Revealing an important role of piezoelectric polymers in nervous-tissue regeneration: A review.

Nerve injuries pose a drastic threat to nerve mobility and sensitivity and lead to permanent dysfunction due to low regenerative capacity of mature neurons. The electrical stimuli that can be provided by electroactive materials are some of the most effective tools for the formation of soft tissues, including nerves. Electric output can provide a distinctly favorable bioelectrical microenvironment, which is especially relevant for the nervous system. Piezoelectric biomaterials have attracted attention in the field of neural tissue engineering owing to their biocompatibility and ability to generate piezoelectric surface charges. In this review, an outlook of the most recent achievements in the field of piezoelectric biomaterials is described with an emphasis on piezoelectric polymers for neural tissue engineering. First, general recommendations for the design of an optimal nerve scaffold are discussed. Then, specific mechanisms determining nerve regeneration via piezoelectric stimulation are considered. Activation of piezoelectric responses via natural body movements, ultrasound, and magnetic fillers is also examined. The use of magnetoelectric materials in combination with alternating magnetic fields is thought to be the most promising due to controllable reproducible cyclic deformations and deep tissue permeation by magnetic fields without tissue heating. In vitro and in vivo applications of nerve guidance scaffolds and conduits made of various piezopolymers are reviewed too. Finally, challenges and prospective research directions regarding piezoelectric biomaterials promoting nerve regeneration are discussed. Thus, the most relevant scientific findings and strategies in neural tissue engineering are described here, and this review may serve as a guideline both for researchers and clinicians.

Defining ferroelectric characteristics with reversible piezoresponse: PUND switching spectroscopy PFM characterization.

Detecting ferroelectricity at micro- and nanoscales is crucial for advanced nanomaterials and materials with complicated topography. Switching spectroscopy piezoresponse force microscopy (SSPFM), which involves measuring piezoelectric hysteresis loops via a scanning probe microscopy tip, is a widely accepted approach to characterize polarization reversal at the local scale and confirm ferroelectricity. However, the local hysteresis loops acquired through this method often exhibit unpredictable shapes, a phenomenon often attributed to the influence of parasitic factors such as electrostatic forces and current flow. Our research has uncovered that the deviation in hysteresis loop shapes can be caused by spontaneous backswitching occurring after polarization reversal. Moreover, we've determined that the extent of this effect can be exacerbated when employing inappropriate SSPFM waveform parameters, including duration, frequency, and AC voltage amplitude. Notably, the conventional 'pulse-mode' SSPFM method has been found to intensify spontaneous backswitching. In response to these challenges, we have redesigned SSPFM approach by introducing the positive up-negative down (PUND) method within the 'step-mode' SSPFM. This modification allows for effective probing of local piezoelectric hysteresis loops in ferroelectrics with reversible piezoresponse while removing undesirable electrostatic contribution. This advancement extends the applicability of the technique to a diverse range of ferroelectrics, including semiconductor ferroelectrics and relaxors, promising a more reliable and accurate characterization of their properties.

Piezoactive Bioorganic Diphenylalanine Films: Mechanism of Phase Formation.

Self-organized peptides are unique materials with various applications in biology, medicine, and nanotechnology. Many of these applications require fabrication of homogeneous thin films having high piezoelectric effect and sufficiently low roughness. Recently, a facile method for the controlled deposition of flat solid films of the most studied peptide, diphenylalanine (FF), has been proposed, which is based on the crystallization of FF in the amorphous phase under the action of water vapor. This method is very advantageous compared with crystallization from a liquid phase reported previously. Here, we thoroughly investigate the mechanism of solid-state transformation from the amorphous to crystalline phase. The study revealed that the process proceeds in two distinct stages, maintaining clamped condition of self-assembling building blocks that preserve the films' morphology and high piezoelectric activity. We emphasize the critical role of water diffusion that governs two-dimensional growth of crystalline domains in FF films, merging in very dense, flat, and homogeneous films. These findings open a wide perspective for using this methodology for the direct fabrication of biofilms from the amorphous phase. We thus expect the application of these films to various nanotechnological applications of self-assembled structures.

A hybrid double perovskite ferroelastic exhibiting the highest number of orientation states.

Integrating NH4+ as a B'-site ion within a three-dimensional double hybrid perovskite resulted in a novel high-temperature ferroelastic, (Me3NOH)2(NH4)[Co(CN)6], which uniquely demonstrates a reversible triclinic-to-cubic phase transition at 369 K and offers a record-setting 24 orientation states, the highest ever reported among all ferroelastics.

Effect of Fe3O4 Nanoparticles Modified by Citric and Oleic Acids on the Physicochemical and Magnetic Properties of Hybrid Electrospun P(VDF-TrFE) Scaffolds.

This study considers a fabrication of magnetoactive scaffolds based on a copolymer of vinylidene fluoride and trifluoroethylene (P(VDF-TrFE)) and 5, 10, and 15 wt.% of magnetite (Fe3O4) nanoparticles modified with citric (CA) and oleic (OA) acids by solution electrospinning. The synthesized Fe3O4-CA and Fe3O4-OA nanoparticles are similar in particle size and phase composition, but differ in zeta potential values and magnetic properties. Pure P(VDF-TrFE) scaffolds as well as composites with Fe3O4-CA and Fe3O4-OA nanoparticles demonstrate beads-free 1 µm fibers. According to scanning electron (SEM) and transmission electron (TEM) microscopy, fabricated P(VDF-TrFE) scaffolds filled with CA-modified Fe3O4 nanoparticles have a more homogeneous distribution of magnetic filler due to both the high stabilization ability of CA molecules and the affinity of Fe3O4-CA nanoparticles to the solvent used and P(VDF-TrFE) functional groups. The phase composition of pure and composite scaffolds includes a predominant piezoelectric ß-phase, and a γ-phase, to a lesser extent. When adding Fe3O4-CA and Fe3O4-OA nanoparticles, there was no significant decrease in the degree of crystallinity of the P(VDF-TrFE), which, on the contrary, increased up to 76% in the case of composite scaffolds loaded with 15 wt.% of the magnetic fillers. Magnetic properties, mainly saturation magnetization (Ms), are in a good agreement with the content of Fe3O4 nanoparticles and show, among the known magnetoactive PVDF or P(VDF-TrFE) scaffolds, the highest Ms value, equal to 10.0 emu/g in the case of P(VDF-TrFE) composite with 15 wt.% of Fe3O4-CA nanoparticles.

Molecular Design of a Metal-Nitrosyl Ferroelectric with Reversible Photoisomerization.

The development of photo-responsive ferroelectrics whose polarization may be remotely controlled by optical means is of fundamental importance for basic research and technological applications. Herein, we report the design and synthesis of a new metal-nitrosyl ferroelectric crystal (DMA)(PIP)[Fe(CN)5(NO)] (1) (DMA = dimethylammonium, PIP = piperidinium) with potential phototunable polarization via a dual-organic-cation molecular design strategy. Compared to the parent non-ferroelectric (MA)2[Fe(CN)5(NO)] (MA = methylammonium) material with a phase transition at 207 K, the introduction of larger dual organic cations both lowers the crystal symmetry affording robust ferroelectricity and increases the energy barrier of molecular motions, endowing 1 with a large polarization of up to 7.6 µC cm-2 and a high Curie temperature (Tc) of 316 K. Infrared spectroscopy shows that the reversible photoisomerization of the nitrosyl ligand is accomplished by light irradiation. Specifically, the ground state with the N-bound nitrosyl ligand conformation can be reversibly switched to both the metastable state I (MSI) with isonitrosyl conformation and the metastable state II (MSII) with side-on nitrosyl conformation. Quantum chemistry calculations suggest that the photoisomerization significantly changes the dipole moment of the [Fe(CN)5(NO)]2- anion, thus leading to three ferroelectric states with different values of macroscopic polarization. Such optical accessibility and controllability of different ferroelectric states via photoinduced nitrosyl linkage isomerization open up a new and attractive route to optically controllable macroscopic polarization.

Novel Biocompatible Magnetoelectric MnFe2 O4 Core@BCZT Shell Nano-Hetero-Structures with Efficient Catalytic Performance.

Magnetoelectric (ME) small-scale robotic devices attract great interest from the scientific community due to their unique properties for biomedical applications. Here, novel ME nano hetero-structures based on the biocompatible magnetostrictive MnFe2 O4 (MFO) and ferroelectric Ba0.85 Ca0.15 Zr0.1 Ti0.9 O3 (BCZT) are developed solely via the hydrothermal method for the first time. An increase in the temperature and duration of the hydrothermal synthesis results in increasing the size, improving the purity, and inducing morphology changes of MFO nanoparticles (NPs). A successful formation of a thin epitaxial BCZT-shell with a 2-5 nm thickness is confirmed on the MFO NPs (77 ± 14 nm) preliminarily treated with oleic acid (OA) or polyvinylpyrrolidone (PVP), whereas no shell is revealed on the surface of pristine MFO NPs. High magnetization is revealed for the developed ME NPs based on PVP- and OA-functionalized MFO NPs (18.68 ± 0.13 and 20.74 ± 0.22 emu g-1 , respectively). Moreover, ME NPs demonstrate 95% degradation of a model pollutant Rhodamine B within 2.5 h under an external AC magnetic field (150 mT, 100 Hz). Thus, the developed biocompatible core-shell ME NPs of MFO and BCZT can be considered as a promising tool for non-invasive biomedical applications, environmental remediation, and hydrogen generation for renewable energy sources.

Quantitative Characterization of Local Thermal Properties in Thermoelectric Ceramics Using "Jumping-Mode" Scanning Thermal Microscopy.

Thermoelectric conversion may take a significant share in future energy technologies. Oxide-based thermoelectric composite ceramics attract attention for promising routes for control of electrical and thermal conductivity for enhanced thermoelectric performance. However, the variability of the composite properties responsible for the thermoelectric performance, despite nominally identical preparation routes, is significant, and this cannot be explained without detailed studies of thermal transport at the local scale. Scanning thermal microscopy (SThM) is a scanning probe microscopy method providing access to local thermal properties of materials down to length scales below 100 nm. To date, realistic quantitative SThM is shown mostly for topographically very smooth materials. Here, methods for SThM imaging of bulk ceramic samples with relatively rough surfaces are demonstrated. "Jumping mode" SThM (JM-SThM), which serves to preserve the probe integrity while imaging rough surfaces, is developed and applied. Experiments with real thermoelectric ceramics show that the JM-SThM can be used for meaningful quantitative imaging. Quantitative imaging is performed with the help of calibrated finite-elements model of the SThM probe. The modeling reveals non-negligible effects associated with the distributed nature of the resistive SThM probes used; corrections need to be made depending on probe-sample contact thermal resistance and probe current frequency.

Spatially-Resolved Study of the Electronic Transport and Resistive Switching in Polycrystalline Bismuth Ferrite.

Ferroelectric materials attract much attention for applications in resistive memory devices due to the large current difference between insulating and conductive states and the ability of carefully controlling electronic transport via the polarization set-up. Bismuth ferrite films are of special interest due to the combination of high spontaneous polarization and antiferromagnetism, implying the possibility to provide multiple physical mechanisms for data storage and operations. Macroscopic conductivity measurements are often hampered to unambiguously characterize the electric transport, because of the strong influence of the diverse material microstructure. Here, we studied the electronic transport and resistive switching phenomena in polycrystalline bismuth ferrite using advanced conductive atomic force microscopy (CAFM) at different temperatures and electric fields. The new approach to the CAFM spectroscopy and corresponding data analysis are proposed, which allow deep insight into the material band structure at high lateral resolution. Contrary to many studies via macroscopic methods, postulating electromigration of the oxygen vacancies, we demonstrate resistive switching in bismuth ferrite to be caused by the pure electronic processes of trapping/releasing electrons and injection of the electrons by the scanning probe microscopy tip. The electronic transport was shown to be comprehensively described by the combination of the space charge limited current model, while a Schottky barrier at the interface is less important due to the presence of the built-in subsurface charge.

A Comprehensive Study of Synthesis and Analysis of Anisotropic Iron Oxide and Oxyhydroxide Nanoparticles.

One-dimensional anisotropic nanoparticles are of great research interest across a wide range of biomedical applications due to their specific physicochemical and magnetic properties in comparison with isotropic magnetic nanoparticles. In this work, the formation of iron oxides and oxyhydroxide anisotropic nanoparticles (ANPs) obtained by the co-precipitation method in the presence of urea was studied. Reaction pathways of iron oxide and oxyhydroxide ANPs formation are described based on of X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and pulse magnetometry studies. It is shown that a nonmonotonic change in the Fe3O4 content occurs during synthesis. The maximum content of the Fe3O4 phase of 47.4% was obtained at 12 h of the synthesis. At the same time, the reaction products contain ANPs of α-FeOOH and submicron isotropic particles of Fe3O4, the latter formation can occur due to the oxidation of Fe2+ ions by air-oxygen and Ostwald ripening processes. A subsequent increase in the synthesis time leads to the predominant formation of an α-FeOOH phase due to the oxidation of Fe3O4. As a result of the work, a methodological scheme for the analysis of iron oxide and oxyhydroxide ANPs was developed.

Triboelectric Generator Based on Oriented Self-Assembled Peptide Microbelts.

Along with piezoelectric nanogenerators, triboelectric nanogenerators (TENGs) collecting energy from mechanical vibrations proved to be simple, low-cost, and efficient sources of electricity for various applications. In view of possible biomedical applications, the search for TENGs made of biomolecular and biocompatible materials is demanding. Diphenylalanine (FF) microstructures are promising for these applications due to their unique characteristics and ability to form various morphologies (microribbons, spherical vesicles, fibrils, micro- and nanotubes, nanorods, etc.). In this work, we developed a contact-separate mode TENG based on arrays of oriented FF microbelts deposited by dip-coating technique and studied their performance under various temperature treatments. We show that these TENGs outperform piezoelectric nanogenerators based on FF microbelts in terms of short-circuit current (ISC), open-circuit voltage (VOC), and output power. It was found that bound water captured in FF nanochannels mainly affects VOC, whereas mobile water increases ISC. We also found that the cyclization of FF molecules increases the performance of TENG likely due to an increase in surface energy and surface flattening.

Comprehensive Study on the Reinforcement of Electrospun PHB Scaffolds with Composite Magnetic Fe3O4-rGO Fillers: Structure, Physico-Mechanical Properties, and Piezoelectric Response.

This is a comprehensive study on the reinforcement of electrospun poly(3-hydroxybutyrate) (PHB) scaffolds with a composite filler of magnetite-reduced graphene oxide (Fe3O4-rGO). The composite filler promoted the increase of average fiber diameters and decrease of the degree of crystallinity of hybrid scaffolds. The decrease in the fiber diameter enhanced the ductility and mechanical strength of scaffolds. The surface electric potential of PHB/Fe3O4-rGO composite scaffolds significantly increased with increasing fiber diameter owing to a greater number of polar functional groups. The changes in the microfiber diameter did not have any influence on effective piezoresponses of composite scaffolds. The Fe3O4-rGO filler imparted high saturation magnetization (6.67 ± 0.17 emu/g) to the scaffolds. Thus, magnetic PHB/Fe3O4-rGO composite scaffolds both preserve magnetic properties and provide a piezoresponse, whereas varying the fiber diameter offers control over ductility and surface electric potential.

Engineering of Pyroelectric Crystals Decoupled from Piezoelectricity as Illustrated by Doped α-Glycine.

Design of pyroelectric crystals decoupled from piezoelectricity is not only a topic of scientific curiosity but also demonstrates effects in principle that have the potential to be technologically advantageous. Here we report a new method for the design of such materials. Thus, the co-doping of centrosymmetric crystals with tailor-made guest molecules, as illustrated by the doping of α-glycine with different amino acids (Threonine, Alanine and Serine). The polarization of those crystals displays two distinct contributions, one arising from the difference in dipole moments between guest and host and the other from the displacement of host molecules from their symmetry-related positions. These contributions exhibit different temperature dependences and response to mechanical deformation. Thus, providing a proof of concept for the ability to design pyroelectric materials with reduced piezoelectric coefficient (d22 ) to a minimal value, below the resolution limit of the method (<0.005 pm/V).

Piezo-Responsive Hydrogen-Bonded Frameworks Based on Vanillin-Barbiturate Conjugates.

A concept of piezo-responsive hydrogen-bonded π-π-stacked organic frameworks made from Knoevenagel-condensed vanillin-barbiturate conjugates was proposed. Replacement of the substituent at the ether oxygen atom of the vanillin moiety from methyl (compound 3a) to ethyl (compound 3b) changed the appearance of the products from rigid rods to porous structures according to optical microscopy and scanning electron microscopy (SEM), and led to a decrease in the degree of crystallinity of corresponding powders according to X-ray diffractometry (XRD). Quantum chemical calculations of possible dimer models of vanillin-barbiturate conjugates using density functional theory (DFT) revealed that π-π stacking between aryl rings of the vanillin moiety stabilized the dimer to a greater extent than hydrogen bonding between carbonyl oxygen atoms and amide hydrogen atoms. According to piezoresponse force microscopy (PFM), there was a notable decrease in the vertical piezo-coefficient upon transition from rigid rods of compound 3a to irregular-shaped aggregates of compound 3b (average values of d33 coefficient corresponded to 2.74 ± 0.54 pm/V and 0.57 ± 0.11 pm/V), which is comparable to that of lithium niobate (d33 coefficient was 7 pm/V).

Core-Shell Magnetoactive PHB/Gelatin/Magnetite Composite Electrospun Scaffolds for Biomedical Applications.

Novel hybrid magnetoactive composite scaffolds based on poly(3-hydroxybutyrate) (PHB), gelatin, and magnetite (Fe3O4) were fabricated by electrospinning. The morphology, structure, phase composition, and magnetic properties of composite scaffolds were studied. Fabrication procedures of PHB/gelatin and PHB/gelatin/Fe3O4 scaffolds resulted in the formation of both core-shell and ribbon-shaped structure of the fibers. In case of hybrid PHB/gelatin/Fe3O4 scaffolds submicron-sized Fe3O4 particles were observed in the surface layers of the fibers. The X-ray photoelectron spectroscopy results allowed the presence of gelatin on the fiber surface (N/C ratio-0.11) to be revealed. Incubation of the composite scaffolds in saline for 3 h decreased the amount of gelatin on the surface by more than ~75%. The differential scanning calorimetry results obtained for pure PHB scaffolds revealed a characteristic melting peak at 177.5 °C. The presence of gelatin in PHB/gelatin and PHB/gelatin/Fe3O4 scaffolds resulted in the decrease in melting temperature to 168-169 °C in comparison with pure PHB scaffolds due to the core-shell structure of the fibers. Hybrid scaffolds also demonstrated a decrease in crystallinity from 52.3% (PHB) to 16.9% (PHB/gelatin) and 9.2% (PHB/gelatin/Fe3O4). All the prepared scaffolds were non-toxic and saturation magnetization of the composite scaffolds with magnetite was 3.27 ± 0.22 emu/g, which makes them prospective candidates for usage in biomedical applications.

Exploring Charged Defects in Ferroelectrics by the Switching Spectroscopy Piezoresponse Force Microscopy.

Monitoring the charged defect concentration at the nanoscale is of critical importance for both the fundamental science and applications of ferroelectrics. However, up-to-date, high-resolution study methods for the investigation of structural defects, such as transmission electron microscopy, X-ray tomography, etc., are expensive and demand complicated sample preparation. With an example of the lanthanum-doped bismuth ferrite ceramics, a novel method is proposed based on the switching spectroscopy piezoresponse force microscopy (SSPFM) that allows probing the electric potential from buried subsurface charged defects in the ferroelectric materials with a nanometer-scale spatial resolution. When compared with the composition-sensitive methods, such as neutron diffraction, X-ray photoelectron spectroscopy, and local time-of-flight secondary ion mass spectrometry, the SSPFM sensitivity to the variation of the electric potential from the charged defects is shown to be equivalent to less than 0.3 at% of the defect concentration. Additionally, the possibility to locally evaluate dynamics of the polarization screening caused by the charged defects is demonstrated, which is of significant interest for further understanding defect-mediated processes in ferroelectrics.

Wake-up Free Ferroelectric Rhombohedral Phase in Epitaxially Strained ZrO2 Thin Films.

Zirconia- and hafnia-based thin films have attracted tremendous attention in the past decade because of their unexpected ferroelectric behavior at the nanoscale, which enables the downscaling of ferroelectric devices. The present work reports an unprecedented ferroelectric rhombohedral phase of ZrO2 that can be achieved in thin films grown directly on (111)-Nb:SrTiO3 substrates by ion-beam sputtering. Structural and ferroelectric characterizations reveal (111)-oriented ZrO2 films under epitaxial compressive strain exhibiting switchable ferroelectric polarization of about 20.2 µC/cm2 with a coercive field of 1.5 MV/cm. Moreover, the time-dependent polarization reversal characteristics of Nb:SrTiO3/ZrO2/Au film capacitors exhibit typical bell-shaped curve features associated with the ferroelectric domain reversal and agree well with the nucleation limited switching (NLS) model. The polarization-electric field hysteresis loops point to an activation field comparable to the coercive field. Interestingly, the studied films show ferroelectric behavior per se, without the need to apply the wake-up cycle found in the orthorhombic phase of ZrO2. Overall, the rhombohedral ferroelectric ZrO2 films present technological advantages over the previously studied zirconia- and hafnia-based thin films and may be attractive for nanoscale ferroelectric devices.

Hybrid Triboelectric-Electromagnetic Nanogenerators for Mechanical Energy Harvesting: A Review.

Motion-driven electromagnetic-triboelectric energy generators (E-TENGs) hold a great potential to provide higher voltages, higher currents and wider operating bandwidths than both electromagnetic and triboelectric generators standing alone. Therefore, they are promising solutions to autonomously supply a broad range of highly sophisticated devices. This paper provides a thorough review focused on major recent breakthroughs in the area of electromagnetic-triboelectric vibrational energy harvesting. A detailed analysis was conducted on various architectures including rotational, pendulum, linear, sliding, cantilever, flexible blade, multidimensional and magnetoelectric, and the following hybrid technologies. They enable highly efficient ways to harvest electric energy from many forms of vibrational, rotational, biomechanical, wave, wind and thermal sources, among others. Open-circuit voltages up to 75 V, short-circuit currents up to 60 mA and instantaneous power up to 144 mW were already achieved by these nanogenerators. Their transduction mechanisms, including proposed models to make intelligible the involved physical phenomena, are also overviewed here. A comprehensive analysis was performed to compare their respective construction designs, external excitations and electric outputs. The results highlight the potential of hybrid E-TENGs to convert unused mechanical motion into electric energy for both large- and small-scale applications. Finally, this paper proposes future research directions toward optimization of energy conversion efficiency, power management, durability and stability, packaging, energy storage, operation input, research of transduction mechanisms, quantitative standardization, system integration, miniaturization and multi-energy hybrid cells.

Modeling of Self-Assembled Peptide Nanotubes and Determination of Their Chirality Sign Based on Dipole Moment Calculations.

The chirality quantification is of great importance in structural biology, where the differences in proteins twisting can provide essentially different physiological effects. However, this aspect of the chirality is still poorly studied for helix-like supramolecular structures. In this work, a method for chirality quantification based on the calculation of scalar triple products of dipole moments is suggested. As a model structure, self-assembled nanotubes of diphenylalanine (FF) made of L- and D-enantiomers were considered. The dipole moments of FF molecules were calculated using semi-empirical quantum-chemical method PM3 and the Amber force field method. The obtained results do not depend on the used simulation and calculation method, and show that the D-FF nanotubes are twisted tighter than L-FF. Moreover, the type of chirality of the helix-like nanotube is opposite to that of the initial individual molecule that is in line with the chirality alternation rule general for different levels of hierarchical organization of molecular systems. The proposed method can be applied to study other helix-like supramolecular structures.

Local Piezoelectric Properties of Doped Biomolecular Crystals.

Piezoelectricity is the ability of certain crystals to generate mechanical strain proportional to an external electric field. Though many biomolecular crystals contain polar molecules, they are frequently centrosymmetric, signifying that the dipole moments of constituent molecules cancel each other. However, piezoelectricity can be induced by stereospecific doping leading to symmetry reduction. Here, we applied piezoresponse force microscopy (PFM), highly sensitive to local piezoelectricity, to characterize (01¯0) faces of a popular biomolecular material, α-glycine, doped with other amino acids such as L-alanine and L-threonine as well as co-doped with both. We show that, while apparent vertical piezoresponse is prone to parasitic electrostatic effects, shear piezoelectric activity is strongly affected by doping. Undoped α-glycine shows no shear piezoelectric response at all. The shear response of the L-alanine doped crystals is much larger than those of the L-threonine doped crystals and co-doped crystals. These observations are rationalized in terms of host-guest molecule interactions.