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At least 1,009 records · Page 56

Suppression of Midinfrared Plasma Resonance Due to Quantum Confinement in δ-Doped Silicon

The classical Drude model provides an accurate description of the plasma resonance of three-dimensional materials, but only partially explains two-dimensional systems where quantum mechanical effects dominate such as P:δ layers—atomically thin sheets of phosphorus dopants in silicon that induce electronic properties beyond traditional doping. Previously it was shown that P:δ layers produce a distinct Drude tail feature in ellipsometry measurements. However, the ellipsometric spectra could not be properly fit by modeling the δ layer as a discrete layer of classical Drude metal. In particular, even for large broadening corresponding to extremely short relaxation times, a plasma resonance feature was anticipated but not evident in the experimental data. In this work, we develop a physically accurate description of this system, which reveals a general approach to designing thin films with intentionally suppressed plasma resonances. Our model takes into account the strong charge-density confinement and resulting quantum mechanical description of a P:δ layer. Here, we show that the absence of a plasma resonance feature results from a combination of two factors: (i) the sharply varying charge-density profile due to strong confinement in the direction of growth; and (ii) the effective mass and relaxation time anisotropy due to valley degeneracy. The plasma resonance reappears when the atoms composing the δ layer are allowed to diffuse out from the plane of the layer, destroying its well-confined two-dimensional character that is critical to its distinctive electronic properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Direct Observation of Ultrafast Defect-Bound and Free Exciton Dynamics in Defect-Engineered WS 2 Monolayers

Defects in two-dimensional transition metal dichalcogenides (TMDCs) broadly affect their optical and electronic properties. Directly capturing the ultrafast processes of exciton trapping and defect-bound exciton formation is crucial for understanding and advancing defect-mediated optoelectronics and quantum technologies. However, the weak transient optical absorption of defect-bound excitons has limited their experimental observation to date. Here, we report the direct observation of the ultrafast dynamics of defect-bound excitons in monolayer WS 2 crystals with a high density of monosulfur vacancies (V S ) and W-site defect complexes (S W V S ) resulting from synthesis by alkali metal halide-assisted chemical vapor deposition. The dynamics of excitons bound to these defects, along with their coherent interactions with free excitons, are elucidated using ultrafast optical spectroscopy. Using above band-edge photoexcitation, we find that both free and defect-bound excitons simultaneously form within 300 fs from hot carrier relaxation. The defect-bound excitons exhibit shorter lifetimes than free excitons, leading to a population difference of the corresponding excitonic states and free exciton trapping within a 1–100 ps window. Band-edge photoexcitation of free and defect-bound exciton states reveals ultrafast interconversion within ∼150 fs (comparable to our temporal resolution), indicating possible coherent coupling between these states. We further demonstrate efficient up-conversion of defect-bound excitons to free excitons with photon energies up to ∼300 meV below the free exciton resonance. In conclusion, these findings provide insights into the ultrafast dynamics of defect-bound excitons in TMDCs and their coupling with free excitons, which are relevant to defect-engineered optoelectronic, quantum photonic, and valleytronic applications.

36 MATERIALS SCIENCE↗

Lunar accelerometer network gravitational observatory (LANGO)

With ground-based interferometers detecting hundreds of gravitational-wave (GW) events, GW astronomy has continued to blossom. U.S. and European scientists are developing plans to construct third-generation ground-based interferometers. ESA has proceeded through the mission formulation phase of space-based interferometer in a lower-frequency band, 10 –4 –0.1 Hz. Despite all these exciting developments, there is still a missing frequency band, 0.1–10 Hz. This mid-frequency band is rich with interesting astrophysical events. Coalescence and merger of intermediate-mass black holes (IMBHs) will occur in this frequency band. Coalescing stellar-mass BHs will pass through this frequency band days before they reach the frequency band of LIGO and Virgo. Detection of such signals would enable a mid-frequency detector to issue an advance notice to the high-frequency GW detectors, as well as to optical, x-ray and γ-ray telescopes. We propose Lunar Accelerometer Network Gravitational Observatory (LANGO) to detect GWs in this frequency band. In the first phase (LANGO 1), we propose to deploy four ambient-temperature (250 K) accelerometers in the tetrahedral or in a square configuration on the hemisphere facing the Earth. After successful operation at 250 K, LANGO would be upgraded to a cryogenic (4 K) version with over two orders of magnitude increased sensitivity (LANGO 2), with coherent rejection of seismic noise implemented. LANGO is a full-tensor detector, capable of determining the source direction and wave polarization. Each test mass (TM) is suspended as a pendulum with resonance frequency ∼ 0.01 Hz, thus is only weakly coupled to the lunar surface horizontally. LANGO is designed to detect the relative motion of globally separated, nearly free, TMs by using the Moon as a large quiet platform. LANGO 1 and 2 accelerometers aim at sensitivities ⩽ 10 –11 m s –2 Hz –1/2 and ⩽ 10 –13 m s –2 Hz –1/2 in the horizontal axes over the frequency band of 1 mHz–10 Hz, which yield GW sensitivities 1.1 x 10 -21 Hz -1/2 and 3.8 x 10 -24 Hz -1/2 at 1 Hz, respectively. The LANGO accelerometers will be 10 3 –10 5 times more sensitive than Apollo seismometers. With such sensitivity, LANGO will also make great contribution to the advancement of lunar geophysics.

79 ASTRONOMY AND ASTROPHYSICS↗

Electron shelving of a superconducting artificial atom

Interfacing long-lived qubits with propagating photons is a fundamental challenge in quantum technology. Cavity and circuit quantum electrodynamics (cQED) architectures rely on an off-resonant cavity, which blocks the qubit emission and enables a quantum non-demolition (QND) dispersive readout. However, no such buffer mode is necessary for controlling a large class of three-level systems that combine a metastable qubit transition with a bright cycling transition, using the electron shelving effect. Here we demonstrate shelving of a circuit atom, fluxonium, placed inside a microwave waveguide. With no cavity modes in the setup, the qubit coherence time exceeds 50 μs, and the cycling transition’s radiative lifetime is under 100 ns. By detecting a homodyne fluorescence signal from the cycling transition, we implement a QND readout of the qubit and account for readout errors using a minimal optical pumping model. Our result establishes a resource-efficient (cavityless) alternative to cQED for controlling superconducting qubits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Design and fabrication of robust hybrid photonic crystal cavities

Abstract Heterogeneously integrated hybrid photonic crystal cavities enable strong light–matter interactions with solid state, optically addressable quantum memories. A key challenge to realizing high quality factor ( Q ) hybrid photonic crystals is the reduced index contrast on the substrate compared to suspended devices in air. This challenge is particularly acute for color centers in diamond because of diamond’s high refractive index, which leads to increased scattering loss into the substrate. Here, we develop a design methodology for hybrid photonic crystals utilizing a detailed understanding of substrate-mediated loss, which incorporates sensitivity to fabrication errors as a critical parameter. Using this methodology, we design robust, high-Q, GaAs-on-diamond photonic crystal cavities, and by optimizing our fabrication procedure, we experimentally realize cavities with Q approaching 30,000 at a resonance wavelength of 955 nm.

Abulnaga, Alex↗

Tailoring coherent charge transport in graphene by deterministic defect generation

Harnessing the wave-nature of charge carriers in solid state devices, electron optics investigates and exploits coherent phenomena, in analogy with optics and photonics. Typically, this requires complex electronic devices leveraging macroscopically coherent charge transport in two-dimensional electron gases and superconductors. Here, collective coherent effects are induced in a simple counterintuitive architecture by defect engineering. Deterministically introduced lattice defects in graphene enable the phase coherent charge transport by playing the role of potential barriers, instead of scattering centres as conventionally considered. Thus, graphene preserves its quasi-ballistic quantum transport and can support phase-matched charge carrier waves. Based on this approach, multiple electronic Fabry-Pèrot cavities are formed by creating periodically alternating defective and pristine nano-stripes through low energy electron-beam irradiation. Indeed, defective stripes behave as partially reflecting mirrors and resonantly confine the charge carrier waves within the pristine areas, giving rise to Fabry-Pèrot resonant modes. These modes experimentally manifest as sheet resistance oscillations, as also confirmed by Landauer-Büttiker simulations. Moreover, these coherent phenomena survive up to 30 K for both polarities of charge carriers, contrarily to traditional monopolar electrostatically created Fabry-Pèrot interferometers. Our study positions defective graphene as an innovative platform for coherent electronic devices, with potential applications in nano and quantum technologies.

Melchioni, Nicola↗

Benzenesulfonamide Derivatives as Complexants and Extractants for Addressing the Mercury Problem at the Savannah River Site

Mercury (Hg) is a major global pollutant arising from both natural and anthropogenic sources. Its widespread use in medicinal and industrial applications makes it a common chemical exposure and environmental pollutant. It can exist in several forms which include: Metallic mercury (Hg{sup 0}), mercurous (Hg{sub 2}{sup 2+}), mercuric salts (Hg{sup 2+}), and organic mercury (e.g. CH{sub 3}Hg{sup +}), with the latter being the most toxic of all the species. Due to mercury's high toxicity, new approaches towards its detection has received significant attention in the scientific community. Mercury exposure at the Savannah River Site (SRS) has been a recent concern especially with increasing amounts of organic mercury in the saltstone. It originates mainly from its use as an acidic dissolution catalyst of aluminum cladding from target fuels within the uranium and plutonium processing operations [1]. It is present to an amount of about 60 metric tons in the high-level waste (HLW) tanks. Organic Mercury species have been found in low activity waste (LAW) at the site that eventually ends up in the saltstone. Therefore, there is a need for: i) Converting organic mercury to other less toxic forms and ii) Complexation and removal of Hg prior of disposal of LAW in saltstone. Various methods have been developed for selective sensing of mercury in the presence of other toxic metals. These methods include using ligands that can form organo-soluble metal complexes with different optical and spectroscopic properties that can be used for toxic metal sensing. In 2005, our group pioneered an ion-exchange extraction method, in which o-phenylenediamine-derived disulfonamides were used to complex and selectively extract and sense Pb{sup 2+} from aqueous solutions into an organic phase [2,3]. Herein, a disulfonamide and a bis-dansylamide have been shown to extract, complex and sense Hg(II). Ligand 1: The crystal structure of the disulfonamide-Hg complex confirms the complexation of Hg(II) with the ligand. Complexation was corroborated by the {sup 1}H-NMR spectra obtained after contacting solutions of various concentrations of Hg{sup 2+} with 2 mM ligand in chloroform. Distinct resonances are observed at Hg/L ratio of 0.5 that are also observed for the isolated 1:2 complex. In the presence of excess mercury, new resonances, as well as the movement of Et{sub 3}N resonances indicate the formation of a different Hg-sulfonamide-triethylamine complex, presumably having 1:1 Hg:L stoichiometry. The electronic spectra of aqueous phases after extraction show that there was no free ligand absorption at 0.5 eq of Hg, indicating a complete complexation. Complexation was also confirmed by the UV-visible titrations with Hg{sup 2+} at constant ligand concentration. pH-dependent extraction carried out shows that extraction of Hg(II) by ligand 1 was over 90% for most alkaline pHs. Ligand 2: The crystal structure of the Ligand 2 complex formed with Hg(OAc){sub 2} shows a remarkable coordination pattern with 4:2 metal:ligand stoichiometry. The fluorescent bis-dansyl disulfonamide derivative was found to complex and sense HgCl{sub 2} and Hg(OAc){sub 2} by demonstrating fluorescence quenching upon Hg(II) addition in comparison with other metals (Zn(II), Cd(II), Pb(II)). No were observed for Cu(II), Ag(I) and Co(II). We have shown the complexation of Hg(II) by a disulfonamide and a bis-dansyl disulfonamide ligand using several spectroscopic methods. Ligand 1 was able to extract mercury into chloroform and form a complex in the presence of excess mercury by synergistic complexation with triethylamine acting as a co-ligand. X-ray and NMR both confirm a 1:2 HgL{sub 2} stoichiometry. Ligand 2 can be used for sensing of Hg(II) as fluorescence quenching was observed after addition of Hg(II)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Prolonging All-Optical Molecular Electron Spin Coherence in the Tissue Transparency Window

Coherent electron spin states within paramagnetic molecules hold significant potential for microscopic quantum sensing. However, all-optical coherence measurements amenable to high spatial and temporal resolution under ambient conditions remain a significant challenge. Here we conduct room-temperature, picosecond time-resolved Faraday ellipticity/rotation (TRFE/R) measurements of the electron spin decoherence time T 2 * in [IrBr 6 ] 2- . Decoherence is strongly sensitive to solution phase viscosity, pointing to molecular tumbling as an important decoherence mechanism. Accordingly, immobilization of [IrBr 6 ] 2- molecules in thin polymer films results in an order-of-magnitude increase in coherence lifetime and significantly greater magnetic field sensitivity. Here, by tuning energies of ligand-to-metal charge transfer (LMCT) states, TRFE/R enables spin initialization and readout in the tissue transparency window, paving the way toward all-optical, ultrafast molecular electron spin coherence imaging in biological systems.

Electron paramagnetic resonance spectroscopy↗

Strong NIR II Chiroptical Response and Magnetic Anisotropy via Modular Installation of Chiral Capping Ligands on a Light-Emitting Diradicaloid Scaffold

Low-energy molecular lumiphores have seen increased interest due to potential imaging and communications applications. Specifically, molecules that emit in the near-infrared (NIR, 700–1700 nm) or telecom (∼1260–1625 nm) regions, where attenuation is minimized in biological tissue and optical fibers, respectively, can drastically improve image resolution and depth penetration; however, bright low-energy emission is rare due to exponentially decreasing quantum yields in this region. Chiral molecules exhibiting strong NIR or telecom absorption/emission would be of particular interest due to advanced security and spintronics applications, but these compounds remain scarce and are currently restricted to lanthanide or nanoparticle-based systems. Here, we report the synthesis of a chiral organic-based NIR emitter, enabled by simple peripheral installation of chiral capping ligands. These ligands twist the achiral NIR-emissive core, breaking inversion symmetry. Furthermore, this twisting enables strong chiroptical responses observed via static and transient circular dichroism and increased magnetic anisotropy through electron paramagnetic resonance (EPR) measurements, establishing this strategy as a promising method for the development of new chiral emitters and sensors.

Electron paramagnetic resonance spectroscopy↗

Plasmon-Mediated Intramolecular Methyl Migration with Nanoscale Spatial Control

Plasmonic materials interact strongly with light to focus and enhance electromagnetic radiation down to nanoscale volumes. Due to this localized confinement, materials that support localized surface plasmon resonances are capable of driving energetically unfavorable chemical reactions. In certain cases, the plasmonic nanostructures are able to preferentially catalyze the formation of specific photoproducts, which offers an opportunity for the development of solar-driven chemical synthesis. Here, using plasmonic environments, we report inducing an intramolecular methyl migration reaction, forming 4-methylpyridine from N-methylpyridinium. Using both experimental and computational methods, we were able to confirm the identity of the N-methylpyridinium by making spectral comparisons against possible photoproducts. This reaction involves breaking a C–N bond and forming a new C–C bond, highlighting the ability of plasmonic materials to drive complex and selective reactions. Additionally, we observe that the product yield depends strongly on optical illumination conditions. This is likely due to steric hindrance in specific regions on the nanostructured plasmonic substrate, providing an optical handle for driving plasmonic catalysis with spatial specificity. Furthermore, this work adds yet another class of reactions accessible by surface plasmon excitation to the ever-growing library of plasmon-mediated chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Integrated photonic molecule Brillouin laser with a high-power sub-100-mHz fundamental linewidth

Photonic integrated lasers with an ultra-low fundamental linewidth and a high output power are important for precision atomic and quantum applications, high-capacity communications, and fiber sensing, yet wafer-scale solutions have remained elusive. Here we report an integrated stimulated Brillouin laser (SBL), based on a photonic molecule coupled resonator design, that achieves a sub-100-mHz fundamental linewidth with greater than 10-mW output power in the C band, fabricated on a 200-mm silicon nitride (Si 3 N 4 ) CMOS-foundry compatible wafer-scale platform. The photonic molecule design is used to suppress the second-order Stokes (S2) emission, allowing the primary lasing mode to increase with the pump power without phase noise feedback from higher Stokes orders. The nested waveguide resonators have a 184 million intrinsic and 92 million loaded Q, over an order of magnitude improvement over prior photonic molecules, enabling precision resonance splitting of 198 MHz at the S2 frequency. We demonstrate S2-suppressed single-mode SBL with a minimum fundamental linewidth of 71±18 mHz, corresponding to a 23±6-mHz 2 /Hz white-frequency-noise floor, over an order of magnitude lower than prior integrated SBLs, with an ∼11-mW output power and 2.3-mW threshold power. The frequency noise reaches the resonator-intrinsic thermo-refractive noise from 2-kHz to 1-MHz offset. The laser phase noise reaches −155 dBc/Hz at 10-MHz offset. The performance of this chip-scale SBL shows promise not only to improve the reliability and reduce size and cost but also to enable new precision experiments that require the high-speed manipulation, control, and interrogation of atoms and qubits. Realization in the silicon nitride ultra-low loss platform is adaptable to a wide range of wavelengths from the visible to infrared and enables integration with other components for systems-on-chip solutions for a wide range of precision scientific and engineering applications including quantum sensing, gravitometers, atom interferometers, precision metrology, optical atomic clocks, and ultra-low noise microwave generation.

Liu, Kaikai (ORCID:0000000213609646)↗

Precision Loading and Delivery of Molecular Cargo by Size-Controlled Coacervation of Gold Nanoparticles Functionalized with Elastin-like Peptides

Thermoresponsive elastin-like peptides (ELPs) have been extensively investigated in biotechnology and medicine, but little attention has been paid to the process by which coacervation causes ELP-decorated particles to aggregate. Here, using gold nanoparticles (AuNPs) functionalized with a cysteine-terminated 96-repeat of the VPGVG sequence (V96-Cys), we show that the size of the clusters that reversibly form above the ELP transition temperature can be finely controlled in the 250 to 930 nm range by specifying the concentration of free V96-Cys in solution and using AuNPs of different sizes. We further find that the localized surface plasmon resonance peak of the embedded AuNPs progressively red-shifts with cluster size, likely due to an increase in particle–particle contacts. We exploit this fine control over size to homogeneously load precise amounts of the dye Nile Red and the antibiotic Tetracycline into clusters of different hydrodynamic diameters and deliver cargos near-quantitatively by deconstructing the aggregates below the ELP transition temperature. Beyond establishing a key role for free ELPs in the agglomeration of ELP-functionalized particles, our results provide a path for the thermally controlled delivery of precise quantities of molecular cargo. This capability might prove useful in combination photothermal therapies and theranostic applications, and to trigger spatially and temporally uniform responses from biological, electronic, or optical systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrical control of coherent spin rotation of a single-spin qubit

Nitrogen vacancy (NV) centers, optically active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. One of the critical challenges to develop NV-based quantum operation platforms results from the difficulty in locally addressing the quantum spin states of individual NV spins in a scalable, energy-efficient manner. Here, we report electrical control of the coherent spin rotation rate of a single-spin qubit in NV-magnet based hybrid quantum systems. By utilizing electrically generated spin currents, we are able to achieve efficient tuning of magnetic damping and the amplitude of the dipole fields generated by a micrometer-sized resonant magnet, enabling electrical control of the Rabi oscillation frequency of NV spins. Our results highlight the potential of NV centers in designing functional hybrid solid-state systems for next-generation quantum-information technologies. The demonstrated coupling between the NV centers and the propagating spin waves harbored by a magnetic insulator further points to the possibility to establish macroscale entanglement between distant spin qubits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Multipolariton control in attosecond transient absorption of autoionizing states

Tunable attosecond transient absorption spectroscopy is an ideal tool for studying and manipulating autoionization dynamics in the continuum. We investigate near-resonant two-photon couplings between the bright 3s –1 4p and dark 3s –1 4f autoionizing states of argon that lead to Autler-Townes-like interactions, forming entangled light-matter states or polaritons. We observe that one-photon couplings with intermediate dark states play an important role in this interaction, leading to the formation of multiple polaritonic branches whose energies exhibit avoided crossings as a function of the dressing-laser frequency. Our experimental measurements and theoretical essential-state simulations show good agreement and reveal how the delay, frequency, and intensity of the dressing pulse govern the properties of autoionizing polariton multiplets. Furthermore, these results demonstrate new pathways for quantum control of autoionizing states with optical fields.

74 ATOMIC AND MOLECULAR PHYSICS↗

Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy

We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ~100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. Finally, we suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.

47 OTHER INSTRUMENTATION↗

Exploring the impact of vibrational cavity coupling strength on ultrafast CN + c -C 6 H 12 reaction dynamics

Abstract Molecular polaritons, hybrid light-matter states resulting from strong cavity coupling of optical transitions, may provide a new route to guide chemical reactions. However, demonstrations of cavity-modified reactivity in clean benchmark systems are still needed to clarify the mechanisms and scope of polariton chemistry. Here, we use transient absorption to observe the ultrafast dynamics of CN radicals interacting with a cyclohexane ( c -C 6 H 12 ) and chloroform (CHCl 3 ) solvent mixture under vibrational strong coupling of a C–H stretching mode of c- C 6 H 12 . By modulating the c -C 6 H 12 :CHCl 3 ratio, we explore how solvent complexation and hydrogen (H)-abstraction processes proceed under collective cavity coupling strengths ranging from 55 to 85 cm −1 . Reaction rates remain unchanged for all extracavity, on-resonance, and off-resonance cavity coupling conditions, regardless of coupling strength. These results suggest that insufficient vibrational cavity coupling strength may not be the determining factor for the negligible cavity effects observed previously in H-abstraction reactions of CN with CHCl 3 .

Chen, Liying↗

Origin of high optical contrast in zinc-zinc oxide electrodeposits for dynamic windows

The control of solar light and heat emission through windows is an important strategy for increasing the energy efficiency of buildings. Reversible Zn electrodeposition has recently emerged as a promising method for constructing electronically tintable robust dynamic windows. In Zn electrodeposits formed from dimethyl sulfoxide (DMSO) electrolytes during device tinting, we observe extraordinary absorption that is in excess of what is predicted by the Beer-Lambert law for a uniform Zn thin film. Here, the charge required to electroplate these films is abnormally low, significantly less than previously reported dynamic windows based on reversible metal electrodeposition, which facilitates the construction of large-area devices that switch uniformly. Finite-difference time-domain (FDTD) simulations are used to investigate the origin of this enhanced absorption, which arises from plasmonic effects among the Zn nanoparticles and ZnO dendrites in the film. The dielectric ZnO dendrites promote absorption via slit-like Zn-dielectric-Zn structures that from hybrid surface plasmon resonance at metal walls. Through these investigations, we provide design principles to construct low-charge and high-contrast metal and metal oxide-based dynamic windows.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Making and breaking terahertz waves with fluid plasmas

Vigorous research efforts during the past several decades have successfully closed the “terahertz gap” between microwaves and infrared light, offering new and increasingly efficient ways to produce, detect, and manipulate radiation fields in the terahertz (THz) frequency range. In our laboratory, THz time-domain spectroscopy (THz-TDS) and optical-pump THz-probe (OPTP) experiments have been routinely utilized as ultrafast spectroscopy tools to investigate a variety of emerging quantum materials and metamaterials. The ultrafast THz pulses are produced by femtosecond laser excitation of photoconductive antennas, semiconductor surfaces (InAs), and nonlinear crystals (ZnTe, GaSe, and LiNbO 3 ). Photoconductive antennas and nonlinear crystals also allow for the coherent detection of these pulses in the time domain, with amplitude and phase spectra obtained in the frequency domain via fast Fourier transform. Although such solid-state schemes are highly desirable in many aspects and thus also commonly utilized in many research laboratories and industrial applications, they typically suffer from limited bandwidths due to the absorption and frequency dispersion induced primarily by phonon resonances, limiting THz applications such as spectroscopy of emerging materials, imaging and detection, and biomedical characterization.

77 NANOSCIENCE AND NANOTECHNOLOGY↗