Over the past decade, terahertz electromagnetic waves with sub-millimeter wavelength (30 µm to 3 mm) have attracted much attention due to the wide range of applications in medical and industrial fields. Magnetic thin film heterostructures (spintronic emitters) consisting of ferromagnet and nonmagnetic metal layers have recently emerged as broadband THz sources that may have advantages over conventional sources such as photoconductive antennas (PCA) and nonlinear crystals. Here, we demonstrate how to use spintronic emitters patterned into microstructures of different geometries and dimensions to modify the characteristic electromagnetic spectrum of the emitted THz waves. Furthermore, we theoretically explore the possibility of combining emergent spintronic emitters with conventional PCA as hybrid emitters for THz pulse shaping and controlling the handedness of the polarization of THz waves. This new method takes advantage of the broad bandwidth of spintronic emitters and high-intensity THz emission at the low frequency of PCAs. These modelings are confirmed by preliminary experiments. Our results are beneficial to the production of functional THz devices with tunable parameters.
Quasi-2D perovskites have gained significant attention in the field of optics and photonics recently due to their intriguing optical properties. Endowed with optical properties typically found in both 2D and 3D systems, they offer a premier platform for tunable optical devices. Here we studied the prospects of Quasi-2D perovskites for lasing by first delving into excitonic and free carrier ultrafast dynamics, exploring into random lasing from naturally formed cavities in planar films and investigating lasing from structurally-tuned nanowires. Our results give insights on the fundamental radiative processes in these novel materials and build a foundation for future experiments and applications.
Cesium lead bromide nanocrystals, in contrast to most other materials, exhibit near-unity photoluminescence quantum yields (PLQY). When excited below the band gap, they absorb the photons and show anti-Stokes photoluminescence (ASPL), emitting higher energy, band-gap photons. Simultaneous existence of near-unity PLQY and ASPL can be used to optically cool these materials. In this talk, I will report near-unity ASPL efficiencies in CsPbBr3 nanocrystals and attribute it to resonant multiple-phonon absorption by polarons. The theory explains paradoxically large efficiencies for intrinsically disfavored, multiple-phonon-assisted ASPL in nanocrystals.
CsPbBr3 perovskite nanocrystals have been identified as a potential medium to realize condensed phase optical refrigeration. This is due to its near unity emission quantum yields and efficient anti-Stokes photoluminescence (ASPL). Despite much work on CsPbBr3’s optical response, the origin of its efficient ASPL remains unclear. We conduct detailed optical spectroscopy measurements in conjunction with theory to establish mechanistic insights into CsPbBr3’s up-conversion process. Experimental techniques utilized include: temperature-dependent and detuning energy-dependent ASPL measurements, temperature-tunable photothermal heterodyne absorption spectroscopy, and ultrafast transient differential absorption (TDA) spectroscopy.
Band structures engineering of periodic optical structures enables the control of light propagation and localization. Although photons trapped inside 2D lattices can be described within the first Brillouin zone in reciprocal space, the wavevectors of scattered photons outside the lattice are limited by the 3D light cone, which depicts the free-photon dispersion in the surroundings. Because plasmonic nanoparticle lattices show unique dual properties of light trapping and strong scattering, this material platform is promising for investigations of radiative losses. This talk describes how light-cone surface lattice resonance (SLRs) from plasmonic nanoparticle lattices allow the observation of radiated electromagnetic fields. We theoretically predicted the angular distributions of the radiated fields, and experimentally probed the light-cone SLR modes by in-plane lasing emission. These results provide a nanolaser design strategy to achieve tunable lasing colors by lattice rotation.
Dynamic control over the permittivity of materials enables control over the amplitude, phase, and polarization of light. Thus, to realize practical tunable devices, it is important to perform a detailed dynamic characterization of technology-relevant materials with substantially tunable optical properties. In this work, we demonstrate extraordinarily large, unity-order permittivity modulation in zinc oxide through interband pumping. The large permittivity changes actively enable large reflectance modulation in both lithography-free mirrors (70% at 31.6 mJ/cm2 pump) and nanodisk resonators (55% at 7.6 mJ/cm2 pump fluence). The relaxation time for this response is 20 ps. We explore the physical origins of the permittivity modulation and determine the physical limits. The results of this study will advance the realization of ultrafast dynamic optical devices for optical switching, beam-steering, and spectroscopy.
Controlling the permittivity of materials enables control over the amplitude, phase and polarization of light interacting with them. Tailorable and tunable transparent conducting oxides have applications in optical switching, beam steering, imaging, sensing, and spectroscopy.
In this work, we experimentally demonstrate wide tailoring and tuning of the optical properties of oxides to achieve fast switching with large modulation depths. In cadmium oxide, the permittivity and the epsilon-near-zero points can be tailored via yttrium doping to achieve large, ENZ-enhanced mid-IR reflectance modulation. In zinc oxide, the permittivity is tuned by interband pumping, achieving large reflectance modulation in the telecom regime. With aluminum-doped zinc oxide, we demonstrate tailorable Berreman-type absorbers that can achieve ultrafast switching in the telecom frequencies. Our work will pave the way to practical optical switching spanning the telecom to the mid-infrared wavelength regimes.
All-optical switching of metasurfaces enables dynamic control of the amplitude, phase and the polarization of light at picosecond timescales. The large free-carrier induced permittivity changes in transparent conducting oxides enable all-optical switching at femtosecond to picosecond timescales in planar, unpatterned films, without the need for lithography.
In this work, we experimentally demonstrate the wide-tuning of the optical properties of three materials to achieve fast optical switching with large modulation depth. Lithography-free designs such as Fabry-Perot cavities, metal-dielectric mirrors, and Berreman-type metasurfaces are demonstrated to showcase optical switching at powers on the order of 1 mJ/cm2. The switching speeds can vary from 50 ps in cadmium oxide, 20 ps in ZnO to 2 ps in aluminum-doped zinc oxides. Our work will pave the way to practical optical switching spanning the telecom to the mid-infrared wavelength regimes.
We experimentally investigate how the static and dynamic optical properties of cadmium oxide evolve with yttrium doping, for the design of optical and plasmonic devices spanning the near-infrared to the mid-infrared wavelengths. The metallicity is seen to increase and the epsilon-near-zero point blue-shifts with increasing yttrium-concentrations. We demonstrate broadband, optical-pump-induced reflection and transmission modulation ((up to 135% near ENZ), with picosecond response-times controlled by doping-concentration.
In recent years terahertz (THz) technology has been an emerging research field with a broad range of applications. THz radiation falls between the infrared and microwave radiation in the electromagnetic spectrum. Most THz sources to date are not related to the spin degree of freedom; however, recent research efforts in spintronics and ferromagnetism demonstrated that the electron spin offers completely new opportunities for the generation of ultrafast photocurrents. For instance, magnetic heterostructures are very easy to pattern and potentially allow to tailor THz emission characteristics by design. Here, we demonstrate that an ultrafast spin-current pulse driven by a femtosecond laser pulse can create THz transients in microstructured magnetic heterostructures due to the inverse spin Hall effect. We compare the THz electric field and the THz spectrum of a control CoFeB/Pt film with microstructured CoFeB/Pt wires as well as microstructured CoFeB/MgO wires patterned on an extended Pt film. We find that the THz electric field amplitude is proportional to the coverage of the CoFeB/Pt heterostructure on top of the MgO substrate. Furthermore, we analyze the magnetization direction dependence of the THz transients with respect to the easy axis of the ferromagnetic wire. The presented results are the first steps towards shaping and controlling the THz properties by microstructuring of spintronics-based THz emitters.
All-optical modulation of light using metallic nanostructures can potentially enable processing of information with speed in the terahertz range. This is because the optical nonlinearity of metals dictated by the electron-phonon coupling is intrinsically fast. Nobel metals have achieved great success to this end due to their superior plasmonic properties in the visible. However, each type of noble metals only works in a specific wavelength range and therefore broadband spectral response covering the wide visible spectrum can be a challenge. Here we introduce indium-tin-oxide nanorod arrays (ITO-NRAs) which exhibit broadband response covering the visible spectrum. We show that the static spectral response of ITO-NRAs does not depend on the incident polarization and is insensitive to whether the lattice is a square or a rectangle. We further demonstrate that the transmission spectrum can be slightly shifted by changing the sample temperature, as well as adjusting the doping concentration which can be achieved by annealing the sample in oxygen rich environments. When pumped by an optical pulse with photon energy above the bandgap, the transmission can be modified in the entire visible range. These preliminary results show that ITONRAs offer unique opportunities for all-optical modulation in optical frequencies.
Quantum wells (QWs) are thin semiconductor layers than confine electrons and holes in one dimension. They are widely used for optoelectronic devices, particularly semiconductor lasers, but have so far been produced using expensive epitaxial crystal-growth techniques. This has motivated research into the use of colloidal semiconductor nanocrystals, which can be synthesized chemically at low cost, and can be processed in the solution phase. However, initial demonstrations of optical gain from colloidal nanocrystals involved high thresholds.
Recently, colloidal synthesis methods have been developed for the production of thin, atomically flat semiconductor nanocrystals, known as nanoplatelets (NPLs). We investigated relaxation of high-energy carriers in colloidal CdSe NPLs, and found that the relaxation is characteristic of a QW system. Carrier cooling and relaxation on time scales from picoseconds to hundreds of picoseconds are dominated by Auger-type exciton-exciton interactions. The picosecond-scale cooling of hot carriers is much faster than the exciton recombination rate, as required for use of these NPLs as optical gain and lasing materials.
We therefore investigated amplified spontaneous emission using close-packed films of NPLs. We observed thresholds that were more than 4 times lower than the best reported value for colloidal nanocrystals. Moreover, gain in these films is 4 times higher than gain reported for other colloidal nanocrystals, and saturates at pump fluences more than two orders of magnitude above the ASE threshold. We attribute this exceptional performance to large optical cross-sections, relatively slow Auger recombination rates, and narrow ensemble emission linewidths.
Energy-resolving gamma-ray detectors are of particular interest for the detection of illicit radioactive materials at border crossings and other portals because they offer fast, contactless screening that can discriminate between dangerous and benign materials. Among detector classes, scintillators offer an intriguing balance between cost and performance, but current technologies rely on single-crystal materials that are not scalable to portal-relevant detector sizes. Thus, there is a recognized need for novel, processible, high-performance scintillating materials or composites. Composites based on semiconductor nanocrystal quantum dots (QDs) are of interest because of their potentially high gamma-stopping power, high emission quantum yields, and low-cost solution synthesis and processing. Yet the performance of these and other granular nanomaterials has not met expectations. We suggest that this is due to the general lack of insight into the gamma-to-photons transduction process within these inherently more complex materials, which reduces the development and refinement of candidates to simple trial-and-error. Here, we describe the development of ultrafast transient cathodoluminescence as a unique spectroscopic tool for probing the population of excited states formed within a material during scintillation, and thus determining the major sources of energy loss. Our analysis shows that in the case of CdSe/ZnS core/shell QDs, any efficiency loss due to previously blamed factors of low-stopping power and high reabsorptive losses are likely dwarfed by the losses attributable to efficient, non-radiative Auger recombination. We examine how we reached this conclusion, and how this insight defines the characteristics needed in the next generation of scintillating QD composites.
We report a novel type of nanocomposite of conjugated polymer (regio-regular polythiophene) with infrared-sensitive, PbSe quantum dots (QD), which have size-tunable lowest-energy absorption bands between 0.3 and 1 eV. Thin film devices show very good diode characteristics and sizable photovoltaic response with an open circuit voltage, Voc, of ~ 0.3-0.4 V and short circuit current density, Jsc, of ~ 0.2mA/cm2, which is significantly higher than recently reported in PbS QD-based devices. This is the evidence of a quite efficient photoinduced charge transfer between the polymer and QD, with infrared sensitivity. Photocurrent under reverse bias is significantly enhanced to Jph ~ 1 mA/cm2 indicating that the polythiophene/PbSe QD system can be used as effective infrared photodetectors. Detailed spectroscopic studies of photoresponse over a wide spectral range are presented. Quenching of photoluminescence by PbSe QDs has also been studied to gain more understanding of energy and charge transfer in this system.
KEYWORDS: Diffraction gratings, Diffraction, Second-harmonic generation, Near field scanning optical microscopy, Polymer thin films, Thin films, Polarization, Near field optics, Near field, Polymers
Electrical poling induces polar ordering of molecules in a grating that has been holographically inscribed on a thin film of polymer functionalized with azobenzene side chains. Depending on the surface relief amplitude, the resulting χ(2) grating, seen by second harmonic generation (SHG) near-field scanning optical microscopy (NSOM), can have a periodic structure significantly different from the topographical image. The far-field linear and SHG diffraction patterns correlate well with the grating structures. Poling of the thin-film grating, which presumably has photo-driven non-uniform material properties within each period, leads to the more complex structure of the χ(2) grating.
KEYWORDS: Second-harmonic generation, Near field scanning optical microscopy, Near field optics, Imaging spectroscopy, Nonlinear optics, Near field, Harmonic generation, Signal processing, Absorption, Signal detection
Techniques of coherent nonlinear spectroscopy (second harmonic generation and third harmonic generation) are combined with near-field scanning optical microscopy for imaging selected chemical and physical environments in biological matter on a nanoscopic scale. Resonant enhancement of nonlinear signals is utilized as a method of producing chemically selective contrast while the order of the process provides environmental selectivity. Systems studied include natural killer cells and erythrocytes.
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