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Chemiluminescence, a process of transduction of energy stored within chemical bonds of ground-state reactants into light via high-energy excited intermediates, is known in solution, but has remained undetected in macroscopic crystalline solids. By detecting thermally induced chemiluminescence from centimeter-size crystals of an organic peroxide here we demonstrate direct transduction of heat into light by thermochemiluminescence of bulk crystals. Heating of crystals of lophine hydroperoxide to ~115 °C results in detectable emission of blue-green light with maximum at 530 nm with low chemiluminescent quantum yield [(2.1 ± 0.1) × 10 ‒7  E mol ‒1 ]. Spectral comparison of the thermochemiluminescence in the solid state and in solution revealed that the solid-state thermochemiluminescence of lophine peroxide is due to emission from deprotonated lophine. With selected 1,2-dioxetane, endoperoxide and aroyl peroxide we also establish that the thermochemiluminescence is common for crystalline peroxides, with the color of the emitted light varying from blue to green to red. Chemiluminescence is known in solution, but has remained undetected in macroscopic crystalline solids so far. Here the authors demonstrate direct transduction of heat into light by thermochemiluminescence in a centimeter-size lophine hydroperoxide crystal.

Molecular crystals can be bent elastically by expansion or plastically by delamination into slabs that glide along slip planes. Here we report that upon bending, terephthalic acid crystals can undergo a mechanically induced phase transition without delamination and their overall crystal integrity is retained. Such plastically bent crystals act as bimorphs and their phase uniformity can be recovered thermally by taking the crystal over the phase transition temperature. This recovers the original straight shape and the crystal can be bent by a reverse thermal treatment, resulting in shape memory effects akin of those observed with some metal alloys and polymers. We anticipate that similar memory and restorative effects are common for other molecular crystals having metastable polymorphs. The results demonstrate the advantage of using intermolecular interactions to accomplish mechanically adaptive properties with organic solids that bridge the gap between mesophasic and inorganic materials in the materials property space. Molecular crystals can be bent elastically by expansion or contraction on opposite faces, or plastically by delamination into slabs that glide along slip planes. Here the authors report crystals that can be bent plastically while undergoing a mechanically induced phase transition without delamination.

Organic crystals are emerging as mechanically compliant, light-weight and chemically versatile alternatives to the commonly used silica and polymer waveguides. However, the previously reported organic crystals were shown to be able to transmit visible light, whereas actual implementation in telecommunication devices requires transparency in the near-infrared spectral range. Here we demonstrate that single crystals of the amino acid L-threonine could be used as optical waveguides and filters with high mechanical and thermal robustness for transduction of signals in the telecommunications range. On their (00 1 ¯ ) face, crystals of this material have an extraordinarily high Young’s modulus (40.95 ± 1.03 GPa) and hardness (1.98 ± 0.11 GPa) for an organic crystal. First-principles density functional theory calculations, used in conjunction with analysis of the energy frameworks to correlate the structure with the anisotropy in the Young’s modulus, showed that the high stiffness arises as a consequence of the strong charge-assisted hydrogen bonds between the zwitterions. The crystals have low optical loss in the O, E, S and C bands of the spectrum (1250−1600 nm), while they effectively block infrared light below 1200 nm. This property favors these and possibly other related organic crystals as all-organic fiber-optic waveguides and filters for transduction of information. Fiber-optics based on organic crystals could have potential for unique telecommunications applications but typically transmit visible wavelengths. Here the authors present mechanically robust organic crystals with favourable optical properties across the main telecommunication bands in the near-infrared.

Dynamic organic crystals are rapidly gaining traction as a new class of smart materials for energy conversion, however, they are only capable of very small strokes (<12%) and most of them operate through energetically cost-prohibitive processes at high temperatures. We report on the exceptional performance of an organic actuating material with exceedingly large stroke that can reversibly convert energy into work around room temperature. When transitioning at 295–305 K on heating and at 265–275 K on cooling the ferroelectric crystals of guanidinium nitrate exert a linear stroke of 51%, the highest value observed with a reversible operation of an organic single crystal actuator. Their maximum force density is higher than electric cylinders, ceramic piezoactuators, and electrostatic actuators, and their work capacity is close to that of thermal actuators. This work demonstrates the hitherto untapped potential of ionic organic crystals for applications such as light-weight capacitors, dielectrics, ferroelectric tunnel junctions, and thermistors. Organic electronics requires dynamic materials, however, most of them have small strokes and operate at high temperatures. Here, the authors describe organic crystal that repeatedly expands and contracts nearly half its length around room temperature.

The growing freshwater scarcity has caused increased use of membrane desalination of seawater as a relatively sustainable technology that promises to provide long-term solution for the increasingly water-stressed world. However, the currently used membranes for desalination on an industrial scale are inevitably prone to fouling that results in decreased flux and necessity for periodic chemical cleaning, and incur unacceptably high energy cost while also leaving an environmental footprint with unforeseeable long-term consequences. This extant problem requires an immediate shift to smart separation approaches with self-cleaning capability for enhanced efficiency and prolonged operational lifetime. Here, we describe a conceptually innovative approach to the design of smart membranes where a dynamic functionality is added to the surface layer of otherwise static membranes by incorporating stimuli-responsive organic crystals. We demonstrate a gating effect in the resulting smart dynamic membranes, whereby mechanical instability caused by rapid mechanical response of the crystals to heating slightly above room temperature activates the membrane and effectively removes the foulants, thereby increasing the mass transfer and extending its operational lifetime. The approach proposed here sets a platform for the development of a variety of energy-efficient hybrid membranes for water desalination and other separation processes that are devoid of fouling issues and circumvents the necessity of chemical cleaning operations. The performance of membrane desalination of seawater is hampered by fouling. Here the authors develop smart gating hybrid membranes by surface coating with polymer-embedded thermosalient crystals. These membranes enhance pure water flux by over 40% in saltwater desalination by osmotic distillation.

The realm of self-healing materials integrates chemical and physical mechanisms that prevent wear and fracturing and extend the operational lifetime. Unlike the favorable rheology of amorphous soft materials that facilitates efficient contact between fragments, the efficiency of recovery of atomistically ordered materials is restricted by slower interfacial mass transport and the need for ideal physical alignment, which limits their real-world application. We report drastic enhancements in efficiency and recovery time in the self-healing of anilinium bromide, challenging these limitations. Crystals of this material recovered up to 49% within seconds and up to 95% after 100 min via ferroelastic detwinning. The spatial evolution of strain during cracking and healing was measured in real time using digital image correlation. Favorable alignment and strong ionic bonding across the interface of partially fractured crystals facilitate self-healing. This study elevates organic crystals close to the best-in-class self-healing polymers and sets an approach for durable crystal-based optoelectronics. Self-healing in structurally ordered materials is restricted by slow interfacial mass transport and the need for ideal physical alignment. Here the authors show self-healing in an anilinium bromide crystals achieving up to 95% recovery through ferroelastic detwinning.

Although a plethora of metal complexes have been characterized, those having multifunctional properties are very rare. This article reports three isotypical complexes, namely [Cu(benzoate) L 2 ], where L = 4-styrylpyridine (4spy) ( 1 ), 2′-fluoro-4-styrylpyridine (2F-4spy) ( 2 ) and 3′-fluoro-4-styrylpyridine (3F-4spy) ( 3 ), which show photosalient behavior (photoinduced crystal mobility) while they undergo [2+2] cycloaddition. These crystals also exhibit anisotropic thermal expansion when heated from room temperature to 200°C. The overall thermal expansion of the crystals is impressive, with the largest volumetric thermal expansion coefficients for 1 , 2 and 3 of 241.8, 233.1 and 285.7 × 10 −6  K −1 , respectively, values that are comparable to only a handful of other reported materials known to undergo colossal thermal expansion. As a result of the expansion, their single crystals occasionally move by rolling. Altogether, these materials exhibit unusual and hitherto untapped solid-state properties.