Smart Materials Research Articles

Advances in Molecular Photoswitches: From Azobenzenes to Azoquinolines

Molecular photoswitches represent a dynamic and ever-growing research area based on the ability of molecules to convert (switch) between cis- (Z) and trans- (E) isomers. Azobenzenes are the most popular and widely employed Z-E photoswitchable molecules in the development of photoresponsive, multifunctional smart materials for various applications. The promising avenues in this field include molecular fine-tuning of azobenzene- based photoswitches and the creation of single or dual-functional probes. This short overview highlights recent advances in the design of molecular photoswitches, particularly the molecular design strategies of azobenzene-based photoswitches with their structural and electronic features. Particular attention is paid to azoquinolines, which seem to be a promising alternative to azobenzenes in the design of novel multifunctional photoswitches with improved photochromic properties. Here, we have also developed the novel star-shaped multiazoquinoline photoswitch comprising individual azoquinoline-based photochromes connected to a central trisubstituted 1,3,5-triformylphloroglucinol core by quantum chemical calculations. This unique structure is favorable for independent Z-E isomerization of each azoquinoline-based photochrome within one macromolecule.

Azobenzene-Functionalized Semicrystalline Liquid Crystal Elastomer Springs for Underwater Soft Robotic Actuators.

As actuated devices become smaller and more complex, there is a need for smart materials and structures that directly function as complete mechanical units without an external power supply. The strategy uses light-powered, twisted, and coiled azobenzene-functionalized semicrystalline liquid crystal elastomer (AC-LCE) springs. This twisting and coiling, which has previously been used for only thermally, electrochemically, or absorption-powered muscles, maximizes uniaxial and radial actuation. The specially designed photochemical muscles can undergo about 60% tensile stroke and provide 15kJ m-3 of work capacity in response to light, thus providing about three times and two times higher performance, respectively, than previous azobenzene actuators. Since this actuation is photochemical, driven by ultraviolet (UV) light and reversed by visible light, isothermal actuation can occur in a range of environmental conditions, including underwater. In addition, photoisomerization of the AC-LCEs enables unique latch-like actuation, eliminating the need for continuous energy application to maintain the stroke. Also, as the light-powered muscles processed to be either homochiral or heterochiral, the direction of actuation can be reversed. The presented approach highlights the novel capabilities of photochemical actuator materials that can be manipulated in untethered, isothermal, and wet environmental conditions, thus suggesting various potential applications, including underwater soft robotics.

Scalable Production of Functional Fibers with Nanoscale Features for Smart Textiles.

Functional fibers, retaining nanoscale characteristics or nanomaterial properties, represent a significant advance in nanotechnology. Notably, the combination of scalable manufacturing with cutting-edge nanotechnology further expands their utility across numerous disciplines. Manufacturing kilometer-scale functional fibers with nanoscale properties are critical to the evolution of smart textiles, wearable electronics, and beyond. This review discusses their design principles, manufacturing technologies, and key advancements in the mass production of such fibers. In addition, it summarizes the current applications and state of progress in scalable fiber technologies and provides guidance for future advances in multifunctional smart textiles, by highlighting the upcoming impending demands for evolving nanotechnology. Challenges and directions requiring sustained effort are also discussed, including material selection, device design, large-scale manufacturing, and multifunctional integration. With advances in functional fibers and nanotechnology in large-scale production, wearable electronics, and smart textiles could potentially enhance human-machine interaction and healthcare applications.

Second Generation Zwitterionic Aza‐Diarylethene: Photoreversible CN Bond Formation, Three‐State Photoswitching, Thermal Energy Release, and Facile Photoinitiation of Polymerization

Diarylethenes are a well‐studied and optimized class of photoswitches with a wide range of applications, including data storage, smart materials, or photocontrolled catalysis and biological processes. Most recently, aza‐diarylethenes have been developed in which carbon‐carbon bond connections are replaced by carbon‐nitrogen connections. This structural elaboration opens an entire new structure and property space expanding versatility and applicability of diarylethenes. In this work, we present the second generation of zwitterionic aza‐diarylethenes, which finally allows for fully reversible photoswitching and precise control over all three switching states. High‐yielding photoswitching between the neutral open form and a zwitterionic Z isomer is achieved with two different wavelengths of light. The third zwitterionic E isomeric state can be reached up to 87% upon irradiation with a third wavelength. Its high energy content of >10 kcal/mol can be released thermally by deliberate solvent change as trigger mechanism, rendering aza‐diarylethenes into interesting candidates for molecular solar thermal energy storage (MOST) applications. The third state further serves as locking state, allowing to toggle light‐responsiveness reversibly between thermally labile and thermally stable switching. Further, irradiation of the zwitterionic states leads to highly efficient photopolymerization of methyl acrylate (MA), directly harnessing the unleashed chemical reactivity of aza‐diarylethene in materials applications.

Second Generation Zwitterionic Aza-Diarylethene: Photoreversible CN Bond Formation, Three-State Photoswitching, Thermal Energy Release, and Facile Photoinitiation of Polymerization.

Diarylethenes are a well-studied and optimized class of photoswitches with a wide range of applications, including data storage, smart materials, or photocontrolled catalysis and biological processes. Most recently, aza-diarylethenes have been developed in which carbon-carbon bond connections are replaced by carbon-nitrogen connections. This structural elaboration opens an entire new structure and property space expanding versatility and applicability of diarylethenes. In this work, we present the second generation of zwitterionic aza-diarylethenes, which finally allows for fully reversible photoswitching and precise control over all three switching states. High-yielding photoswitching between the neutral open form and a zwitterionicZisomer is achieved with two different wavelengths of light. The third zwitterionicEisomeric state can be reached up to 87% upon irradiation with a third wavelength. Its high energy content of >10 kcal/mol can be released thermally by deliberate solvent change as trigger mechanism, rendering aza-diarylethenes into interesting candidates for molecular solar thermal energystorage (MOST) applications. The third state further serves as locking state, allowing to toggle light-responsiveness reversibly between thermally labile and thermally stable switching. Further, irradiation of the zwitterionic states leads to highly efficient photopolymerization of methyl acrylate (MA),directly harnessing the unleashed chemical reactivity of aza-diarylethene in materials applications.

Effect of carbon fibers modification on joint adhesion steel-epoxy resin-aluminum

The combination of high-performance steel with aluminum or aluminum alloys shows a wide range of application in high technologies field like aerospace, smart materials, etc. The problem in using of adhesive bonding technology for these substrates is the weak mechanical occlusion between steel/aluminum and common coatings. In this study, different methods of treatment of carbon fiber were employed to enhance the adhesion strength in steel-epoxy resin filled with carbon fiber-aluminum triplex. The treatment of carbon fibers with 3-glicidyloxypropyl-trimetoxysilane after their oxidation in 65 wt.% nitric acid leads to the additives which improve the adhesion strength of epoxy resins at 15 wt.% contain on 67.5% in comparison with neat epoxy up to 20 MPa. This result can be explained by the change of failure mechanism from “cohesive’ to “adhesive” that leads to an increase of adhesion strength to steel and aluminum. The SEM study shown that 60–80 nm thick two-layer interphase formed between carbon fiber and epoxy matrix. The mechanical strength of this interphase governs the mechanical and adhesion performance of steel-epoxy resin-aluminum triplex. Taking into account the mechanical properties and adhesive strength of these composites, it emerges as a potential candidate for advanced materials.

Performance analysis of vertical smart isolator based on magnetorheological elastomer

ABSTRACT As one of the field-dependent smart materials whose stiffness and damping properties can change instantaneously and reversibly, magnetorheological elastomer (MRE) has been extensively utilized on base isolation for vibration reduction. However, most previous studies have focused on the shear dynamic performance of MRE isolators, and there are few reports on the vertical extrusion performance of basic isolators within construction equipment. In this paper, MRE materials with strong bearing capacity and suitable vertical stiffness were fabricated by comprehensively considering the selection of raw materials, particle ratio, and sample size. The tension-compression viscoelasticity of the prepared MRE under varying magnetic fields and strain amplitudes was experimentally evaluated using an MRE axial MR testing system. Eventually, a single-degree-of-freedom dynamic test rig for vibration isolation of equipment in buildings, which integrates a vertical isolator with MRE as the core component, was constructed to perform a series of experimental investigations on the alterable frequency vibration capability of the designed MRE vertical isolator. The test results reveal that the controllable stiffness-damping properties of the prepared MRE in the axial tension-compression mode can enable the developed vertical isolator to exhibit superior frequency shifting and vibration attenuating characteristics in structural vibration.

Smart Green Cotton Textiles with Hierarchically Responsive Conductive Network for Personal Healthcare and Thermal Management.

Whereas cotton as an abundant natural cellulose has been widely used for sustainable and skin-friendly textiles and clothes, developing cotton fabrics with smart functions that could respond to various stimuli is still eagerly desired while remaining a great challenge. Herein, smart multiresponsive cotton fabric with hierarchically copper nanowire interwoven MXene conductive networks that are seamlessly assembled along a 3D woven fabric template for efficient personal healthcare and thermal comfort regulation is successfully developed. The robust hierarchically interwoven conductive network was "glued" and protected by organic conductive polymer poly(3,4-ethylenedioxythiophene) along a 3D interconnected fabric template to enhance interfacial adherent and environmental stability. Benefiting from the robust multiresponsive hierarchically interwoven conductive network, smart cotton fabric exhibits real-time response to various external stimuli (light/electrical/heat/temperature/stress), and the details of human activities can be accurately recognized and monitored. Furthermore, the porous structure of 3D smart fabric induced strong capillary force and confinement to phase change materials PEG, which exhibits a wide range of phase transition temperatures for efficient thermal comfort regulation. After further encapsulation with transparent fluorosilicone resin, the smart cotton fabric exhibits excellent self-cleaning performance with water/oil repellent. The smart multiresponsive cotton fabrics hold great promise in next-generation wearable systems for efficient personal healthcare and thermal management.

Utilization of Tea Polyphenols as Color Developers in Reversible Thermochromic Dyes for Thermosensitive Color Change and Enhanced Functionality of Polyester Fabrics

Thermochromic textiles possess the capability to indicate ambient temperature through color changes, enabling real-time temperature monitoring and providing temperature warnings for body heat management. In this study, three thermochromic dyes—blue, red, and yellow—were synthesized using crystalline violet lactone (CVL), 6′-(diethylamino)-1′,3′-dimethyl-fluoran (DDF), and 3′,6′-dimethoxyfluoran (DOF) as leuco dyes, respectively, with biomass tea polyphenol serving as the color developer and tetradecanol as the phase change material. The chemical structures of these dyes were characterized using UV spectroscopy, infrared spectroscopy, Raman spectroscopy and 1H NMR. The thermochromic mechanisms were investigated, revealing that the binding bonds between the leuco dyes and the color developer broke and reorganized with temperature changes, imparting reversible thermochromic property. Polyester fabrics were dyed using an impregnation method to produce three reversible thermochromic fabrics in blue, red, and yellow. The structure and properties of these fabrics were analyzed, showing a significant increase in the UPF value from 26.3 to approximately 100, indicating enhanced UV resistance. Water contact angle measurements revealed that the contact angle of undyed polyester fabrics was 139°, while that of dyed polyester fabrics decreased by about 40°, indicating improved hydrophilicity. Additionally, the fabric inductive static tester showed that the static voltage half-life of dyed polyester fabric was less than 1 s, demonstrating a significant antistatic effect. Infrared thermal imaging results indicated that during the warming and cooling process, the thermochromic polyester fabric exhibited specific energy storage and insulation effects at 38 °C, close to the human body temperature. This study presented a novel approach to developing smart color-changing textiles using biomass-derived thermochromic dyes, offering diverse materials for personal thermal management, and intelligent insulation applications.

Recycling primary batteries into advanced graphene flake-based multifunctional smart textiles for energy storage, strain sensing, electromagnetic interference shielding, antibacterial, and deicing applications

Batteries are extensively used owing to their pivotal role in energy storage. However, their adverse environmental impact remains a significant challenge. The prevailing technologies for treating and handling battery waste are remarkably complex and expensive, highlighting the urgent need to upcycle spent battery materials into valuable resources to mitigate their environmental footprint. To that end, this paper reports a scheme for recycling graphite rods and Zn from Zn–C batteries. In this approach, polymeric composites synthesized using graphene flakes extracted from the graphite rods of spent batteries are used to fabricate multifunctional cotton textiles, and the outer Zn case of the spent batteries is employed as a Zn anode in energy storage devices. The synthesized multifunctional fabric shows excellent energy storage performance, particularly in Zn-ion hybrid supercapacitors, achieving a specific capacitance of 140 F g−1 at a scan rate of 0.5 A g−1; an electromagnetic interference shielding efficiency of ∼48 dB; wearable sensing capabilities for human motion detection; and Joule heating behavior for deicing. Moreover, the fabric exhibits remarkable antibacterial efficiency, with an approximately 27-mm-wide inhibition zone against both Gram-positive and Gram-negative bacteria. The “waste-to-wonder” strategy presented herein holds promise for environmental protection and innovative multifunctional textile fabrication.

True pinch mode of magnetorheological fluids

Abstract Magnetorheological (MR) fluids are representatives of smart materials. They react to magnetic fields by developing a yield stress. The effect has been employed in real-world applications such as automotive chassis systems or optical finishing. By convention, MR devices can be operated in at least one of the fundamental modes: flow, shear, squeeze, gradient pinch of which the former has been the least studied and understood. In pinch mode, the material in the flow channel is exposed to non-uniform magnetic fields in the direction parallel to fluid flow. As a result, only the volume of MR fluid near the channel walls are energized to modify the particular material property (yield stress). The result is the channel’s effective diameter change. The behavior of the material in pinch mode is unique and unseen in the other controllable fluids. To study the material’s characteristics in the specific mode, the authors developed a novel circuit concept for energizing the material in an effort to achieve the ’true-zero’ pinch mode magnetic behavior. Contrary to the existing pinch mode valve concepts, the concept valve allows to achieve zero magnetic flux density in the center of the flow channel regardless of the current level. To test the hypothesis a prototype valve was modeled, manufactured and tested across a range of external (flow rate, current/magnetic flux) stimuli. The obtained results yield sufficient evidence proven by results of magnetic simulations to support the underlying hypothesis. The experimental results illustrate the pinch mode type behaviour, i.e. the slope change in the pressure vs flow rate characteristics.

Enhancement of Curie Temperature and Photoluminescent Properties of Ho1.98Sm0.02Sn2O7 and Ho1.90Er0.10Sn2O7 Smart Materials

Enhancement of Curie Temperature and Photoluminescent Properties of Ho1.98Sm0.02Sn2O7 and Ho1.90Er0.10Sn2O7 Smart Materials

Polyaniline‐Doped Textile‐Based Triboelectric Nanogenerator: Self‐Powered Device for Wearable Electronics

ABSTRACTThe emergence of wearable electronics in contemporary lifestyles has spurred the need for smart fabrics capable of harnessing biomechanical energy. In the present study, a flexible polyaniline‐doped textile‐based triboelectric nanogenerator (PT‐TENG) is designed to harvest low‐frequency mechanical vibrations and convert them into electricity. For the device fabrication, five different textile fabrics are doped with conducting PANI, which is utilized as the tribopositive material, PVC thin film as the tribonegative material, and Al foil as electrodes. The PT‐TENG works in vertical‐contact separation mode, devised in arch structure for easy and complete contact between the working layers. Interestingly, the device featuring a PANI‐doped silk fabric generated the highest output voltage of 257.68 V and a current of 5.36 μA, respectively. Additionally, the PT‐TENG exhibits mechanical durability and electrical stability during continuous 7000 cyclic operations. Furthermore, the PT‐TENG showcases practical applications such as charging commercial capacitors, powering green LEDs and smartwatches, and as a self‐powered touch sensor. Thus, the PT‐TENG offers a facile fabrication process and robustness, highlighting its potential for sustainable energy harvesting in wearable electronics.

Dynamically customizable 4D printed shape memory polymer biomedical devices: a review

Abstract There is an increased risk of complications and even surgical failures for various types of medical devices due to difficult to control configurations and performances, incomplete deployments, etc. Shape memory polymers (SMPs)-based 4D printing technology offers the opportunity to create dynamic, personalized, and accurately controllable biomedical devices with complex configurations. SMPs, typical representatives of intelligent materials, are capable of programmable deformation in response to stimuli and dynamic remodeling on demand. 4D printed SMP medical devices not only enable active control of configuration, performance and functionality, but also open the way for minimally invasive treatments and remote controllable deployment. Here, the shape memory mechanism, actuation methods, and printing strategies of active programmable SMPs are reviewed, and cutting-edge advances of 4D printed SMPs in the fields such as bone scaffolds, tracheal stents, cardiovascular stents, cell morphological regulation, and drug delivery are highlighted. In addition, promising and meaningful future research directions for 4D printed SMP biomedical devices are discussed. The development of 4D printed SMP medical devices is inseparable from the in-depth cooperation between doctors and engineers. The application of 4D printed SMP medical devices will facilitate the rapid realization of "smart medical care" and accelerate the process of "intelligentization" of medical devices.

Exploring Students Awareness, Access and Utilization of Artificial Intelligence (AI) in Architectural Design

Artificial intelligence has become a trending topic in the last decade and has permeated all spheres of life and profession and Architecture is no exception. The use of artificial intelligence in architecture is still in its infancy as more research is still being carried out in the application of artificial intelligence in architecture to solve problems ranging from intelligent material design to architectural plan solutions. This study aimed to examine students’ levels of awareness, access, and use of artificial intelligence in architectural design at selected tertiary institutions in Southeast Nigeria. The three tertiary institutions selected are; The Department of Architectural Technology, Akanu Ibiam Federal Polytechnic Unwana, The Department of Architectural Technology Abia State Polytechnic, Aba and The Department of Architecture, Abia State University, Uturu. The main objective is to carry out a survey to investigate the awareness, access, and utilization of artificial intelligence (AI) in architectural design among students in selected tertiary institutions in Southeast Nigeria. This study adopted a descriptive research design of the survey method and employed a three-sectioned questionnaire to elicit information from the respondents. The sample size included a multistage sample of 300 undergraduates across three tertiary institutions in Ebonyi State and Abia State. The findings of the study were that the majority of the students are not aware of artificial intelligence and will use AI if they are aware of it and have access to it for their architectural design. Therefore, there is a need for integrating AI-related courses and workshops into the Architectural curriculum which can lead to better-prepared graduates who are proficient in using advanced design tools, potentially increasing their employability and innovation in the field. This study concluded that students' ability to explore digital resources such as AI for Architectural design is dependent on their awareness and access to digital technologies. A lack of these will result in a lack of use and lack of skill to use them.

Optimising Nanoparticle Dispersion Time for Enhanced Thermomechanical Properties in DGEBA-Based Shape Memory Polymer Composites

Shape-memory polymers (SMPs) are smart materials that can change shape upon an external stimulus. This phenomenon is called the shape memory effect (SME), which is caused by entropy change due to rapid molecular motion in the polymer segments. Due to the inherently weak thermomechanical properties, use of SMPs is limited in many engineering applications. Therefore, SMPs are often reinforced with fibres and nanoparticles (NPs). NPs offered greater flexibility due to their superior physical, chemical, electrical, mechanical, and thermal properties. However, the homogeneous distribution of NPs is crucial for composition’s stability and enhancement of the base material’s properties. Among the different techniques used for dispersing NPs, ultrasonic irradiation has shown excellent emulsifying and crushing performance. The sonication process is essential for mitigating agglomerates; however, prolonged sonication time probably increases epoxy temperature, micro-bubbles, cavitation, breaking apart molecules and finally degrading the epoxy resin performances. This paper provides critical insight of nanoparticle dispersion into diglycidyl ether of bisphenol A epoxies (DGEBA). DGEBA epoxy resin was added to TiO2 NPs and sonicated for 60 min with 5 min intervals while the temperature of epoxy was maintained below 60oC by using a water cooling throughout the sonication process. The process parameters such as amplitude, mode, epoxy volume and the weight percentage of NPs were kept constant. After each sonication step, Fourier-transform infrared spectroscopy (FTIR) was performed using Thermo Scientific™ and analysed through OMNIC™ Professional quantitation software. In accordance with FTIR results, until 30 min of the sonication, DGEBA resin was not degraded. In order to confirm the performances and the reinforcing effect of NPs, thermo-mechanical and shape memory properties were compared with the neat specimen. The outcomes of this research have suggested quick guidance to find optimum NP dispersion time for DGEBA resins, which has been hardly studied before.

Hydrogels Innovation: A Review on Recent Development, Characterization, and Applications

Hydrogels are special materials that can hold a large amount of water and form 3D networks. In the past few years, there have been exciting improvements in hydrogel technology, bringing new ideas to many different areas. By trying out new materials like smart hydrogels that can respond to different conditions, provided new ways to deliver medicine precisely, build tissues, and create wearable gadgets. Among the most significant developments is the creation of smart hydrogels, which can react dynamically to different environmental stimuli. With their ability to release therapeutic chemicals under regulated conditions in response to particular physiological cues, these intelligent materials have enormous potential for the administration of precision medicine. These kinds of customized drug delivery systems have the power to completely change how treatments are administered by reducing adverse effects and increasing therapeutic efficacy. Hydrogels are also useful in tissue engineering, where they are used as scaffolds to create biological tissues that function. Hydrogel-based tissue constructions, which imitate the extracellular matrix, offer a favorable microenvironment for cell proliferation and differentiation, promoting the healing of injured or ill tissues. With its enormous potential in regenerative medicine, this revolutionary strategy offers hope for the treatment of ailments including organ failure. this article gives a thorough look at the recent developments in hydrogels, characterization techniques, and the new application of hydrogels in various fields of science. In summary, new developments in hydrogel technology have opened up a plethora of opportunities in a variety of scientific fields. The adaptable properties of hydrogels continue to spur innovation in a variety of fields, including wearable technology, tissue engineering, and precision medicine. These applications offer revolutionary answers to urgent social issues.

Valorization of nopal wastes to produce quantum dots: optimizing synthesis and exploring in smart textile applications

Quantum carbon dots (QCDs) were efficiently synthesized from post-extraction residues generated during nopal fabric production using a hydrothermal treatment. These QCDs were applied to nopal fabrics, enhancing their UV solar radiation absorption. The synthesized QCDs exhibited fluorescence emissions in the 200–300 nm range. An eco-friendly dispersion was created by incorporating QCDs into TiO2 for use in smart textiles, which underlines our commitment to maintaining a sustainable process. Bright and fluorescent patterns were successfully applied to commercial and nopal fabrics using a spray printing technique. Additionally, the QCDs demonstrated pH-sensitive color changes, paving the way for practical applications. This work represents an initial step towards a circular economy by utilizing residues from nopal fabric production to synthesize quantum dots, which may be employed in smart textiles applications with UV absorption capabilities.

Improved barrier, mechanical and antioxidant properties of pH-responsive film by incorporating dialdehyde starch and anthocyanins into rice protein/sodium alginate

This study aimed to develop rice protein/sodium alginate (RP/SA) pH-responsive films with enhanced properties by incorporating dialdehyde starch (DAS) and Lycium ruthenicum anthocyanins (LRA) and the film was applied to monitor the fruit freshness. The effect of the DAS and LRA content on the morphology, mechanical, water barrier, oxygen barrier, ultraviolet-blocking and thermal stability properties of RP/SA-based films was investigated. The best water vapor permeability of the film was 3.33 g·mm/(m2·d·kPa) with 10 % DAS. With increasing the DAS content from 0 % to 20 %, the tensile strength of the film was increased by 66.3 % compared with that of the film without DAS, while the thermal stability, oxygen barrier and ultraviolet light barrier properties were significantly enhanced. These results may be due to the formation of a compact structure observed by scanning electron microscopy, and stronger hydrogen bonding interactions and lower binding energy in the RP/SA/DAS/LRA system obtained by Fourier transform infrared spectroscopy, X-ray diffraction and molecular dynamics simulation. The RP/SA/DAS10/LRA5 film had 51.6 times higher antioxidant property than the film without LRA and exhibited significant color variations with changes in fresh-cut cantaloupe quality. The developed RP/SA-based films with improved properties are potential intelligent food packaging materials.

Au···I coinage bonds: Boosting photoluminescence efficiency and solid‐state molecular motion

AbstractCoinage bonds, a type of noncovalent interaction, occur between group 11 elements (Au, Ag, and Cu) with electron donor groups. Despite theoretical validation, empirical evidence remains limited. In this study, an aggregation‐induced emission (AIE)‐active Au(I) complex, ITCPAu, which exhibits Au···I coinage bonds, was revealed based on the single‐crystal X‐ray diffraction and theoretical calculations. Further examination of the luminescence properties of the ITCPAu revealed multiswitchable behavior, including mechanochromism and thermochromism. Nearly pure white‐light emission was achieved with Commission Internationale de L'Eclairage (CIE) 1931 chromaticity coordinates of (0.30, 0.31) by grinding the green‐emissive ITCPAu monomer crystals. Moreover, visualization and manipulation of solid‐state molecular motion (SSMM) in the yellow‐emissive ITCPAu dimer crystals, driven by the robust Au···I coinage bonds, were revealed through a combination of crystal engineering and luminescent properties. Furthermore, to support the robust Au···I coinage bonds, a versatile carrier for small solvent molecules in crystal lattices was developed for uptake and release. Our findings provide experimental and theoretical evidence for Au···I coinage bonds, highlighting their ability to boost photoluminescence quantum yield (PLQY) and trigger SSMM, emphasizing their potential in developing smart materials with stimuli‐responsive properties.