete electrical control of both the amplitude and phase of the metasurface second-order nonlinear susceptibility, with a tuning range of 0 to 30 nm V −1 for the magnitude and 0-2π for the phase of the nonlinear optical response. Using these properties, we achieve complete on-off SHG modulation and beam diffraction tuning through electrically controlled amplitude and phase gratings.

Science & Technology - Other Topics↗

Photo‐Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room‐Temperature Diamond

Abstract The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV 0 to SiV ‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV ‒ , on the other hand, yields only fractional recombination into SiV 2‒ , a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simulating nonlinear optical processes on a superconducting quantum device

Simulating plasma physics on quantum computers is difficult because most problems of interest are nonlinear, but quantum computers are not naturally suitable for nonlinear operations. In weakly nonlinear regimes, plasma problems can be modelled as wave–wave interactions. In this paper, we develop a quantization approach to convert nonlinear wave–wave interaction problems to Hamiltonian simulation problems. We demonstrate our approach using two qubits on a superconducting device. Unlike a photonic device, a superconducting device does not naturally have the desired interactions in its native Hamiltonian. Nevertheless, Hamiltonian simulations can still be performed by decomposing required unitary operations into native gates. To improve experimental results, we employ a range of error-mitigation techniques. Apart from readout error mitigation, we use randomized compilation to transform undiagnosed coherent errors into well-behaved stochastic Pauli channels. Moreover, to compensate for stochastic noise, we rescale exponentially decaying probability amplitudes using rates measured from cycle benchmarking. We carefully consider how different choices of product-formula algorithms affect the overall error and show how a trade-off can be made to best utilize limited quantum resources. This study provides an example of how plasma problems may be solved on near-term quantum computing platforms.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Two-Dimensional Ferroelectric Altermagnets: From Model to Material Realization

Multiferroic altermagnets offer new opportunities for magnetoelectric coupling and electrically tunable spintronics. However, due to intrinsic symmetry conflicts between altermagnetism and ferroelectricity, achieving their coexistence, known as ferroelectric altermagnets (FEAM), remains an outstanding challenge, especially in two-dimensional (2D) systems. Here, we propose a universal, symmetry-based design principle for 2D FEAM, supported by tight-binding models and first-principles calculations. We show that lattice distortions can break spin equivalence and introduce the necessary rotation-related symmetry, enabling altermagnetism with electrically reversible spin splitting. Guided by this framework, we identify a family of 2D vanadium oxyhalides and sulfide halides as promising FEAM candidates. In these compounds, pseudo Jahn-Teller distortions and Peierls-like dimerization cooperatively establish the required symmetry conditions. Here, we further propose the magneto-optical Kerr effect as an experimental probe to confirm FEAM and its electric spin reversal. Furthermore, our findings provide a practical framework for 2D FEAM and advancing electrically controlled spintronic devices.

2D materials↗

Cyclotron resonance in a kagome spin liquid candidate material

We propose cyclotron resonance as an optical probe for emergent fractionalized excitations in U⁡(1) quantum spin liquids, focusing on kagome antiferromagnets. In contrast to conventional systems, where cyclotron resonance directly couples to charged carriers, spinons in spin liquids are charge-neutral and interact only through an emergent gauge field, making direct probing challenging. We identify two key mechanisms by which an external physical electromagnetic field induces emergent electric and magnetic fields, enabling indirect coupling to spinons. Using these mechanisms, we compute the absorption rate of the cyclotron resonance response for Dirac spinons forming Landau levels. Our analysis shows that, although the absorption per layer is small, the absence of a skin-depth limitation in insulating spin liquids allows for cumulative absorption comparable to graphene in realistic sample sizes for the recently discovered spin-liquid candidate material YCu 3⁢ (OH) 6⁢ Br 2 ⁢[Br 1−𝑦 ⁢(OH) 𝑦 ]. Furthermore, our proposed cyclotron-resonance measurement is a decisive, practical test for spinon Landau levels, providing quantitative expectations where clear experimental evidence has so far been lacking.

Dzyaloshinskii-Moriya interaction↗

Coherent charge hopping suppresses photoexcited small polarons in ErFeO 3 by antiadiabatic formation mechanism

Polarons are prevalent in condensed matter systems with strong electron-phonon coupling. The adiabaticity of the polaron relates to its transport properties and spatial extent. To date, only adiabatic small polaron formation has been measured following photoexcitation. The lattice reorganization energy is large enough that the first electron–optical phonon scattering event creates a small polaron without requiring substantial carrier thermalization. We measure that frustrating the iron-centered octahedra in the rare-earth orthoferrite ErFeO 3 leads to antiadiabatic polaron formation. Coherent charge hopping between neighboring Fe 3+ –Fe 2+ sites is measured with transient extreme ultraviolet spectroscopy and lasts several picoseconds before the polaron forms. The resulting small polaron formation time is an order of magnitude longer than previous measurements and indicates a shallow potential well, even in the excited state. The results emphasize the importance of considering dynamic electron-electron correlations, not just electron-phonon–induced lattice changes, for small polarons for transport, catalysis, and photoexcited applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Transverse orbital angular momentum and polarization entangled spatiotemporal structured light

Intra-system entanglement occurs between non-separable modes within the same system. For optical systems, the various degrees of freedom of light represent different modes, and the potential use of light to create higher dimensional classical entangle states offers a promising potential to drive new technological developments. In this work, we present experimental results demonstrating the orthogonality between transverse orbital angular momentum (t-OAM) of different spatiotemporal topological charges, a previously unverified property of t-OAM. Based on those results, we developed methods to create and characterize a novel family of t-OAM and polarization entangled spatiotemporal structured light. We further provide theoretical analysis to support our study of the entanglement between those modes. By demonstrating the feasibility of leveraging t-OAM as a new family of modes for classical entanglement, our work represents a new advancement towards higher dimensional classical entanglement strategies.

42 ENGINEERING↗

Search for 3D topological superconductors using laser-based spectroscopy (Final Technical Report)

The three-dimensional topological superconductor (3D TSC) is a novel quantum phase of matter that is predicted to exhibit exotic thermal and electrical properties, which may serve applications ranging from precision thermal management and sensing technologies to fault-tolerant quantum information processing. Over the past decade, there has been an intensive effort to realize 1D and 2D TSCs by artificially engineering them from combinations of already existing materials. For example, coupling conventional superconductors to spin-orbit coupled 1D nanowires or to 2D topological insulator surfaces by the proximity effect provides a route to realizing 1D and 2D TSCs respectively. However no artificial engineering strategy is available for a 3D TSC. Therefore, current searches are limited to intrinsically superconducting compounds whose topological properties are difficult to predict. The overarching goal of this project was to realize and to identify 3D TSCs in bulk single crystals using novel laser-based spectroscopic techniques. One major thrust was to develop ultralow temperature and ultra-high-resolution angle-resolved photoemission spectroscopy (ARPES) to directly measure the dispersion of Majorana excitations that are predicted to exist on the surfaces of 3D TSCs. Another major thrust was to develop a rational route to realize 3D TSCs by identifying their precursor phases. It is theoretically proposed that the critical fluctuations of certain ordered electronic phases can mediate Cooper pairing in odd-parity channels and lead to topological superconductivity. Therefore, 3D TSCs may potentially emerge upon suppressing these inversion symmetry broken precursor phases to a critical point with external perturbations such as pressure, strain or even light. To test this hypothesis, we studied candidate materials using a suite of symmetry-sensitive optical probes including rotational anisotropy optical second harmonic generation (RA-SHG) and time-resolved coherent phonon spectroscopy, all operable under high-pressure and low temperature environments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Time-of-flight detection of terahertz phonon-polariton

A polariton is a fundamental quasiparticle that arises from strong light-matter interaction and as such has attracted wide scientific and practical interest. When light is strongly coupled to the crystal lattice, it gives rise to phonon-polaritons (PPs), which have been proven useful in the dynamical manipulation of quantum materials and the advancement of terahertz technologies. Yet, current detection and characterization methods of polaritons are still limited. Traditional techniques such as Raman or transient grating either rely on fine-tuning of external parameters or complex phase extraction techniques. To overcome these inherent limitations, we propose and demonstrate a technique based on a time-of-flight measurement of PPs. We resonantly launch broadband PPs with intense terahertz fields and measure the time-of-flight of each spectral component with time-resolved second harmonic generation. The time-of-flight information, combined with the PP attenuation, enables us to resolve the real and imaginary parts of the PP dispersion relation. We demonstrate this technique in the van der Waals magnets NiI 2 and MnPS 3 and reveal a hidden magnon-phonon interaction. We believe that this approach will unlock new opportunities for studying polaritons across diverse material systems and enhance our understanding of strong light-matter interaction.

condensed-matter physics↗

Indistinguishable photons from an artificial atom in silicon photonics

Silicon is the ideal material for building electronic and photonic circuits at scale. Integrated photonic quantum technologies in silicon offer a promising path to scaling by leveraging advanced semiconductor manufacturing and integration capabilities. However, the lack of deterministic quantum light sources and strong photon-photon interactions in silicon poses a challenge to scalability. In this work, we demonstrate an indistinguishable photon source in silicon photonics based on an artificial atom. We show that a G center in a silicon waveguide can generate high-purity telecom-band single photons. We perform high-resolution spectroscopy and time-delayed two-photon interference to demonstrate the indistinguishability of single photons emitted from a G center in a silicon waveguide. Our results show that artificial atoms in silicon photonics can source single photons suitable for photonic quantum networks and processors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Origin of reduced efficiency in GaN-based micro-LEDs studied by scanning near-field optical microscopy

The quantum efficiency of micro-light emitting diodes (micro-LEDs) is lower than that of large area LEDs. This efficiency reduction is typically attributed to the nonradiative Shockley–Read–Hall recombination at the surface defects and current leakage through the sidewall region without a clear distinction between these effects. In this work, we attempt to find out which of these phenomena is most critical for the reduced efficiency of micro-LEDs. This has been done by mapping electroluminescence (EL) and photoluminescence (PL) and measuring PL dynamics in blue GaN micro-LEDs fabricated by dry etching. It has been found that in the as-etched device, the EL intensity is much lower than in devices with KOH etching and atomic layer deposition of SiO 2 . This effect is especially pronounced close to the sidewalls. On the other hand, PL decay times are similar in as-etched and passivated devices, both in their center and at the sidewalls. This allows concluding that the main mechanism of the reduced efficiency of micro-LEDs fabricated by dry etching is the current leakage in the sidewall region and not the nonradiative recombination. The KOH etching has been found to be the most efficient means to eliminate the current leakage.

36 MATERIALS SCIENCE↗