Nonresonant Excitation Research Articles

Selection criteria of piezoelectric materials for double-parabolic-reflectors ultrasonic transducers (DPLUS) for high-power ultrasound

To suit double parabolic reflectors wave-guided ultrasonic transducer (DPLUS) for high-power ultrasound applications, we investigated the selection criteria of piezoelectric materials for DPLUS. Four piezoelectric materials were prepared: two lead–zirconate–titanate (PZT) types and two lead-free types. For non-resonant excitation of the DPLUS waveguide, the piezoelectric constant e and the thickness of piezoelectric materials are two important evaluation indexes. PZT 5H was found as the best candidate. For resonant excitation of the DPLUS waveguide, two situations should be distinguished. For low-frequency modes excitation, the discussed modes matching issue is essential. For high-frequency modes excitation, high-power properties of the piezoelectric material are important for improving the vibration output of DPLUS; LFP 0202 was found as the best candidate. Low-frequency modes can achieve 8 m s−1 of maximum peak vibration velocity, but high-frequency modes were smaller than 2 m s−1. Results are important to design the DPLUS for various high-power ultrasound applications.

Plasmonic Au Nanoparticle Arrays for Monitoring Photopolymerization at the Nanoscale

The localized surface plasmon resonance (LSPR) of Au nanoparticles (NPs) was used to monitor photopolymerization at the nanoscale by in situ monitoring the optical response of AuNPs during the light-induced polymerization process. To show the interest of this approach, two configurations were used, which correspond to a resonant and a nonresonant excitation regime between the photopolymer and the AuNPs used as nanoprobes. We show that not only this method enables the progress monitoring of the photopolymerization reaction at the nanometric scale but also can highlight the near-field coupling effect responsible for the acceleration of the photoinduced reaction. This methodology appears very interesting to study the photoinduced nanofabrication processes of metal/polymer hybrid nanoparticles and more globally to study the photopolymerization reactions at the nanometric scale.

Broadband SERS Enhancement by DNA Origami Assembled Bimetallic Nanoantennas with Label-Free Single Protein Sensing.

Engineering hotspots in surface-enhanced Raman spectroscopy (SERS) through precisely controlled assembly of plasmonic nanostructures capable of expanding intense field enhancement are highly desirable to enhance the potentiality of SERS as a label-free optical tool for single molecule detection. Inspired by DNA origami technique, we constructed plasmonic dimer nanoantennas with a tunable gap decorated with Ag-coated Au nanostars on origami. Herein, we demonstrate the single-molecule SERS enhancements of three dyes with emission in different spectral regions after incorporation of single dye molecules in between two nanostars. The enhancement factors (EFs) achieved in the range of 109-1010 for all the single dye molecules, under both resonant and nonresonant excitation conditions, would enable enhanced photostability during time-series measurement. We further successfully explored the potential of our designed nanoantennas to accommodate and detect a single thrombin protein molecule after selective placement in the wide nanogap of 10 nm. Our results suggest that such nanoantennas can serve as a broadband SERS enhancer and enable specific detection of target biological molecules with single-molecule sensitivity.

Topological phase transition in an all-optical exciton-polariton lattice

Topological insulators are a class of electronic materials exhibiting robust edge states immune to perturbations and disorder. This concept has been successfully adapted in photonics, where topologically nontrivial waveguides and topological lasers were developed. However, the exploration of topological properties in a given photonic system is limited to a fabricated sample, without the flexibility to reconfigure the structure in situ. Here, we demonstrate an all-optical realization of the orbital Su–Schrieffer–Heeger model in a microcavity exciton-polariton system, whereby a cavity photon is hybridized with an exciton in a GaAs quantum well. We induce a zigzag potential for exciton polaritons all-optically by shaping the nonresonant laser excitation, and measure directly the eigenspectrum and topological edge states of a polariton lattice in a nonlinear regime of bosonic condensation. Furthermore, taking advantage of the tunability of the optically induced lattice, we modify the intersite tunneling to realize a topological phase transition to a trivial state. Our results open the way to study topological phase transitions on-demand in fully reconfigurable hybrid photonic systems that do not require sophisticated sample engineering.

Interlayer interaction in 2H-MoTe2/hBN heterostructures

Interlayer vibrational modes in 2H-MoTe2/hBN heterostructures were investigated by low-frequency Raman spectroscopy. A series of low-frequency Raman modes are observed for MoTe2 thicknesses of 1–4 layers: the shear modes of MoTe2 persist in the heterostructure with no shift in the frequency, but the breathing modes show dramatic changes in the heterostructures. The number and the frequencies of the breathing modes do not depend on the twist angle between the two materials but strongly vary with the layer thicknesses of both MoTe2 and hBN layers. The breathing modes were observed for both resonant (1.96 eV) and non-resonant (2.41 eV) excitations. The breathing mode frequencies were analyzed by using the linear chain model, and the interfacial force constant between 2 H-MoTe2 and hBN is estimated to be 3.77 × 1019 N m−3.

Enhancement of Room-Temperature Photoluminescence and Valley Polarization of Monolayer and Bilayer WS2 via Chiral Plasmonic Coupling.

Transition-metal dichalcogenides with intrinsic spin-valley degree of freedom have enabled great potentials for valleytronic and optoelectronic applications. However, the degree of valley polarization is usually low under nonresonant excitation at room temperature due to the phonon-assisted intervalley scattering. Here, achiral and chiral Au arrays are designed to enhance the optical response and valley polarization in monolayer and bilayer WS2. A considerable band edge emission with 7 times increment is realized under the resonant coupling with Au dimer-prism arrays. Valley polarization enhancement is quantitatively predicted by the inherent mechanisms from elevated electromagnetic field intensity and radiation efficiency and further realized in polarized photoluminescence. A tunable valley polarization up to 30.0% is achieved in bilayer WS2 under a nonresonant excitation at room temperature. All of these results provide a promising route toward the development of room-temperature valley-dependent optoelectronic devices.

Position-controlled quantum emitters with reproducible emission wavelength in hexagonal boron nitride

Single photon emitters (SPEs) in low-dimensional layered materials have recently gained a large interest owing to the auspicious perspectives of integration and extreme miniaturization offered by this class of materials. However, accurate control of both the spatial location and the emission wavelength of the quantum emitters is essentially lacking to date, thus hindering further technological steps towards scalable quantum photonic devices. Here, we evidence SPEs in high purity synthetic hexagonal boron nitride (hBN) that can be activated by an electron beam at chosen locations. SPE ensembles are generated with a spatial accuracy better than the cubed emission wavelength, thus opening the way to integration in optical microstructures. Stable and bright single photon emission is subsequently observed in the visible range up to room temperature upon non-resonant laser excitation. Moreover, the low-temperature emission wavelength is reproducible, with an ensemble distribution of width 3 meV, a statistical dispersion that is more than one order of magnitude lower than the narrowest wavelength spreads obtained in epitaxial hBN samples. Our findings constitute an essential step towards the realization of top-down integrated devices based on identical quantum emitters in 2D materials.

Resonance-Enhanced Excitation of Interlayer Vibrations in Atomically Thin Black Phosphorus.

The strength of interlayer coupling critically affects the physical properties of 2D materials such as black phosphorus (BP), where the electronic structure depends sensitively on layer thickness. Rigid-layer vibrations reflect directly the interlayer coupling strength in 2D van der Waals solids, but measurement of these characteristic frequencies is made difficult by sample instability and small Raman scattering cross sections in atomically thin elemental crystals. Here, we overcome these challenges in BP by performing resonance-enhanced low-frequency Raman scattering under an argon-protective environment. Interlayer breathing modes for atomically thin BP were previously unobservable under conventional (nonresonant) excitation but became strongly enhanced when the excitation energy matched the sub-band electronic transitions of few-layer BP, down to bilayer thicknesses. The measured out-of-plane interlayer force constant was found to be 10.1 × 1019 N/m3 in BP, which is comparable to graphene. Accurate characterization of the interlayer coupling strength lays the foundation for future exploration of BP twisted structures and heterostructures.

Coherent vibrational dynamics reveals lattice anharmonicity in organic\u2013inorganic halide perovskite nanocrystals

The halide ions of organic-inorganic hybrid perovskites can strongly influence the interaction between the central organic moiety and the inorganic metal halide octahedral units and thus their lattice vibrations. Here, we report the halide-ion-dependent vibrational coherences in formamidinium lead halide (FAPbX3, X = Br, I) perovskite nanocrystals (PNCs) via the combination of femtosecond pump–probe spectroscopy and density functional theory calculations. We find that the FAPbX3 PNCs generate halide-dependent coherent vibronic wave packets upon above-bandgap non-resonant excitation. More importantly, we observe several higher harmonics of the fundamental modes for FAPbI3 PNCs as compared to FAPbBr3 PNCs. This is likely due to the weaker interaction between the central FA moiety and the inorganic cage for FAPbI3 PNCs, and thus the PbI64− unit can vibrate more freely. This weakening reveals the intrinsic anharmonicity in the Pb-I framework, and thus facilitating the energy transfer into overtone and combination bands. These findings not only unveil the superior stability of Br–based PNCs over I–based PNCs but are also important for a better understanding of their electronic and polaronic properties.

Hard X-ray transient grating spectroscopy on bismuth germanate

Optical-domain transient grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique that is used to probe vibrational, magnetic and electronic degrees of freedom in the time domain1. The newly developed coherent X-ray free-electron laser sources allow its extension to the X-ray regime. X-rays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element specificity can address core excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. Here, we demonstrate TG excitation in the hard X-ray range at 7.1 keV. In bismuth germanate (BGO), the non-resonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.

A Versatile DNA Origami-Based Plasmonic Nanoantenna for Label-Free Single-Molecule Surface-Enhanced Raman Spectroscopy.

DNA origami technology allows for the precise nanoscale assembly of chemical entities that give rise to sophisticated functional materials. We have created a versatile DNA origami nanofork antenna (DONA) by assembling Au or Ag nanoparticle dimers with different gap sizes down to 1.17 nm, enabling signal enhancements in surface-enhanced Raman scattering (SERS) of up to 1011. This allows for single-molecule SERS measurements, which can even be performed with larger gap sizes to accommodate differently sized molecules, at various excitation wavelengths. A general scheme is presented to place single analyte molecules into the SERS hot spots using the DNA origami structure exploiting covalent and noncovalent coupling schemes. By using Au and Ag dimers, single-molecule SERS measurements of three dyes and cytochrome c and horseradish peroxidase proteins are demonstrated even under nonresonant excitation conditions, thus providing long photostability during time-series measurement and enabling optical monitoring of single molecules.

Suppression of galloping oscillations by injecting a high-frequency excitation.

Galloping is an aeroelastic instability which incites oscillatory motion of elastic structures when subjected to an incident flow. Because galloping is often detrimental to the integrity of the structure, many research studies have focused on investigating methodologies to suppress these oscillations. These include using passive energy sinks, altering the surface characteristics of the structure, actively changing the shape of the boundary layer through momentum injection and using feedback control algorithms. In this paper, we demonstrate that the critical flow speed at which galloping is activated can be substantially increased by subjecting the galloping structure to a high-frequency non-resonant base excitation. The average effect of the high-frequency excitation is to produce additional linear damping in the slow response which serves to suppress the galloping instability. We study this approach theoretically and demonstrate its effectiveness using experimental tests performed on a galloping cantilevered structure. It is demonstrated that the galloping speed can be tripled in some experimental cases. This article is part of the theme issue 'Vibrational and stochastic resonance in driven nonlinear systems (part 2)'.

Polariton spin jets through optical control

We demonstrate spin polarized jets in extended systems of ballistic exciton-polariton condensates in semiconductor microcavities using optical non-resonant excitation geometries. The structure of the spin jets is determined by the digitally reprogrammable, spatially non-uniform, degree of circular polarization of the excitation laser. The presence of the laser excitation, strong particle interactions, and spin-relaxation leads to a tunable spin-dependent potential landscape for polaritons, with the appearance of intricate polarization patterns due to coherent matter-wave interference. Our work realizes polarization-structured coherent light sources in the absence of gauge fields.

Cavity buildup dispersion spectroscopy

Measurements of ultrahigh-fidelity absorption spectra can help validate quantum theory, engineer ultracold chemistry, and remotely sense atmospheres. Recent achievements in cavity-enhanced spectroscopy using either frequency-based dispersion or time-based absorption approaches have set new records for accuracy with uncertainties at the sub-per-mil level. However, laser scanning or susceptibility to nonlinearities limits their ultimate performance. Here we present cavity buildup dispersion spectroscopy (CBDS), probing the CO molecule as an example, in which the dispersive frequency shift of a cavity resonance is encoded in the cavity’s transient response to a phase-locked non-resonant laser excitation. Beating between optical frequencies during buildup exactly localizes detuning from mode center, and thus enables single-shot dispersion measurements. CBDS can yield an accuracy limited by the chosen frequency standard and measurement duration and is currently 50 times less susceptible to detection nonlinearity compared to intensity-based methods. Moreover, CBDS is significantly faster than previous frequency-based cavity-enhanced methods. The generality of CBDS shows promise for improving fundamental research into a variety of light–matter interactions.

Optimal design of inerter‐based nonpacked particle damper considering particle rolling

AbstractThis paper presents an optimal design method for a nonpacked particle damper (NPPD) based on a simplified mechanical model and corresponding damping mechanism analysis. First, an equivalent inertial single‐particle mechanics model (EISM) and the corresponding equivalent principle were proposed to consider the influence of particle rolling on the vibration reduction. The experimental verification of the EISM under seismic ground motion was subsequently carried out. Based on a reasonable verification of the proposed model, an analytical solution of the EISM single‐degree‐of‐freedom structure system for the symmetric two‐impacts‐per‐cycle motion was obtained. The influence analyses of collision distance on the damping effect and the damping mechanism under resonance and nonresonance harmonic excitation were performed. The theoretical calculation formula for the optimal collision distance for energy consumption was obtained based on the damping mechanism analysis. Finally, numerical simulations under harmonic excitation and seismic ground motion were carried out to verify the rationality and generalization of the proposed optimal collision distance. Accordingly, an optimal design method for the NPPD was proposed. Based on the proposed optimization method, the vibration reduction effect of NPPD under far‐field records, near‐fault pulse‐like records, and near‐fault nonpulse records are discussed. The analysis results show that the vibration reduction effect of the NPPD is affected by the response frequency of the uncontrolled structure. The proposed optimization method can be used as the basis for the optimization of NPPD under earthquakes.

Coherence in single photon emission from droplet epitaxy and Stranski–Krastanov quantum dots in the telecom C-band

The ability of two photons to interfere lies at the heart of many photonic quantum networking concepts and requires that the photons are indistinguishable with sufficient coherence times to resolve the interference signals. However, for solid-state quantum light sources, this can be challenging to achieve as they are in constant interaction with noise sources in their environment. Here, we investigate the noise sources that affect InAs/InP quantum dots emitting in the telecom C-band by comparing their behavior on a wetting layer for Stranski–Krastanov grown quantum dots with a nearly wetting layer-free environment achieved with the droplet epitaxy growth mode. We show that the droplet epitaxy growth mode is beneficial for a quiet environment, leading to 96% of exciton transitions having a coherence time longer than the typical detector resolution of 100 ps, even under non-resonant excitation. We also show that the decay profile indicates the presence of slow dephasing processes, which can be compensated for experimentally. We finally conduct Hong–Ou–Mandel interference measurements between subsequently emitted photons and find a corrected two-photon interference visibility of 98.6 ± 1.6% for droplet-epitaxy grown quantum dots. The understanding of the influence of their surroundings on the quantum optical properties of these emitters is important for their optimization and use in future quantum networking applications.

Решетки населенностей, создаваемые в газе атомов водорода с помощью ультрафиолетовых аттосекундных импульсов

The possibility of population density grating in a gas of hydrogen atoms using a pair ultraviolet (UV) attosecond pulses that do not overlap in the medium is studied. Wherein the central frequency of the pulses can both coincide with the frequency of the resonant transition 1−2 from the main state in the first excited state (the main line of the Lyman series), and be detuned from it. The results of numerical calculations are in agreement with the analytical values ​​obtained on the basis of approximate solution of Schrödinger equation using perturbation theory. It is shown that under resonant excitation the greatest efficiency of the grating is achieved with an increase in the pulse duration. When nonresonant excitation, on the contrary, the system is more efficiently excited by short quasi-unipolar subcycle pulses than bipolar multicycle pulses. The results obtained can be applicable to coherent excitation of a single atom (thin layer) using a pair of UV pulses. The possibility of controlling the modulation depth of the gratings by changing the carrier envelope phase (CEP) of attosecond pulses is shown.

Nonlinear dynamical response of interacting bosons to synthetic electric field

We theoretically study the non-linear response of interacting neutral bosonic gas in a synthetically driven one-dimensional optical lattice. In particular, we examine the bosonic analogue of electronic higher harmonic generation in a strong time-dependent synthetic vector potential manifesting itself as the synthetic electric field. We show that the vector potential can generate reasonably high harmonics in the insulating regime, while the superfluid regime exhibits only a few harmonics. In the insulating regime, the number of harmonics increases with the increase in the strength of the vector potential. This originates primarily due to the field-driven resonant and non-resonant excitations in the neutral Mott state and their recombination with the ground state. If the repulsive interaction between two atoms ($U$) is close to the strength of the gauge potential ($A_0$), the resonant quasiparticle-quasihole pairs on nearest-neighbor sites, namely dipole states are found to a play a dominant role in the generating higher harmonics. However, in the strong-field limit $A_0\gg U$, the nonresonant states where quasiparticle-quasihole pairs are not on nearest-neighbor sites give rise to higher harmonics.

Photon-avalanche-like upconversion in NdAl3(BO3)4 nanoparticles excited at 1064 nm

We report efficient nonresonant ground-state excitation at 1064 nm of trivalent neodymium (Nd3+) ions in stoichiometric neodymium aluminum borate NdAl3(BO3)4 nanoparticles, which are crystalline and, besides the large content of Nd3+ ions, present excellent photoluminescence properties. Upconversion (UC) emission was observed, and the energy pathways were identified starting from multi-phonon assisted ground-state absorption (4I9/2 → 4F3/2) and excited-state absorption (4I11/2 → 4F3/2) with the population of the 4I11/2 level by thermal coupling with the ground state. The excited state 4I11/2 is also populated by relaxations of the Nd3+ ions at upper-lying levels. Cross-relaxation between two Nd3+ ions (4F3/2, 4I9/2) → (4I15/2, 4I15/2) with subsequent phonon emission leads to two ions at the 4I11/2 level, with every iteration triggering a photon-avalanche-like emission, which greatly enhances the efficiency of the UC emissions. Ladder thermal excitation 4F3/2 → (4F5/2, 2H9/2) → (4F7/2, 4S3/2) → 4F9/2 was achieved, and the ground-state relaxation from these levels provided emission at 880 nm, 810 nm, 750 nm, and 690 nm, respectively. Energy transfer UC (Auger) between Nd3+ ions at the 4F3/2 level allowed the population of (2G3/2, 4G7/2) from which relaxations to the 4I9/2, 4I11/2, and 4I13/2 states provided emissions around 536 nm, 600 nm, and 660 nm, respectively. Associated with the nonradiative relaxations, we observed the heating of the nanoparticles (22 °C–240 °C) with subsequent thermal enhancement of the frequency UC emissions due to population redistribution between the coupled energy levels of the Nd3+ ions. The present results have potential applications in super-resolution imaging and nanothermometry.

Spatially confined vector fields at material-induced resonances in near-field-coupled systems.

Local electric fields play the key role in near-field optical examinations and are especially appealing when exploring heterogeneous or even anisotropic nano-systems. Scattering-type near-field optical microscopy (s-SNOM) is the most commonly used method applied to explore and quantify such confined electric fields at the nanometer length scale: while most works so far did focus on analyzing the z-component oriented perpendicular to the sample surface under p-polarized tip/sample illumination only, recent experimental efforts in s-SNOM report that material resonant excitation might equally allow to probe in-plane electric field components. We thus explore this local vector-field behavior for a simple particle-tip/substrate system by comparing our parametric simulations based on finite element modelling at mid-IR wavelengths, to the standard analytical tip-dipole model. Notably, we analyze all the 4 different combinations for resonant and non-resonant tip and/or sample excitation. Besides the 3-dimensional field confinement under the particle tip present for all scenarios, it is particularly the resonant sample excitations that enable extremely strong field enhancements associated with vector fields pointing along all cartesian coordinates, even without breaking the tip/sample symmetry! In fact, in-plane (s-) resonant sample excitation exceeds the commonly-used p-polarized illumination on non-resonant samples by more than 6 orders of magnitude. Moreover, a variety of different spatial field distributions is found both at and within the sample surface, ranging from electric fields that are oriented strictly perpendicular to the sample surface, to fields that spatially rotate into different directions. Our approach shows that accessing the full vector fields in order to quantify all tensorial properties in nanoscale and modern-type materials lies well within the possibilities and scope of today's s-SNOM technique.