Recent advances in ultrafast nonlinear optics have caused the terahertz (THz) spectral window (100 GHz-10 THz), lying between the microwave and infrared regions, to gain prominence. This yet-to-be fully explored spectral band is now attracting much attention for its potential in future millimeter and submillimeter wave communications and sensing. Needed for such applications are systems and methods for modulating THz beams.
The present disclosure may be better understood with reference to the following figures. Matching reference numerals designate corresponding parts throughout the figures, which are not necessarily drawn to scale.
As described above, needed are systems and methods for modulating terahertz (THz) beams for the purpose of exploiting the THz spectral window for communications and/or sensing applications. Disclosed herein are examples of such systems and methods. In one embodiment, a system comprises a multiferroic nanoparticle heterostructure through which a THz beam propagates. In some embodiments, the heterostructure comprises a plurality of multiferroic nanoparticles that each includes a ferromagnetic core that is surrounded by a ferroelectric shell. The multiferroic nanoparticles are sandwiched between two thin substrates, such as mica substrates, and the heterostructure is positioned within an external direct current (DC) magnetic field that is either parallel or anti-parallel to the propagation direction of the THz beam. When the magnetic field is antiparallel to the direction of the beam, the amplitude of the beam can be modulated. When the magnetic field is parallel to the direction of the beam, both the amplitude and the phase of the beam can be modulated.
In the following disclosure, various specific embodiments are described. It is to be understood that those embodiments are example implementations of the disclosed inventions and that alternative embodiments are possible, including “hybrid” embodiments that include features of one or more different embodiments. All such embodiments are intended to fall within the scope of this disclosure.
Introduction
In today's world of miniaturization, where nanotechnologies are providing promising solutions for future applications, researchers are now trying to exploit such nanotechnologies in the millimeter and submillimeter wave regimes. In particular, nanostructures are being explored for the generation, detection, and manipulation of THz radiation. Be it nanometer field-effect transistors (FETs), nano-hot electron bolometers, THz modulators based on plasmonic or graphene, THz vacuum nanoelectronics, THz polarizers based on ferrofluids or polymer-embedded magnetic nanoparticles, superparamagnetic-nanoparticle enhanced THz imaging, or wireless nanosensor networks for nanorobots, it is evident that nanostructures are likely to play a significant role in the development of future THz systems for many real-world applications. In the disclosure that follows, a novel approach is described in which strain-mediated magnetoelectric coupling in a multiferroic nanoparticle heterostructure results in dynamically tunable, magnetic field direction-defined, amplitude/phase mode-selective modulation of THz beams.
Magnetoelectric multiferroics are a family of advanced electronic materials that simultaneously possess both magnetism and ferroelectricity. Although studies have been conducted on the realization of multiferroic effects in both bulk and heterostructured materials, few have examined strain-mediated magnetoelectricity at THz frequencies. In fact, previous research on probing magnetoelectric coupling with THz radiation has mostly examined single-phase systems, in which ferromagnetic (FM) and ferroelectric (FE) order parameters coexist (e.g., rare earth manganites, perovskite helimagnets, or other multiferroic oxides). The inventors have studied magneto-elasto-electric (MEE) coupling in engineered multiferroic composite nanoparticles, in which dynamic coupling between the ferromagnetic and ferroelectric order parameters has been realized in a biphasic system.
The multiferroic nanoparticles comprise core-shell nanoparticles that comprise an FM core and an FE shell. One such nanoparticle that was studied is a nanoparticle comprising a cobalt ferrite (CoFe2O4, (CFO)) core and a barium titanate (BaTiO3, (BTO)) shell. As mentioned above, assemblies of these nanostructures are operated under the influence of an external DC magnetic field, which, through magnetostriction in the FM core, induces stress-mediated piezoelectricity in the outer FE shell. When the magnetic field is applied antiparallel to the propagation direction of the traversing beam, amplitude modulation occurs owing to the magnetostrictive effect of the core. When the magnetic field applied along the propagation direction, however, the FM-FE coupling further enables an additional controllable phase modulation. This brings about an opportunity for nanoparticle-enabled dynamic THz wave propagation control by demonstrating a THz amplitude/phase mode-switch in which the mode of modulation can be dynamically switched by simply changing the direction of the applied external DC magnetic field.
Described below is a study in which core-shell nanoparticles and the multiferroic nanoparticle heterostructures were created and used to modulate a THz beam within external DC magnetic fields.
Synthesis and Characterization of CFO-BTO Nanoparticles
A hydrothermal method was employed to synthesize the FM-FE ([1−x] CFO-[x] BTO, where x=40 mol %) core-shell nanoparticles. Commercially available CFO nanoparticles (acquired from Alfa Aesar Inc.) were used for the cores. A polymerized method following the Pechini route of reaction was used to prepare the BTO shells utilizing the commercially available reagents barium carbonate (BaCO3) and titanium tetraisopropoxide (Ti[OCH(CH3)2]4).
The transmission electron microscope (TEM) images of
Terahertz Magneto-Optical Experimental System
An experimental THz time-domain spectroscopy (THz-TDS) system 10, shown in
With further reference to
Referring again to
During the experiments, all THz measurements obtained using the system 10 were acquired in the dark (eliminating ambient light) while ensuring that no stray radiation/laser light reached the nanoparticle heterostructure 26. The both the x and y components of the transmitted THz beam was recorded.
Directional Control of THz Wave Propagation
To realize magnetic field direction-defined THz wave propagation control, the experiments were carried out in four different configurations using an input THz beam polarized along the x direction ({right arrow over (E)}THz) and propagating along the z direction (wave vector k∥Hz). THz temporal profiles Ext and Eyt, were captured after transmission through the sample, with the external static magnetic field 1 T≤±B≤4 T applied parallel (+B) and antiparallel (−B) to z. Measurements were performed for both CFO and CFO-BTO separately to decouple their respective contributions. For each set of THz-TDS measurements, nanoparticles with a layer thickness of approximately 100 μm were assembled between two mica substrates. The reference THz-TDS waveforms were measured with only the two substrates.
As shown in
Similar field-dependent amplitude variations were also observed for the relative y-polarized waveforms, ΔEy(±B)≈(Eyt(±B)−Eyt(B =0)) transmitted through CFO. However, very little field-dependent response was measured for CFO-BTO along this polarization direction.
Magnetostriction and Faraday Rotation Influencing THz Propagation in CFO Nanoparticles
To understand the phenomena observed for CFO-BTO nanoparticles, one must first understand how the transmitted THz radiation is affected by the CFO nanoparticles alone.
Magnetostriction is described by a 4th-rank tensor, xlm=Nlmjk·Hj·Hk, where xlm, Nlmjk, and Hj,k represent the strain, magnetostrictive coefficient, and applied magnetic field tensor components, respectively. Inverse spinel structured (AB2O4) CFO is known to exhibit magnetic anisotropy and possesses a strong magnetostrictive property. The quadratic fitting coefficient Γ can therefore be defined as Γ=yΔd, where y is the absorption coefficient per unit thickness and the relative change of the material thickness Δd is a function of the effective magnetostriction Δdxlm=Nlmjk·Hj·Hk.
Furthermore, a large ΔEy(±B)|CFO signal was also recorded. Although it appears to have a similar dependence on the applied field, the signal's amplitude is five to six times less than that of ΔEx(±B)|CFO (see
The changes in amplitude observed in the THz beam while transmitted through the CFO nanoparticles ΔEx,y(±B)|CFO are thus described as a combined effect of magnetostriction and Faraday rotation. The differences observed in the value of Γ for (+)ve and (−)ve B (as mentioned above) can therefore be explained as a contribution from Faraday rotation, where the magnetization of the CFO nanoparticles induced by the applied magnetic field changes ΔEx(±B)|CFO by rotating the polarization of the incident THz beam {right arrow over (E)}TH
Although, from the magnetization measurements, it appears that B is mostly higher than the saturating field for CFO Hsat|CFO (1.184 T), it should be taken into consideration that the magnetization measurements were performed at room temperature, while the THz measurements were taken at 4 K. The increase in coercive fields observed with decreasing temperature explains why it will still retain its nonlinear behavior even at higher values of the applied field, as corroborated by the hysteretic response exhibited when ΔEy(±B)|CFO and ΔEx(±B)|CFO were plotted together (
Finally, the shifted maxima in the curve of
Magnetostrictive-Magnetoelastoelectric Interactions in FM-FE Nanocomposite System
Having established that the observed THz amplitude modulation in CFO nanoparticles is due to magnetostriction and Faraday rotation, focus is now directed to the magnetoelectric CFO-BTO nanoparticles. The transmission spectra (along with the reference THz signal through air) and the extracted refractive index and absorption coefficient of the nanoparticles are shown in
aijk
Heterostructured multiferroics are typically comprised of both magnetostrictive and piezoelectric phases that can potentially be coupled by an external field. CFO-BTO is structurally compatible, and thus has been used to fabricate the core-shell nanocomposites presented here. Physically, the applied external static magnetic field B produces a variation in the strain components of the magnetostrictive CFO cores due to the field dependent orientation of their magnetic dipoles. This magnetostrictive energy originating from the core is mechanically coupled to the FE BTO shell through their common boundaries. Owing to this coupling, the electric dipoles of the piezoelectric BTO layer subsequently develop a stain-induced change in polarization density ΔP|B≡NqΔd (where N is the number of electric dipoles per unit volume, q is the charge content of each dipole, and Δd is the relative shift in the charge separation invoked by the magnetostriction of the core). Considering a surface s enclosing the incremental volume involved, the normal component of polarization {circumflex over (n)}ΔP|B develops a surface charge density σsb=−{circumflex over (n)}·ΔP|B that satisfies the continuity condition of Gauss' law at the surface of the nanoparticles. A finite element analysis (FEA) simulation corroborated this postulation (
One important and unique functionality originating from the observed MEE coupling of the CFO-BTO nanoparticles is its directional response to the applied DC magnetic field. As can be seen in
On the other hand, for +B, dynamic phase shifts, Δϕ, are observed when the THz beam passes through the CFO-BTO nanoparticles. Its prominence becomes more clear when the relative temporal waveforms for +B and −B are plotted together (
is developed (where ε0 is the free-space permittivity). This {right arrow over (E)}sb therefore induces an additional field-dependent phase delay Δϕ in the transmitted THz beam through an electro-optic effect, which depends on the two vectors involved and the angle between them, θ; i.e., Δϕ{right arrow over (E)}THz, {right arrow over (E)}sb, θ.
If the effect for CFO-BTO along the y-polarization, ΔEy(±B)|CFO-BTO is observed (
As demonstrated in
It is noted that the study was performed at high magnetic fields (up to 4 T) and at cryogenic temperatures (4 K) and therefore the performance might appear to be limited as compared with previous reports on the magnetic manipulation of THz waves performed under low magnetic fields. However, it is emphasized that not only the strain-mediated dynamic coupling between a ferromagnetic and a ferroelectric order parameter has been explored in a biphasic system, but the novelty offered by each of the phases has also been exploited to realize a magnetic-field direction-defined THz amplitude/phase mode-switch using an engineered core-shell nanocomposite system. It is believed this can potentially pave the way for new approaches, facilitating biphasic-nanoparticle enabled novel THz modulator designs.
Conclusions
It was demonstrated that MEE coupling in a biphasic nanocomposite system leads to a dynamically tunable non-contact magnetic field direction-defined amplitude/phase mode-selective modulation of THz waves. The magnetoelasto-electric (MEE) effect explored in the above-described study is a strain-mediated dynamic coupling between the ferromagnetic and ferroelectric order parameters, which is engineered and realized in a multiferroic CoFe2O4—BaTiO3 core-shell nanocomposite system. When the magnetic field is applied antiparallel to the THz wave propagation direction, the magnetostrictive (MS) effect is dominant and an amplitude modulation is achieved owing to the contribution from the CFO core of the nanocomposites. When the magnetic field is applied along the direction of the THz wave propagation, the coupled magnetoelastoelectric (MEE) effect is dominant and an additional controllable phase modulation is achieved owing to the coupled-phenomena between the magnetostriction in the core and piezoelectricity in the shell of the nanocomposites. While the relative change in amplitude continues to increase with magnetic field, attaining a value of 16.5% at 4 T, the relative phase-change starts from a value of 28° at 1 T and gradually decreases with increasing field until the reorientation process concludes at 4 T. Both the observed amplitude and phase modulations are achieved in a layer of assembled biphasic nanocomposites of approximately 100 μm thickness. This novel approach therefore demonstrates the potential of engineered biphasic multiferroic nanocomposites in realizing magnetic field control over THz beam propagation.
This application claims priority to co-pending U.S. Provisional Application Ser. No. 62/658,233, filed Apr. 16, 2018, which is hereby incorporated by reference herein in its entirety.
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4648991 | Fang | Mar 1987 | A |
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20190317378 A1 | Oct 2019 | US |
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62658233 | Apr 2018 | US |