Degrees Of Tunability Research Articles

Effect of molecular concentration on excitonic nanostructure based refractive index sensing and near-field enhanced spectroscopy

Organic thin film based excitonic nanostructures are of great interest in modern resonant nanophotonics as a promising alternative for plasmonic systems. Such nanostructures sustain propagating and localized surface exciton modes that can be exploited in refractive index sensing and near-field enhanced spectroscopy. To realize these surface excitonic modes and to enhance their optical performance, the concentration of the excitonic molecules present in the organic thin film has to be quite high so that a large oscillator strength can be achieved. Unfortunately, this often results in a broadening of the material response, which might prevent achieving the very goal. Therefore, systematic and in-depth studies are needed on the molecular concentration dependence of the surface excitonic modes to acquire optimal performance from them. Here, we study the effect of molecular concentration in terms of oscillator strength and Lorentzian broadening on various surface excitonic modes when employed in sensing and spectroscopy. The optical performance of the modes is evaluated in terms of sensing, like sensitivity and figure of merit, as well as near-field enhancement, like enhancement factor and field confinement. Our numerical investigation reveals that, in general, an increase in oscillator strength enhances the performance of the surface excitonic modes while a broadening degrades that as a counteracting effect. Most of all, this demonstrates that the optical performance of an excitonic system is tunable via molecular concentration unlike the plasmonic systems. Moreover, different surface excitonic modes show different degrees of tunability and equivalency in performance when compared to plasmons in metals (silver and gold). Our findings provide crucial information for developing and optimizing novel excitonic nanodevices for contemporary organic nanophotonics.

Electrical control of hybrid exciton transport in a van der Waals heterostructure

Interactions between out-of-plane dipoles in bosonic gases enable the long-range propagation of excitons. The lack of direct control over collective dipolar properties has so far limited the degrees of tunability and the microscopic understanding of exciton transport. In this work we modulate the layer hybridization and interplay between many-body interactions of excitons in a van der Waals heterostructure with an applied vertical electric field. By performing spatiotemporally resolved measurements supported by microscopic theory, we uncover the dipole-dependent properties and transport of excitons with different degrees of hybridization. Moreover, we find constant emission quantum yields of the transporting species as a function of excitation power with radiative decay mechanisms dominating over nonradiative ones, a fundamental requirement for efficient excitonic devices. Our findings provide a complete picture of the many-body effects in the transport of dilute exciton gases, and have crucial implications for studying emerging states of matter such as Bose–Einstein condensation and optoelectronic applications based on exciton propagation.

Negative Reflection and Negative Refraction in Biaxial van der Waals Materials

Negative reflection and negative refraction are exotic phenomena that can be achieved by platforms such as double-negative metamaterial, hyperbolic metamaterial, and phase-discontinuity metasurface. Recently, natural biaxial van der Waals (vdW) materials, which support extremely anisotropic, low-loss, and highly confined polaritons from infrared to visible regime, are emerging as promising candidates for planar reflective and refractive optics. Here, we introduce three degrees of freedom, namely interface, crystal direction, and electric tunability, to manipulate the reflection and refraction of the polaritons. With broken in-plane symmetry contributed by the interface and crystal direction, distinguished reflection, and refraction such as negative and backward reflection, positive and negative refraction could exist simultaneously and exhibit high tunability. The numerical simulations show good consistency with the theoretical analysis. Our findings provide a robust recipe for the realization of negative reflection and refraction in biaxial vdW materials, paving the way for the polaritonics and on-chip integrated circuits.

Temperature-induced phase transitions in the correlated quantum Hall state of bilayer graphene

The quantum Hall system can be used to study many-body physics owing to its multiple internal electronic degrees of freedom and tunability. While quantum phase transitions have been studied intensively, research on the temperature-induced phase transitions of this system is limited. We measured the pure bulk conductivity of a quantum Hall antiferromagnetic state in bilayer graphene over a wide range of temperatures and revealed the two-step phase transition associated with the breaking of the long-range order and short-range antiferromagnetic order. Our findings are fundamental to understanding electron correlation in quantum Hall systems.

In-plane directionality control of strongly localized resonant modes of light in disordered arrays of dielectric scatterers.

In this work we propose and analyze techniques of in-plane directionality control of strongly localized resonant modes of light in random arrays of dielectric scatterers. Based on reported diameters and areal densities of epitaxially grown self-organized nanowires, two-dimensional (2D) arrays of dielectric scatterers have been analyzed where randomness is gradually increased along a preferred direction of directionality enhancement. In view of the multiple-scattering mediated wave dynamics and directionality enhancement of light in such arrays, a more conveniently realizable, practical structure is proposed where a 2D periodic array is juxtaposed with a uniform, random scattering medium. Far- and near-field emission characteristics of such arrays show that in spite of the utter lack of periodicity in the disordered regime of the structure, directionality of the high-Q resonant modes is modified such that on average more than 70% of the output power is emitted along the pre-defined direction of preference. Such directionality enhancement and strong localization are nonexistent when the 2D periodic array is replaced with a one-dimensional Bragg reflector, thereby confirming the governing role of in-plane multiple scattering in the process. The techniques presented herein offer novel means of realizing not only directionality tunable edge-emitting random lasers but also numerous other disordered media based photonic structures and systems with higher degrees of control and tunability.

Evolving Devil's Staircase Magnetization from Tunable Charge Density Waves in Nonsymmorphic Dirac Semimetals.

While several magnetic topological semimetals have been discovered in recent years, their band structures are far from ideal, often obscured by trivial bands at the Fermi energy. Square-net materials with clean, linearly dispersing bands show potential to circumvent this issue. CeSbTe, a square-net material, features multiple magnetic-field-controllable topological phases. Here, it is shown that in this material, even higher degrees of tunability can be achieved by changing the electron count at the square-net motif. Increased electron filling results in structural distortion and formation of charge density waves (CDWs). The modulation wave-vector evolves continuously leading to a region of multiple discrete CDWs and a corresponding complex "Devil's staircase" magnetic ground state. A series of fractionally quantized magnetization plateaus is observed, which implies direct coupling between CDW and a collective spin-excitation. It is further shown that the CDW creates a robust idealized nonsymmorphic Dirac semimetal, thus providing access to topological systems with richmagnetism.

Thermal tuning of band gap properties in planar stretch-dominated lattices with tailorable coefficient of thermal expansion

The development of the current technology has increased the requirement for the versatility of acoustic metamaterials. In this study, the band gap (BG) tuning of the stretch-dominated thermal expansion lattice metamaterials with different configurations composed of triangular units is studied using the finite element method, and a design method for metamaterials tuned by external temperature changes in multiple frequency ranges is proposed. The results indicate that the stretch-dominated thermal expansion material can maintain the original customized thermal expansion performance while possessing the characteristics of the BG in addition to realizing different degrees of BG tunability when the temperature changes. The results provide a theoretical basis for attaining the thermal expansion/tunable BG dual-objectives design. The objective is to achieve the dual goals of tailorable coefficient of thermal expansion and tunable BG design through reasonable material selection and shape optimization.

Influence of Intrinsic Thermal Stability on Switching Rate and Tunability of Dual-Biased Magnetic Tunnel Junctions for Probabilistic Bits

Recently, magnetic tunnel junctions (MTJs) with superparamagnetic free layers (sMTJs) have been proposed as key components in probabilistic bits (p-bits). However, the average fluctuation rates of sMTJs are very sensitive to slight variations in the device dimensions, which creates a major obstacle to their realization in large-scale networks. One possible solution is to implement dual-biasing on p-bits to offset the effects of variations through onboard corrections. In our previous work, we demonstrated that dual-biasing has the unique capability of separate control over the high- and low-state dwell times, which adds an extra degree of tunability in the signals generated. However, these studies investigated dual-biasing on thermally stable MTJs; therefore, the maximum switching rates were lower than the gigahertz rates desired for sMTJ-based p-bit circuits. While dual-biasing on sMTJs rather than thermally stable MTJs would improve the switching rates, some of the flexibility and robustness of dual-biasing may be sacrificed due to the sensitivity of sMTJs. In this letter, we applied the dual-biasing method on 10 MTJs with varying thermal stability factors to test if sMTJs can achieve the same degree of separation between high- and low-state dwell-time tunability as thermally stable MTJs. Our results show that two degrees of tunability was achieved on all MTJs tested, thus demonstrating that dual-biased p-bits can achieve switching rates equal to or greater than single-biased sMTJs.

Unraveling interactions of resonances for tunable low frequency bandgap in multiphase metamaterials under applied deformation

Metamaterial with various degrees of bandgap tunability is an emerging area in manipulating elastic wave transmission characteristics for next generation phononic devices. Although several attempts are made employing multi-fields such as magnetic, electric and thermal etc., mechanical deformation based tunable bandgap is a major interest. However, achieving tunability in terms of broadening or terminating the bandgap in locally resonant acoustic metamaterial (LRAM) remains as challenging tasks. In this work, we propose LRAM by integrating a two-dimensionally periodically arranged square unit cells consisting of soft coated hard inclusion embedded in a polymer scaffold. We develop computational framework to simulate the low frequency bandgap of unit cell under external deformation. At first quasi-static analysis of unit cell has been performed to find static displacement field under prescribed deformation. Further, utilizing Bloch-Floquet wave analysis for the periodic unit cell and finite element based numerical scheme, an eigenvalue problem is formulated to predict dispersion response within irreducible Brillouin zone (IBZ). Analyzing the symmetry group of the unit cell under deformed state for a series of loading, we extract the bandgap responses. Moreover, we illustrate tunable bandgap at low frequency regimes for different inclusion shapes and sizes. To correlate extension and suppression of bandgap under the applied deformation, evolution of local resonances are described with vibration mode shapes.

Light-Driven Halide Exchange Facilitates Complete Crystal Transformation in Nanostructured Perovskites.

Colloidal perovskite nanocrystals (NCs) have shown promise in visible and near-infrared light emission compared with conventional quantum dots because of their sharp and highly efficient emission. Light-driven halide exchange offers high degrees of tunability of perovskite NC composition and photoluminescence properties. A remaining challenge is the incomplete change between bromide and chloride due to the presence of radical quenchers. Herein, an optimized in situ halide exchange method of perovskite NCs is reported. Chloroform is used as the solvent and the precursor to effectively generate halide radicals and ions under ultraviolet light irradiation in an inert atmosphere. This strategy achieves complete crystal transformation in colloidal perovskite NCs such as CsPbBr3-to-CsPbCl3 and Cs4PbBr6-to-CsPbCl3. The exchange reaction rate can be further tuned by the presence of B-site dopants such as Zn2+ and Ce3+. The dopant cations are partially remained in the exchanged perovskite NCs, indicating the predominance of thermodynamic control in the crystal transformation.

Independent Control of Antiparallel- and Parallel-State Thermal Stability Factors in Magnetic Tunnel Junctions for Telegraphic Signals With Two Degrees of Tunability

Magnetic tunnel junctions (MTJs) with low thermal stability at room temperature have been proposed as read units in beyond CMOS computing architectures including stochastic computing unit and probabilistic-bit (p-bit). Networks of multiple interconnected MTJs may face challenges due to potential device-to-device variations in thermal stability from design targets. Recently, we generated tunable telegraphic signals using a thermally stable MTJ through proper control over an external bias field and a dc voltage bias, where we showed that the average dwell times in the antiparallel (AP) and parallel states could be tuned separately. The implication for this method for p-bit designs is that it allows for p-bits to be compatible with the state-of-the-art magnetoresistive random-access memory (MRAM) technology and introduces a second degree of tunability to the input–output characteristics of the device. In this article, we expand on this method in two important ways. First, we demonstrate the applicability of our method to p-bit designs by modeling the transfer function using the existing p-bit models. Our results indicate that the transfer function can be adjusted with slight modifications to the bias field, which allows for the possibility of p-bit circuits capable of on-chip corrections against device-to-device variations in their thermal stabilities. Second, we identify the physical mechanisms that allow for two degrees of tunability in the output signal, which is explained through the Neel–Brown model. This article provides both applicability and predictability to the dual-biasing method.

Thermal conductivity of biomimetic leaf composite

The venous morphology of a typical plant leaf affects its mechanical and thermal properties. Such a material could be considered as a fiber reinforced composite structure where the veins and the rest of the leaf are considered as two materials having highly contrast mechanical and thermal properties. The variegated venations found in nature is idealized into three principal fibers—the central mid-fiber corresponding to the mid-rib, straight parallel secondary fibers attached to the mid-fiber representing the secondary veins, and then another set of parallel fibers emanating from the secondary fibers mimicking the tertiary veins of a typical leaf. This paper addresses the in-plane thermal conductivity of such a composite by considering such a venous fiber morphology embedded in a matrix material. We have considered two cases, fibers having either higher or lower conductivity respect to the matrix. The tertiary fibers do not interconnect the secondary fibers in our present study. We carry out finite element based computational investigation of the thermal conductivity of these composites under uniaxial thermal gradients and study the effect of different fiber architectures. To this end, we use two broad types of architectures both having similar central main fiber but differing in either having only secondary fibers or additional tertiary fibers. The fiber and matrix volume fractions are kept constant and a comparative parametric study is carried out by varying the inclination of the secondary fibers. We find the heat conductivity in the direction of the main fiber (Y direction) increases significantly as the fiber angle of the secondary increases. Furthermore, for composite with metal fibers, the conductivity in the Y direction is further enhanced when composite is manufactured by having secondary fibers forming a closed cell structure. However, for composite with ceramic fibers, the conductivity of the composite in the Y direction is little affected by having secondary fibers closed. An opposite behavior is observed when considering conductivity of the composite in the X direction. The conductivity of the composite in the X direction is reduced with increase in the angle of the secondary fibers. Higher conductivity in the X direction is achieved for composite with no closed cells for composites with metal fibers. The results also indicate that for composites with the constant fiber volume fraction, morphology of tertiary fibers may not significantly alter material conductivities. In conclusion, introducing a leaf-mimicking topology in fiber architecture can provide significant additional degrees of tunability in design of these composite structures.

Mechanism of Single-Site Molecule-Like Catalytic Ethylene Dimerization in Ni-MFU-4l.

A recently developed metal-organic framework (MOF) catalyst for the dimerization of ethylene has a combination of selectivity and activity that surpasses that of commercial homogeneous catalysts, which have dominated this important industrial process for nearly 50 years. The uniform catalytic sites available in MOFs provide a unique opportunity to directly study reaction mechanisms in heterogeneous catalysts, a problem typically intractable due to the multiplicity of coordination environments found in many solid catalysts. In this work, we use a combination of isotopic labeling studies, mechanistic probes, and DFT calculations to demonstrate that Ni-MFU-4l operates via the Cossee-Arlman mechanism, which has also been implicated in homogeneous late transition metal catalysts. These studies demonstrate that metal nodes in MOFs mimic homogeneous catalysts not just functionally, but also mechanistically. They provide a blueprint for the development of advanced heterogeneous catalysts with similar degrees of tunability to their homogeneous counterparts.

Ferroelectric-Driven Performance Enhancement of Graphene Field-Effect Transistors Based on Vertical Tunneling Heterostructures.

A vertical graphene heterostructure field-effect transistor (VGHFET) using an ultrathin ferroelectric film as a tunnel barrier is developed. The heterostructure is capable of providing new degrees of tunability and functionality via coupling between the ferroelectricity and the tunnel current of the VGHFET, which results in a high-performance device. The results pave the way for developing novel atomic-scale 2D heterostructures and devices.

Magneto-tunable one-dimensional graphene-based photonic crystal

We investigate the effect of a perpendicular static magnetic field on the optical bandgap of a one-dimensional (1D) graphene-dielectric photonic crystal in order to examine the possibility of reaching a rich tunable photonic bandgap. The solution of the wave equation in the presence of the anisotropic Hall situation suggests two decoupled circularly polarized wave each exhibiting different degrees of bandgap tunability. It is also numerically demonstrated that applying different values of field intensity lead to perceptible changes in photonic bandgap of such a structure. Finally, the effect of opening a finite electronic gap in the spectrum of graphene on the optical dispersion solution of such a 1D photonic crystal is reported. It is shown that increasing the value of the electronic gap results in the shrinkage of the associated photonic bandgaps.

Transition Metal Dithiolene Near-IR Dyes and Their Applications in Liquid Crystal Devices

Numerous commercial and military applications exist for guest–host liquid crystal (LC) devices operating in the near- to mid-IR region. Progress in this area has been hindered by the severe lack of near-IR dyes with good solubility in the LC host, low impact on the inherent order of the LC phase, good thermal and chemical stability, and a large absorbance maximum tunable by structural modification over a broad range of the near-IR region. Transition metal complexes based on nickel, palladium, or platinum dithiolene cores show substantial promise in meeting these requirements. These new dye complexes are extraordinarily stable, possess liquid crystalline phases in their own right with the proper terminal functional groups, and can have melting points below room temperature. The latter property is especially significant for producing liquid crystal/dye mixtures with both high dye concentration and good resistance to phase separation. Because transition metal dithiolenes are zerovalent, they can exhibit high solubility in LC hosts (up to 10 wt%). The λmax in these materials can range from 600 to 1500 nm, depending on structure. Depending on their overall molecular geometry and the choice of terminal functional groups, transition metal dithiolenes that show either positive or negative dichroism from the same basic core structure can be readily synthesized. When enantiomerically enriched terminal substituents are employed, nickel dithiolenes can induce a chiral mesophase in a nonchiral nematic host. This finding opens the possibility of generating novel LC mixtures with two degrees of tunability—an electronic absorbance band tunable by synthesis, and a selective reflection band tunable by temperature or applied electric field. In this paper, we overview our past and present activities in the design and synthesis of transition metal dithiolene dyes, show some specific applications examples for these materials as near-IR dyes in LC electro-optical devices, and present our most recent results in the computational modeling of physical and optical properties of this interesting class of organometallic optical materials.