Spontaneous Strain Research Articles

Structure and thermal expansion of end-member olivines I: Crystal and magnetic structure, thermal expansion, and spontaneous magnetostriction of synthetic fayalite, Fe2SiO4, determined by high-resolution neutron powder diffraction

AbstractThe lattice parameters and the crystal and magnetic structures of Fe2SiO4 have been determined from 10 K to 1453 K by high-resolution time-of-flight neutron powder diffraction. Fe2SiO4 undergoes two antiferromagnetic phase transformations on cooling from room temperature: the first, at 65.4 K, is to a collinear antiferromagnet with moments on two symmetry-independent Fe ions; the second transition, at ~23 K, is to a structure in which the moments on one of the sets of Fe ions (those on the ‘M1 site’) become canted. The magnetic unit cell is identical to the crystallographic (chemical) unit cell and the space group remains Pbnm throughout. The magnetic structures have been refined and the results found to be in good agreement with previous studies; however, we have determined the spontaneous magnetostrictive strains, which have not been reported previously. In the paramagnetic phase of Fe2SiO4, at temperatures of 70 K and above, we find that the temperature dependence of the linear thermal expansion coefficient of the b axis takes an unusual form. In contrast to the behaviour of the expansion coefficients of the unit-cell volume and of the a and c axes, which show the expected reduction in magnitude below ~300 K, that of the b axis remains almost constant between ~70 K and 1000 K.

Characterization of a Novel Gja8 (Cx50) Mutation in a New Cataract Rat Model.

To describe a novel spontaneous cataract inbred strain isolated from large-scale breeding SD rats, identify the responsible gene mutation, and understand how this mutation affects lens function. Exome sequencing of 12 cataract-associated genes was performed in the affected and healthy relatives. Sequences of rat wild-type or mutant gap junction protein alpha 8 gene (Gja8) were transfected into cells. The expression level of protein was assayed by Western blot analysis. Subcellular localization of connexin 50 (Cx50) was analyzed in confocal fluorescent images. Wound-healing, 5-ethynyl-2'-deoxyuridine incorporation, and attachment assay were performed to characterize the cell migration, proliferation and adhesion. The abnormality was found to be inheritable in an autosomal semi-dominant pattern through different mating patterns. We found a G to T transversion at codon 655 in Gja8, leading to a substitution of valine by phenylalanine (p.V219F). Gja8V219F/+ heterozygotes expressed nuclear cataract while Gja8V219F/V219F homozygotes manifested microphthalmia in addition to cataract. Histology revealed fiber disorders and loss of organelle-free zone in the mutant lens. Cx50V219F altered its location in HeLa cells and inhibited the proliferation, migration and adhesion abilities of HLEB3 cells. The mutation also reduced the expression of focal adhesion kinase and its phosphorylation. The c.655G>T mutation (p.V219F) is a novel mutation in Gja8, inducing semi-dominant nuclear cataracts in a new spontaneous cataract rat model. The p.V219F mutation altered Cx50 distribution, inhibited lens epithelial cell proliferation, migration, and adhesion, and disrupted fiber cell differentiation. As a consequence, the nuclear cataract and small lens formed.

Temperature- and pressure-induced structural transformations in NbN: A first-principles study

Structural transformations at high temperatures and pressures, elastic moduli, hardness, fracture toughness, Debye temperature, stress-shear strain relations, electronic structure, and lattice dynamics in the experimentaly observed NaCl–NbN (δ, Fm-3m), anti-TiP-NbN (ε, P63/mmc), anti-NiAs-NbN (δ′, P63/mmc), WC-NbN (η, P-6m2), and TiP–NbN (ε′, P63/mmc) phases and hypothetical new tP4-129 (P4/nmm), hP6-189 (P-62m), oP8-25 (Pmm2) and cP2-221 (Pm-3m) structures are studied by using first-principles calculations and molecular dynamics simulations. The possible mechanisms of the phase transitions between these structures based on the condensation of a certain phonon mode with subsequent spontaneous strains are suggested. The ε, η and δ′, and cP2-221 structures are brittle materials and exhibit highest shear moduli (200.5–216.8 GPa), Young moduli (492.4–528.8 GPa), Vickers hardness (23.9–27.1 GPa), fracture toughness (4.54–4.72 MPa m1/2), and Debye temperatures (730.5–767.0 K). It is found that the main slip systems should be (0001)<10-10> for ε and η, and both (0001)<10-10> and (0001)<-12-10> for δ’.

Heterogeneity among Clinical Intestinal Escherichia coli Isolates upon Acquired Streptomycin Resistance.

Escherichia coli isolates from inflammatory bowel disease (IBD) patients are often multidrug resistant, including to streptomycin. Streptomycin resistance (StrR) mutations can alter bacterial behavior, which may influence intestinal disease. We generated a spontaneous StrR strain of the intestinal adherent-invasive E. coli (AIEC) strain NC101. Whole-genome sequencing revealed a single missense mutation in rpsL that commonly confers StrR, rpsL-K43N. StrR NC101 exhibited a striking loss of aggregation and significantly increased motility, behaviors that can impact host-microbe interactions. Behavioral changes were associated with reduced transcription of csgA, encoding the biofilm component curli, and increased transcription of fliC, encoding flagellin. Scanning electron microscopy (SEM) detailed morphologic changes consistent with the observed alterations in multicellular behavior. Because intestinal E. coli isolates exhibit remarkable strain-specific differences, we generated spontaneous StrR mutants of 10 clinical E. coli phylotype B2 strains from patients with IBD, colorectal cancer, and urinary tract infection. Out of these 10 StrR clinical strains, two had altered colony morphology on Congo red agar (suggesting changes in extracellular products), and three had significant changes in motility. These changes were not associated with a particular rpsL mutation nor with the presence of virulence genes encoding the inflammation-associated E. coli metabolites yersiniabactin or colibactin. We conclude that common mutations in rpsL, which confer StrR, can differentially alter disease-associated phenotypes across intestinal E. coli strains. These findings highlight the heterogeneity among seemingly similar intestinal E. coli strains and reveal the need to carefully study the strain-specific effects of antibiotic resistance mutations, particularly when using these mutations during strain selection studies. IMPORTANCE We demonstrate that StrR, commonly acquired through a single point mutation in rpsL (a gene encoding part of the 30S bacterial ribosome), strikingly alters the morphology and behavior of a key intestinal AIEC strain, NC101. These changes include remarkably diminished aggregation and significantly increased motility, traits that are linked to AIEC-defining features and disease development. Phenotypic changes were heterogeneous among other StrR clinical E. coli strains, underscoring the need to evaluate the strain-specific effects of commonly acquired antibiotic resistance mutations. This is important, as the results of studies using mutant StrR Enterobacteriaceae strains (e.g., for cloning or in vivo selection) may be confounded beyond our demonstrated effects. Long term, these findings can help researchers better distinguish the contribution of specific E. coli traits to functional changes in the microbiota. Evaluating these strain-level differences could provide insight into the diversity of IBD symptoms and lead to improved therapies for microbiota-driven intestinal disorders.

Spontaneous Strain in Quasi-Two-Dimensional Janus CdSe Nanoplatelets and Its Microscopic Mechanisms

Spontaneous strain and spontaneous folding of thin nanoplatelets are known phenomena whose microscopic mechanisms are still debated. In this work, first-principles calculations are used to study the mechanical stresses that arise in Janus CdSe nanoplatelets and result in their spontaneous strain. Calculations reveal the existence of three microscopic mechanisms of this phenomenon. Two bulk mechanisms are associated with the inverse piezoelectric effect in an electric field created by the difference in electronegativities of ligands and by the depolarizing field resulting from the difference in the potential jumps in electrical double layers on the surfaces of nanoplatelets. These mechanisms account for 5–25% of the observed effect. The third mechanism is associated with the surface strain of nanoplatelets by bridging bonds, and its influence is predominant. It is shown that the latter mechanism causes spontaneous folding of thin CdSe nanoplatelets and, depending on the values of surface stresses and lateral orientation of nanoplatelets, can result in formation of their experimentally observed structures such as scrolls, spirals, and twisted ribbons.

PREPARATION OF NEW HARD ELASTIC POLYMERIC MATERIAL BASED ON ULTRA-HIGH MOLECULAR WEIGHT POLYETHYLENE

A novel approach for the preparation of hard elastic polymeric material based on ultra-high molecular weight polyethylene via the strategy of crazing of polymers has been proposed. This approach includes the process of deformation of the pristine films of ultra-high molecular weight polyethylene via environmental intercrystallite crazing mechanism and subsequent low-temperature spontaneous strain recovery upon stress relaxation. As a result, the material acquires new properties typical for hard elastic materials: restoration of the porous structure upon secondary loading in air up to ~20 vol. % with pore sizes in the nanometer range (up to 10 nm), high reversibility of deformation (50−85%), the effect of opening and closing pores upon cyclic loading. The mechanism of this phenomenon has been proposed and the areas of practical applications of such mechanoresponsive material have been indicated.

Strain Effects in Twisted Spiral Antimonene.

Van der Waals (vdW) layered materials exhibit fruitful novel physical properties. The energy band of such materials depends strongly on their structures, and a tremendous variation in their physical properties can be deduced from a tiny change in inter-layer spacing, twist angle, or in-plane strain. In this work, a kind of vdW layered material of spiral antimonene is constructed, and the strain effects in the material are studied. The spiral antimonene is grown on a germanium (Ge) substrate and is induced by a helical dislocation penetrating through few atomic-layers of antimonene (β-phase). The as-grown spiral is intrinsically strained, and the lattice distortion is found to be pinned around the dislocation. Both spontaneous inter-layer twist and in-plane anisotropic strain are observed in scanning tunneling microscope (STM) measurements. The strain in the spiral antimonene can be significantly modified by STM tip interaction, leading to a variation in the surface electronic density of states (DOS) and a large modification in the work function of up to a few hundreds of millielectron-volts (meV). Those strain effects are expected to have potential applications in building up novel piezoelectric devices.

Pressure induced isostructural phase transition with volume expansion in DyFeO3 orthoferrite

The orthorhombic O and O′ structure phases of ABO3-type perovskites possess the same symmetry and quite different physical properties. In this work, a pressure induced isostructural O′–O phase transition with volume expansion and less distortion in DyFeO3 orthoferrite was experimentally observed and studied by high-pressure x-ray diffraction and Raman spectroscopy measurements. Up to 35.2 GPa, DyFeO3 crystallizes in an orthorhombic Pbnm symmetry structure. With no change in the symmetry group, distinct O′-phase and O-phase were verified below 13.1 GPa and above 15.1 GPa, respectively. Meanwhile, the lattice becomes less distorted and metrically pseudo-cubic on the high-pressure side. The cell volume expands by a step in the intermediate pressure window accompanied by a decrease in spontaneous strain. It is suggested that FeO6 octahedra are more compressible than DyO12 sites under pressure. This work claimed the physical mechanism underlying phonon dynamics and variation of local structure symmetry of DyFeO3, which can be considered as the basic view for RFeO3 perovskites.

Ferroelastic phase transitions in three new layered perovskites: (3-XC6H5CH2CH2NH3)2[CdCl4] (X = F, Cl, and Br)

Two-dimensional organic-inorganic hybrid ferroelastics with high-temperature reversible phase transitions are very rare and have become one of the research hotspots in the field of ferroelastic materials. Herein, we report three new layered organic-inorganic hybrid perovskites based on halogen-substituted phenethylaminium, (3-XC6H5CH2CH2NH3)2[CdCl4] (X = F (1), Cl (2) and Br (3)). They undergo structural phase transitions at 376/371 K, 436/430 K, and 421/411 K, respectively, between the isomorphic high-temperature phases (space group I4/mmm, Z = 2) and different room-temperature phases with the reduced structural symmetries, i.e., P21/a (Z = 2) in 1, P1¯ (Z = 4) in 2, and P21/a (Z = 4) in 3, respectively. These ferroelastic transitions arise from the order-disorder transition of organic cations together with the synchronous displacement of inorganic layers, accompanying with ferroelastic spontaneous strains of 0.16, 0.13 and 0.12 for 1−3, respectively. By enriching layered perovskite ferroelastics based on halogen-substituted cations, this work provides important clues for exploring new ferroic materials based on hybrid crystals.

Attenuating liquid crystal elastomers’ stress concentration by programming initial orientation

Liquid crystal elastomers (LCEs) are a kind of soft smart materials with fascinating programmability and have a broad application prospect. The monodomain LCEs under loading exhibit the semi-soft elasticity due to the stress-induced director rotation and the resulting spontaneous strain. In this article, we aim to reduce the severe stress concentration of LCEs by programming the initial director orientations. We numerically studied the stress concentration behaviors of a LCE sheet containing a small circular hole with different distribution of initial director under uniaxial loading. For monodomain LCE sheets, the stress concentration factor monotonically decreases as the initial director orientation deviates from the loading direction, and achieves its minimum when the deviation angle reaches 45°. This reduction of stress concentration is attributed to the smaller relative net director rotation and the lower resulting spontaneous strain near the hole edge as the deviation angle increases. Since the director rotation near the hole edge is critical for the attenuation of stress concentration, we only program the initial director orientation near the hole edge, and achieve up to 50% reduction in stress concentration factor. Increasing the size of programming area also enhances the attenuation of stress concentration. This work provides a new strategy to reduce the stress concentration in LCEs with geometric defects.

Templating Influence of Regulated Inorganic Framework in Two-Dimensional Ferroelastic Perovskites: (C3 H5 CH2 NH3 )2 [MCl4 ] (M=Mn and Cd).

The remarkable material stability and structural diversity of two-dimensional (2D) organic-inorganic hybrid perovskites (OIHPs) constitute a vast available library of versatile materials. In particular, ferroelastic property, for which the spontaneous strain can be transformed by applying mechanical stress, is very promising for extensive nanotechnological applications. However, integrating ferroelastic property into 2D OIHPs is still in its infancy. Herein, we designed two new 2D OIHPs (C3 H5 CH2 NH3 )2 [MCl4 ] (M=Mn for 1 and Cd for 2), which undergo reversible ferroelastic phase transitions with an Aizu expression 4/mmmFmmm. The templating influence of the more distorted inorganic framework on the disordering of organic cations and the stronger hydrogen bonds has a key role in the striking improvement of Curie temperature from 246 K in 1 to 273 K in 2. Meanwhile, the minimized alteration of structural motif ensures the well maintaining of the ferroelastic performance in the forms of crystals and thin films, as demonstrated by the identifiable evolution of domain structures. This work will provide a fertile new ground for enlarging the limited number of 2D ferroelastic OIHPs with better practical utility.

Soft Actuators Based on Spin‐Crossover Particles Embedded in Thermoplastic Polyurethane

Molecular spin‐crossover (SCO) complexes are phase‐change materials that develop large spontaneous strains across the thermally induced phase transition, which can be advantageously used in designing soft actuators. Herein, a bilayer bending cantilever, made of thermoplastic polyurethane (TPU) with embedded [Fe(NH2trz)3](SO4) SCO particles (25 wt%), is presented. The proposed actuator is fabricated by blade casting an SCO@TPU layer on a conducting Ag@TPU film to convert electrothermal input into mechanical response. Experiments are conducted to characterize the curvature of bilayer beams, which is then further analyzed using the Euler–Bernoulli beam theory. The beam curvature change, free transformation strain, and effective work density associated with the SCO are 0.11 mm−1, 1.6%, and 1.25 mJ cm−3, respectively. Further, the open‐ and closed‐loop response of the actuator is investigated using a custom‐built setup. The open‐loop identification suggests that the actuator gain increases monotonously when the control current increases. This natural adaptive character can explain the drastically diminished response time in closed‐loop proportional–integral–derivative control experiments (2–3 s). Finally, tracking experiments are carried out to evaluate the robustness of the actuator with and without payloads. The results for 30 240 endurance cycles reveal a mean positioning error of 0.8%.

Analytical intrinsic mechanical properties of piezoelectric ceramics under the saturated and unsaturated poling states

The purpose of this paper is to study the intrinsic mechanical contributions of poled piezoelectric ceramics under the three ferroelectric phases [tetragonal (4[Formula: see text]mm), rhombohedral (3[Formula: see text]m) and orthorhombic (mm2)]. The intrinsic elastic coefficients and spontaneous strains of saturated and unsaturated poling piezoelectric ceramics are analyzed and calculated by probability density functions of orientation (PDFOs) and Reuss or Voigt average, and the analytical results of the intrinsic mechanical properties of piezoelectric ceramics with the poling degree are obtained. In addition, this paper also calculates the Young’s modulus and shear modulus of barium titanate (BaTiO3) piezoelectric ceramics by PDFO which are based on the Reuss, Voigt and Hill averages. Comparing them with the published theoretical calculation data shows that the results calculated by the finite element method under the saturated and unsaturated poling states are within the range of the results calculated by us using the three average theories through PDFO, and it shows the accuracy of calculation by PDFO.

Ferroelastic tetragonal-monoclinic phase transition and anisotropic thermal expansion of LuNbO4 ceramics

Rare-earth tantalates (RETaO4) and niobates (RENbO4) are widely studied as promising thermal barrier coatings based on the ferroelastic tetragonal-monoclinic (t-m) phase transition. We studied the t-m transition process, anisotropic thermal expansion coefficients (TECs), and the corresponding spontaneous strain of LuNbO4 by powder high-temperature X-ray diffraction. The results proved that the unit cell volume and TECs continuously increased with increasing temperature, and the dominant mechanisms of thermal expansion were proposed. Two different orientation states (S1 and S2) caused by the t-m transition led to formation of the ferroelastic domains, and the corresponding spontaneous strain was determined. The relationship between the t-m transition and spontaneous strain was proposed for further property tailoring. This work provided an in-depth analysis of the ferroelastic t-m phase transition, and it would advance the applications of ferroelastic ceramics.

Lattice expansion and ferroelectricity of PbxSr1−xTiO3: a phenomenological study

Structural transition, tetragonality, and dielectric properties are investigated along with thermal and compositional expansion of lead strontium titanate in order to reveal composition dependence and structure-property relation of the ferroelectric structure. Based on the available structural and dielectric data, dielectric stiffness and temperature-dependent paraelectric cubic lattice parameters are analyzed. Non-zero sixth-order free energy coefficients are derived for strontium titanate. Spontaneous polarization, spontaneous strain, volumetric change, and dielectric permittivity are modeled as a function of composition, and the theoretical results are in agreement with experimental data reported in the literature and reveal solid solution effect.

Analysis of stress and strain concentration around a centralized elliptical hole in a monodomain liquid crystal elastomer sheet

Liquid crystal elastomers (LCEs) are a kind of soft materials which couple the high elastic deformability with the unique properties of liquid crystals. Such combination endows notched LCEs unusual stress and strain concentration behaviors, which is preliminary discussed by us in the case of a large sheet with a centralized circular hole. Here we extend our study from circular holes to more generalized, elliptical holes. We investigate the stress and strain fields around a centralized elliptical hole in a LCE sheet subjected to uniaxial stretches by finite element methods. The effects of the shape factor, defined as the ratio of the minor-to-major axis of the ellipse, are mainly concerned. Compared with common elastomers like neoHookean, LCEs get higher stress and strain concentration factors (SCFs), and the location of maximal strain deviates slightly from that of maximal stress. With the decrease of the shape factor (a sharper ellipse) the SCFs of LCEs rise much severer than those of neoHookean, and the deviation is diminishing. In addition, as the stretch increases, the region near the root is getting close to an approximately uniaxial stress state, and the high strain region will extend non-monotonously along the hole edge, which differs from a monotonous extension of the high stress region. All the unusual behaviors of LCEs above are attributed to the spontaneous strain induced by director rotation. Attempts to correlate stress and strain concentration behaviors to the spontaneous strain are made in this article.

Magnetoelastic coupling behaviour of nanocrystalline ε-Fe2O3

Preparation of a ceramic sample which preserved the nanoscale grain sizes of ∼10–30 nm has allowed elastic and anelastic properties of ε-Fe2O3 to be investigated as functions of temperature and magnetic field strength by Resonant Ultrasound Spectroscopy in the frequency range ∼0.1–1 MHz. Formal analysis of spontaneous strains, e, from previously obtained high resolution lattice parameter data confirmed that magnetic ordering below ∼500 K is accompanied by strains of up to ∼±0.002 due to coupling with the order parameter, m, according to λem2. However, this coupling does not result in elastic softening that would be expected if the order parameter relaxed in response to an induced strain on the timescale of the acoustic resonances. Stiffening or softening during heating through ∼450–480 K of the initial as prepared material, which acquired a distinct magnetisation parallel to the stress applied during Spark Plasma Sintering, is attributed to changes in magnetic domain configurations involving preferred local alignments of individual moments of monodomain crystals. The crystallographic space group, Pna21, and magnetic space group at room temperature, Pna'21', allow ε-Fe2O3 to be both piezoelectric and piezomagnetic. It is postulated that changes in the effective coefficients of these properties for bulk samples are responsible for the observed variations in acoustic resonance frequencies according to the magnetic domain structure present. No elastic or anelastic anomalies were observed at the commensurate-incommensurate transition near 110 K. Instead, acoustic resonance frequencies changed in response to an applied magnetic field, consistent with viscous motion of magnetic domain walls and the effect of poling on piezo coefficients. Ceramic samples of ε-Fe2O3 could have potentially functional piezoelectric and/or piezomagnetic properties that are tunable by choice of magnetic and thermal history.

Ferroelastic domain identification and toughening mechanism for yttrium tantalate–zirconium oxide

Yttrium tantalate (YTaO4) is the next generation of higher service temperature thermal barrier coatings (TBCs) materials due to its smaller volume effect in phase change, lower thermal conductivity and unique ferroelastic domain structure. However, the low fracture toughness limits its application. We first characterized the diffraction patterns of variants, and two variants (M1 and M2) observed in transmission electron microscopy (TEM) results were determined from four possible variants by mechanical derivation. The role of Zr4+ doping in ferroelastic toughening was explained in detail. With the increase of Zr4+ doping concentration, the monoclinic angle β and the domain rotation angle α decrease, respectively. The spontaneous strain component and the principal strain in the main space also have a similar decreasing trend. The decrease of the ferroelastic domain inversion energy barrier is beneficial to the improvement of fracture toughness. Combining the results of Vickers indentation, we found that Zr4+ could be enriched at the domain boundary to inhibit the generation of cracks. An appropriate amount of Zr4+ is conducive to the improvement of fracture toughness, and the excessive Zr4+ will reduce the fracture toughness due to the generation of by-product t-ZrO2. So, the optimal composition is Y0.44Ta0.44Zr0.12O2 and the best fracture toughness (2.9–3.8MPa m1/2) is equivalent to the commercial 8YSZ. This result will promote the application of a new generation of TBCs.

Entangled polarizations in ferroelectrics: A focused review of polar topologies

Ferroelectric crystals feature asymmetric or polar structures that are switchable under an external electric field, holding promise for information storage. Nanoscale ferroelectrics might exhibit various exotic domain configurations and polar topologies, such as full flux-closure, vortex, skyrmion, and meron. These topological domains were theoretically switchable and may give rise to an unusually high density of memory bits. They would also undergo unusual phase transitions and form hidden, collective polar topological states under external stimulations. Similar domains and spin topologies are well known in ferromagnetic materials, and their topological properties and dynamics are under intensive investigation. However, in ferroelectric materials, the coupling of polarizations to spontaneous strains would be so pronounced that the formations of polar topologies were believed to be impossible. How to stabilize the polar topologies in ferroelectrics, especially in nanoscale ferroelectrics, was known as a big challenge.In this overview, we summarize the recent progress in polar topologies in ferroelectric oxides. We start from a review the discovery of polar topologies, including flux-closure quadrant, vortex, bubble, skyrmion, meron lattice, polar waves, and center-type domains. We also focus on the effects of mechanical and electrical boundary conditions and sample size on the formation of topological structures. In the meanwhile, we emphasize the use of aberration-corrected transmission electron microscope which enables to visualize the ion displacement at a sub-Ångström resolution in real space. And at the end, we envision several aspects to be considered in the future, such as imaging three dimensional (3D) atomic morphology of the topological polar structures, exploring novel polar topologies in other possible systems, and addressing the coupling of polar topologies with flexoelectricity by a combination of quantitative transmission electron microscopy and relevant theoretical approaches.

Pressure Tuning of Coupled Structural and Spin State Transitions in the Molecular Complex [Fe(H2B(pz)2)2(phen)

The large volume change, which accompanies the molecular spin crossover (SCO) phenomenon in some transition metal complexes, prompts frequently the coupling of the SCO with other instabilities. Understanding the driving mechanism(s) of such coupled phase transitions is not only important for fundamental reasons but also provides scope for the development of multifunctional materials. The general theoretical expectation is that the coupling has elastic origin, and the sequence of transitions can be tuned by an externally applied pressure, but dedicated experiments remain scarce. Here, we used high-pressure and low-temperature single-crystal X-ray diffraction to investigate the high-spin (HS) to low-spin (LS) transitions in the molecular complexes [FeII(H2B(pz)2)2(bipy)] and [FeII(H2B(pz)2)2(phen)]. In the bipyridine complex, the SCO is continuous and isostructural over the whole T, P-range (100-300 K, 0-2 GPa). In the phenanthroline derivative, however, the SCO is concomitant with a symmetry-breaking transition (C2/c to P1̅). Structural analysis reveals that the coupling between the two phenomena can be tuned by external pressure from a virtually simultaneous HSC2/c-LSP1̅ transition to the sequence of HSC2/c-LSC2/c-LSP1̅ transitions. The correlation of spontaneous strain and order parameter behaviors highlights that the "separated" transitions remain still connected via strain coupling, whereas the "simultaneous" transitions are partially split.