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At least 145 records · Page 8

Dynamically patterning x-ray beam by a femtosecond optical laser

Modern science and technology have greatly benefitted from our ability to precisely manipulate light waves, in both their spatial and temporal degrees of freedom. In the x-ray region, however, spatial control has been virtually static mainly due to stringent requirements for realizing high-performance optical elements. The lack of dynamic spatial control of x-ray beam has prevented researchers from realizing more sophisticated use of the wave field, which has rapidly advanced in the optical region in the past decades. In this study, we propose a practical scheme to dynamically control local x-ray reflectivity of a perfect silicon crystal by a femtosecond optical laser and demonstrate a programmable spatial x-ray modulator. Our modulator aims for spatial manipulation of the x-ray amplitude and is shown to produce arbitrary grayscale patterns with spatial frequencies up to 25 per millimeter. The proposed modulation scheme opens up a platform to enable advanced x-ray sensing and imaging techniques that can fully harness the wave nature of x-rays.

47 OTHER INSTRUMENTATION↗

Nanoscale ultrafast lattice modulation with a free-electron laser

Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. Finally, these results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.

nonlinear optics↗

Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO 3 Thin Films

The search for thin film electro-optic materials that can retain superior performance under cryogenic conditions has become critical for quantum computing. Barium titanate thin films show large linear electro-optic coefficients in the tetragonal phase at room temperature, which is severely degraded down to ≈200 pm V −1 in the rhombohedral phase at cryogenic temperatures. There is immense interest in manipulating these phase transformations and retaining superior electro-optic properties down to liquid helium temperature. Utilizing the thermodynamic theory of optical properties, a large low-temperature electro-optic response is designed by engineering the energetic competition between different ferroelectric phases, leading to a low-symmetry monoclinic phase with a massive electro-optic response. The existence of this phase is demonstrated in a strain-tuned BaTiO 3 thin film that exhibits a linear electro-optic coefficient of 2516 ± 100 pm V −1 at 5 K, which is an order of magnitude higher than the best reported performance thus far. Importantly, the electro-optic coefficient increases by 100 × during cooling, unlike the conventional films, where it degrades. Further, at the lowest temperature, significant higher order electro-optic responses also emerge. These results represent a new framework for designing materials with property enhancements by stabilizing highly tunable metastable phases with strain.

barium titanate↗

Stable Non-equilibrium Structures in Chiral Nematics under Microfluidic Flow

Cholesteric liquid crystals (CLCs) are compelling responsive materials with applications in next-generation sensing, imaging, and display technologies. While electric fields and surface treatments have been used to manipulate the molecular organization and, subsequently, the optical properties of CLCs, their response to controlled fluid flow has remained largely unexplored. Here, in this study, we investigate the influence of microfluidic flow on the structure of thermotropic CLCs that can exhibit structural coloration. We demonstrate that the shear forces that arise from microfluidic flow align the helical axis of CLCs; alignment is a prerequisite for harnessing the promising photonic properties of CLCs. Moreover, we show that microfluidic flow can generate non-equilibrium structures exhibiting photonic band gaps that are inaccessible in the stationary cholesteric phase. Our findings have implications for the use of CLCs in applications involving flow processing such as additive manufacturing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Infrared nano-imaging of Dirac magnetoexcitons in graphene

Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional electron systems subject to strong magnetic fields are expected to exhibit quantized Hall conductivity, chiral edge currents and distinctive collective modes referred to as magnetoplasmons and magnetoexcitons. Generating these propagating collective modes in charge-neutral samples and imaging them at their native nanometre length scales have thus far been experimentally elusive. Here we visualize propagating magnetoexciton polaritons at their native length scales and report their magnetic-field-tunable dispersion in near-charge-neutral graphene. Imaging these collective modes and their associated nano-electro-optical responses allows us to identify polariton-modulated optical and photo-thermal electric effects at the sample edges, which are the most pronounced near charge neutrality. Our work is enabled by innovations in cryogenic near-field optical microscopy techniques that allow for the nano-imaging of the near-field responses of two-dimensional materials under magnetic fields up to 7 T. In conclusion, this nano-magneto-optics approach allows us to explore and manipulate magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

36 MATERIALS SCIENCE↗

Proton beam quality enhancement by spectral phase control of a PW-class laser system

We report on experimental investigations of proton acceleration from solid foils irradiated with PW-class laser-pulses, where highest proton cut-off energies were achieved for temporal pulse parameters that varied significantly from those of an ideally Fourier transform limited (FTL) pulse. Controlled spectral phase modulation of the driver laser by means of an acousto-optic programmable dispersive filter enabled us to manipulate the temporal shape of the last picoseconds around the main pulse and to study the effect on proton acceleration from thin foil targets. The results show that applying positive third order dispersion values to short pulses is favourable for proton acceleration and can lead to maximum energies of 70 MeV in target normal direction at 18 J laser energy for thin plastic foils, significantly enhancing the maximum energy compared to ideally compressed FTL pulses. The paper further proves the robustness and applicability of this enhancement effect for the use of different target materials and thicknesses as well as laser energy and temporal intensity contrast settings. We demonstrate that application relevant proton beam quality was reliably achieved over many months of operation with appropriate control of spectral phase and temporal contrast conditions using a state-of-the-art high-repetition rate PW laser system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Hidden phonon highways promote photoinduced interlayer energy transfer in twisted transition metal dichalcogenide heterostructures

Vertically stacked van der Waals (vdW) heterostructures exhibit unique electronic, optical, and thermal properties that can be manipulated by twist-angle engineering. However, the weak phononic coupling at a bilayer interface imposes a fundamental thermal bottleneck for future two-dimensional devices. Using ultrafast electron diffraction, we directly investigated photoinduced nonequilibrium phonon dynamics in MoS 2 /WS 2 at 4° twist angle and WSe 2 /MoSe 2 heterobilayers with twist angles of 7°, 16°, and 25°. We identified an interlayer heat transfer channel with a characteristic timescale of ~20 picoseconds, about one order of magnitude faster than molecular dynamics simulations assuming initial intralayer thermalization. Atomistic calculations involving phonon-phonon scattering suggest that this process originates from the nonthermal phonon population following the initial interlayer charge transfer and scattering. Our findings present an avenue for thermal management in vdW heterostructures by tailoring nonequilibrium phonon populations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Trapped-ion quantum simulation of electron transfer models with tunable dissipation

Electron transfer is at the heart of many fundamental physical, chemical, and biochemical processes essential for life. The exact simulation of these reactions is often hindered by the large number of degrees of freedom and by the essential role of quantum effects. Here, we experimentally simulate a paradigmatic model of molecular electron transfer using a multispecies trapped-ion crystal, where the donor-acceptor gap, the electronic and vibronic couplings, and the bath relaxation dynamics can all be controlled independently. By manipulating both the ground-state and optical qubits, we observe the real-time dynamics of the spin excitation, measuring the transfer rate in several regimes of adiabaticity and relaxation dynamics. Our results provide a testing ground for increasingly rich models of molecular excitation transfer processes that are relevant for molecular electronics and light-harvesting systems.

Science & Technology - Other Topics↗

Exploring and Embracing Heterogeneity in Atomically Thin Energy Materials

Atomically thin semiconductors offer extraordinary opportunities for the manipulation of charge carriers, many-body optical excitations, quantum light emitters, and non-charge based quantum numbers. Confinement and reduced dielectric screening in these two-dimensional (2D) materials give rise to large characteristic energies so that many-body and quantum effects are important even at room temperature. Optical excitations in extended homogeneous areas have been investigated intensely, albeit mostly focusing on a limited set of materials, particularly transition metal dichalcogenides. Much less understood are light-matter interactions for other classes of 2D semiconductors, as well as effects that arise in heterogeneous materials, either near naturally occurring defects, impurities, edges and grain boundaries, or as a result of intentional interface formation in heterostructures. Addressing such systems experimentally involves significant challenges: Understanding the atomistic growth mechanisms of 2D semiconductors, so that novel systems with designed properties, specific ‘imperfections’, or controlled interfaces can be realized; and probing of local excitations at scales that match the relevant (micrometer to nanometer) length scales in heterogeneous materials. In this research project, we addressed these challenges by harnessing quantitative in-situ microscopy to study the growth of 2D and layered semiconductors and heterostructures, combined with local spectroscopic measurements of quasiparticles excited at the nanometer scale. An integral part of the research has been the development of novel experimental approaches, both for in-situ microscopy of synthesis and for nanometer-scale spectroscopy. In particular, advanced techniques were developed for cathodoluminescence in scanning transmission electron microscopy (STEM-CL) where a nanometer-focused electron beam is used to locally excite electron-hole pairs, excitons, as well as propagating hybrid light-matter modes such as exciton-polaritons. Experiments were guided and analyzed via computations of structure, chemistry, and excitation spectra. The particular materials focus has been on group IV chalcogenides, a family of less explored 2D/layered semiconductors whose diversity in crystal structure and properties promises access to novel materials architectures and the discovery of phenomena that can support emerging technology needs.

36 MATERIALS SCIENCE↗

Dielectric Resonator Design for Low Power and Low Temperature Microwave Plasma

Waveguide-based microwave plasmas generally operate at high temperatures (2000 - 6000K)[1], making it difficult to directly interface solid materials with the plasma without significant thermal damage. Dielectric microwave resonators (DMRs), long studied for wave-based manipulation of electromagnetic radiation for telecom and optics, can focus radiation to extremely small mode volumes, creating intense localized fields with low-power input.[2] This phenomenon can be used for applications ranging from efficient plasma electronics to near-ambient plasma-materials interactions. Such DMR-based plasmas have been demonstrated a handful of times in the literature, but the majority of research towards this utilize the lowest frequency resonance mode.[3], [4], [5] By carefully controlling the geometry of cylindrical resonators, a variety of electromagnetic modes can be excited. In this work, COMSOL Multiphysics simulations are used to study the electric field enhancement and absorption properties of CaTiO3 DMRs as a function of geometry and excitation frequency. Whereas previous studies have utilized the HEM111 resonance frequency to drive low power plasma excitation, we find that higher order resonance frequencies are more effective at field enhancement and result in less power loss within the dielectric material, hence less wasted heating. The effectiveness of these modes is also geometry dependent and can be computationally optimized for plasma generation. Complementing these computational efforts, we demonstrate a new closed-system reactor design built in a WR-650 waveguide and experimentally demonstrate the formation of atmospheric argon microwave plasma using < 30 W input power on DMR dimers. We observe a shifting resonance frequency as the DMRs heat in response to microwave excitation and develop a Python-based lock-in mechanism to effectively track the DMR resonance over time, leading to stable plasma operation. We use infrared thermal imaging to monitor the temperature of the DMR dimers and surrounding quartz chamber, demonstrating thermal temperatures < 60 degreesC. Finally, we utilize optical emission spectroscopy (OES) to probe the plasma properties as a function of the resonance mode.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Manipulation of quantum dot emission with semiconductor metasurfaces exhibiting magnetic quadrupole resonances

Optical metasurfaces were suggested as a route for engineering advanced light sources with tailored emission properties. In particular, they provide a control over the emission directionality, which is essential for single-photon sources and LED applications. Here, we experimentally study light emission from a metasurface composed of III-V semiconductor Mie-resonant nanocylinders with integrated quantum dots (QDs). Specifically, we focus on the manipulation of the directionality of spontaneous emission from the QDs due to excitation of different magnetic quadrupole resonances in the nanocylinders. To this end, we perform both back focal plane imaging and momentum-resolved spectroscopy measurements of the emission. This allows for a comprehensive analysis of the effect of the different resonant nanocylinder modes on the emission characteristics of the metasurface. Our results show that the emission directionality can be manipulated by an interplay of the excited quadrupolar nanocylinder modes with the metasurface lattice modes and provide important insights for the design of novel smart light sources and new display concepts.

Vaskin, Aleksandr↗

Control of valley polarization in gapped graphene by linearly polarized ultrashort optical pulse

We present a versatile model of gapped graphene to manipulate valley polarization by using ultrafast linearly polarized pulses of zero areas. First, a circularly polarized pulse of a single oscillation produces a valley-selective population of the conduction band by means of topological resonance. Then we apply a linearly polarized femtosecond-long pulse that changes the valley polarization. The magnitude of such a change depends on the amplitude and the direction of polarization of the pulse. In conclusion, our protocol provides a favorable platform for applications in valleytronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Polarization–frequency hyperentangled photons: generation, characterization, and manipulation

Frequency-bin encoding is massively parallelizable and robust for optical fiber transmission. When coupled with an additional degree of freedom (DoF), the expansion of the Hilbert space allows for deterministic controlled operations between two DoFs within a single photon. Such capabilities, when combined with photonic hyperentanglement, are of great value for quantum communication protocols, including dense coding and single-copy entanglement distillation. In this talk, we present an all-fiber-coupled, ultrabroadband polarization–frequency hyperentangled source and conduct comprehensive quantum state tomography across multiple dense wavelength division multiplexing channels spanning the optical C+L-band (1530–1625 nm). In addition, we design and implement a high-fidelity controlled-NOT (cnot) operation between polarization and frequency DoFs by exploiting electro-optic phase modulation within a fiber Sagnac loop. Collectively, our hyperentangled source and two-qubit gate should unlock new opportunities for harnessing polarization–frequency resources in established telecommunication fiber networks for future quantum applications.

Lu, Hsuan-Hao↗

Optically controlled single-valley exciton doublet states with tunable internal spin structures and spin magnetization generation

Manipulating quantum states through light–matter interactions has been actively pursued in two-dimensional materials research. Significant progress has been made toward the optical control of the valley degrees of freedom in semiconducting monolayer transition-metal dichalcogenides, based on doubly degenerate excitons from their two distinct valleys in reciprocal space. Here, we introduce a type of optically controllable doubly degenerate exciton states that come from a single valley, dubbed as single-valley exciton doublet (SVXD) states. They are unique in that their constituent holes originate from the same valence band, making possible the direct optical control of the spin structure of the excited constituent electrons. Combining ab initio GW plus Bethe–Salpeter equation ( GW -BSE) calculations and a theoretical analysis method, we demonstrate such SVXD in substrate-supported monolayer bismuthene—which has been successfully grown using molecular beam epitaxy. In each of the two distinct valleys in the Brillouin zone, strong spin–orbit coupling and C 3 v symmetry lead to a pair of degenerate 1s exciton states (the SVXD states) with opposite spin configurations. Any coherent linear combinations of the SVXD in a single valley can be excited by light with a specific polarization, enabling full manipulation of their internal spin configurations. In particular, a controllable net spin magnetization can be generated through light excitation. Our findings open routes to control quantum degrees of freedom, paving the way for applications in spintronics and quantum information science.

2D materials↗

Selective and Scalable Control of Spin Quantum Memories in a Photonic Circuit

A central goal in many quantum information processing applications is a network of quantum memories that can be entangled with each other while being individually controlled and measured with high fidelity. This goal has motivated the development of programmable photonic integrated circuits (PICs) with integrated spin quantum memories using diamond color center spin-photon interfaces. However, this approach introduces a challenge into the microwave control of individual spins within closely packed registers. Here, we present a quantum memory-integrated photonics platform capable of (i) the integration of multiple diamond color center spins into a cryogenically compatible, high-speed programmable PIC platform, (ii) selective manipulation of individual spin qubits addressed via tunable magnetic field gradients, and (iii) simultaneous control of qubits using numerically optimized microwave pulse shaping. The combination of localized optical control, enabled by the PIC platform, together with selective spin manipulation opens the path to scalable quantum networks on intrachip and interchip platforms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

All-optical seeding of a light-induced phase transition with correlated disorder

Ultrafast manipulation of vibrational coherence is an emergent route to control the structure of solids. However, this strategy can only induce long-range correlations and cannot modify atomic structure locally, which is required in many technologically-relevant phase transitions. Here, we demonstrate that ultrafast lasers can generate incoherent structural fluctuations which are more efficient for material control than coherent vibrations, extending optical control to a wider range of materials. We observe that local, non-equilibrium lattice distortions generated by a weak laser pulse reduce the energy barrier to switch between insulating and metallic states in vanadium dioxide by 6%. In conclusion, seeding inhomogeneous structural-fluctuations presents an alternative, more energy efficient, route for controlling materials that may be applicable to all solids, including those used in data and energy storage devices.

36 MATERIALS SCIENCE↗

Optical polarization analogs in inelastic free-electron scattering

Advances in the ability to manipulate free-electron phase profiles within the electron microscope have spurred development of quantum-mechanical descriptions of electron energy loss (EEL) processes involving transitions between phase-shaped transverse states. Here, we elucidate an underlying connection between two ostensibly distinct optical polarization analogs identified in EEL experiments as manifestations of the same conserved scattering flux. Our work introduces a procedure for probing general tensorial target characteristics including global mode symmetries and local polarization.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

A versatile high-speed x-ray microscope for sub-10 nm imaging

We have developed a next-generation scanning x-ray microscope RASMI (RApid Scanning Microscopy Instrument) for high-throughput tomographic imaging. RASMI is installed at the hard x-ray nanoprobe beamline at NSLS-II and is capable of manipulating 1D multilayer Laue lenses (MLLs) and 2D optics (both zone plates and monolithically assembled 2D MLLs). The sample scanning stage utilizes line-focusing interferometry as an encoder while performing fly-scanning data acquisition. The system can be configured for both position- and time-triggering modes during fly-scanning. The microscope demonstrated a detector-limited data acquisition rate of 1.25 kHz during ptychography measurements. The initial x-ray results yielded a sample-limited resolution of ∼6 nm in 2D. RASMI can be adopted for in-vacuum applications and is a foundation for the next-generation scanning microscopy systems to be developed and commissioned at NSLS-II.

36 MATERIALS SCIENCE↗