Programmable Engineering of Sunlight-Fueled, Full-Wavelength-Tunable, and Chirality-Invertible Helical Superstructures.

Dynamic control of motion at the molecular level is a core issue in promoting the bottom-up programmable modulation of sophisticated self-organized superstructures. Self-assembled artificial nanoarchitectures through subtle noncovalent interactions are indispensable for diverse applications. Here, the active solar renewable energy is used to harness cholesteric liquid crystal (CLC) superstructure devices via delicate control of the dynamic equilibrium between the concentrations of molecular motor molecules with opposite handedness. Thus, the spectral position and handedness of a photonic superstructure can be tuned continuously, bidirectionally, and reversibly within the entire working spectrum (from near-ultraviolet to the thermal infrared region, over 2 µm). With these unique horizons, three advanced photoresponsive chiroptical devices, namely, a mirrorless laser, an optical vortex generator, and an encrypted contactless photorewritable board, are successfully demonstrated. The sunlight-fueled chirality inversion prompts facile switching of functionalities, such as free-space optical communication, stereoscopic display technology, and spin-to-orbital angular momentum conversion. Motor-based chiroptic devices with dynamic and versatility controllability, fast response, ecofriendly characteristics, stability, and high efficiency have potential to replace the traditional elements with static functions. The inexhaustible natural power provides a promising means for outdoor-use optics and nanophotonics.

Control of Large-Area Orderliness of a 2D Supramolecular Chiral Microstructure by a 1D Interference Field.

Self-organized periodic micro/nanostructures caused by stimulus-responsive structural deformation often occur in anisotropic self-assembled supramolecular systems (e.g., liquid crystal systems). However, the long-range orderliness of these structures is often beyond control. In this article, we first demonstrate that a large-area disordered two-dimensional (2D) microgrid chiral structure appears in the cholesteric liquid crystal (CLC) reactive mixture because of the photopolymerization-induced Helfrich deformation effect under exposure to the single UV-laser beam. The result is attributed to the impact of an internal longitudinal strain, which is caused by the pitch contraction of the CLC-monomer region through the continuing compression of the thickening CLC polymer layer adhered on the illuminated substrate of the sample during photopolymerization. The experimental results further show that a one-dimensional (1D) UV-laser interference field can be used to effectively control the postformed 2D microgrid structure to arrange in an orderly manner throughout the large exposed area (an order of centimeter). The optimum ability for controlling the orderliness of the microgrid structure can be achieved if the spacing width of the interference field approximates the periodicity of the postformed 2D microgrids. Several factors, such as the pitch of the CLC mixture and the included angle and intensity of the two interfering laser beams, which influence the orderliness and properties of the 2D microgrid structure, are explored in this study. The result of this research opens a new page to improve the applicability of the Helfrich deformation phenomenon and further provides a reference platform for manipulating, modifying, and even tailoring periodic micro/nanostructures in self-organized supramolecular soft-matter systems for application in advanced optics/photonics.

Wavelength-Tunable and Highly Stable Perovskite-Quantum-Dot-Doped Lasers with Liquid Crystal Lasing Cavities.

This study applies a low-cost solvothermal method to synthesize all-inorganic (lead-free cesium tin halide) perovskite quantum dots (AIPQDs) and to fabricate AIPQD-doped lasers with cholesteric liquid crystal (CLC) lasing cavities. The lasers present highly qualified lasing features of low threshold (150 nJ/pulse) and narrow line width (0.20 nm) that are attributed to the conjunction of the suppression of photoluminescence (PL) loss caused by the quantum confinement of AIPQDs and the amplification of PL caused by the band-edge effect of the CLC-distributed feedback resonator. In addition, the lasers possess highly flexible lasing-wavelength tuning features and a long-term stability under storage at room temperature and under high humidity given the protective role of CLC. These advantages are difficult to confer to typical light-emitting perovskite devices. Given these merits, the AIPQD-doped CLC laser device has considerable potential applications in optoelectronic and photonic devices, including lighting, displays, and lasers.

Wide-Band Spatially Tunable Photonic Bandgap in Visible Spectral Range and Laser based on a Polymer Stabilized Blue Phase.

This work successfully develops a largely-gradient-pitched polymer-stabilized blue phase (PSBP) photonic bandgap (PBG) device with a wide-band spatial tunability in nearly entire visible region within a wide blue phase (BP) temperature range including room temperature. The device is fabricated based on the reverse diffusion of two injected BP-monomer mixtures with a low and a high chiral concentrations and afterwards through UV-curing. This gradient-pitched PSBP can show a rainbow-like reflection appearance in which the peak wavelength of the PBG can be spatially tuned from the blue to the red regions at room temperature. The total tuning spectral range for the cell is as broad as 165 nm and covers almost the entire visible region. Based on the gradient-pitched PSBP, a spatially tunable laser is also demonstrated in this work. The temperature sensitivity of the lasing wavelength for the laser is negatively linear and approximately -0.26 nm/°C. The two devices have a great potential for use in applications of photonic devices and displays because of their multiple advantages, such as wide-band tunability, wide operated temperature range, high stability and reliability, no issue of hysteresis, no need of external controlling sources, and not slow tuning speed (mechanically).

Performance evolution of color cone lasing emissions in dye-doped cholesteric liquid crystals at different fabrication conditions.

This work investigates the performance evolution of color cone lasing emissions (CCLEs) based on dye-doped cholesteric liquid crystal (DDCLC) cells at different fabrication conditions. Experimental results show that the energy threshold (E(th)) and relative slope efficiency (η(s)) of the lasing signal emitted at each cone angle (0°-35°) in the CCLE decreases and increases, respectively, when the waiting time in a homogenously rubbed aligned DDCLC cell is increased from 0 hr to 216 hr (9 days). This result occurs because defect lines gradually shrink with the anchoring of the surface alignment when the waiting time is increased. Hence, the scattering loss decreases, and the dwelling time of the fluorescence photons in the resonator increases, which in turn enhances the CCLE performance. With the aligned cell given the pretreatment of a rapid annealing processing (RAP), the waiting time for obtaining an optimum CCLE can markedly be reduced sixfold. The surface alignment of the DDCLC cell also plays a necessary role in generating the CCLE. This work provides an insight into the temporal evolution of the performance for the CCLE laser and offers a method (RAP) of significantly speeding up the formation of a CCLE laser with optimum performance.

Photosensitive and all-optically fast-controllable photonic bandgap device and laser in a dye-doped blue phase with a low-concentration azobenzene liquid crystal.

This work demonstrates the feasibility of a novel photosensitive and all-optically fast-controllable photonic bandgap (PBG) device based on a dye-doped blue phase (DDBP), embedded with a low-concentration azobenzene liquid crystal (azo-LC). PBG of the DDBP can be reversibly fast-tuned off and on with the successive illumination of a weak UV and green beams. UV irradiation can transform the trans azo-LCs into bend cis isomers, which can easily disturb LCs at the boundary between the double twisting cylinders (DTCs) and the disclinations, and, then, quickly destabilize BPI to become a BPIII-like texture with randomly-oriented DTCs. Doing so may quickly destroy the BP PBG structure. However, with the successive illumination of a green beam, the BPI PBG device can be fast-turned on, owing to the fast disappearance of the disturbance of the azo-LCs on the boundary LCs via the green-beam-induced cis → trans back isomerization. The response time and irradiated energy density for turning off (on) the BP PBG device under the UV (green) beam irradiation are only 120 ms (120 ms) and 0.764 mJ/cm(2) (2.12 mJ/cm(2)), respectively, which are a thousand-fold reduction in photoswitching a traditional cholesteric LC (CLC) PBG device based on similar experimental conditions (i.e., materials used, azo-LC concentration (1 wt%), spectral position of PBG peak, sample thickness, and temperature difference for a working temperature lower than the clearing one). The BP PBG device can significantly contribute to efforts to develop a photosensitive and all-optically fast-controlling LC laser.

Spatially tunable photonic bandgap of wide spectral range and lasing emission based on a blue phase wedge cell.

This study demonstrates for the first time a continuously tunable photonic bandgap (PBG) of wide spectral range based on a blue phase (BP) wedge cell. A continuously shifting PBG of the BP wedge cell occurs due to the thickness gradient of the wedge cell at a fixed temperature. The wedge cell provides a gradient of boundary force on the LCs and thus forms a distribution of BP crystal structure with a gradient lattice. Additionally, a spatially tunable lasing emission based on a dye-doped BP (DDBP) wedge cell is also demonstrated. The tunable band of the PBG and lasing emission is about 130 nm and 70 nm, respectively, which tuning spectral ranges are significantly wider than those of CLC and DDCLC wedge cells, respectively. Such a BP device has a significant potential in applications of tunable photonic devices and displays.

Optically tunable/switchable omnidirectionally spherical microlaser based on a dye-doped cholesteric liquid crystal microdroplet with an azo-chiral dopant.

This paper presents an optically wavelength-tunable and intensity-switchable dye-doped cholesteric liquid crystal (DDCLC) spherical microlaser with an azo-chiral dopant. Experimental results present that two functions of optical control - tunability of lasing wavelength and switchability of lasing intensity - can be obtained for this spherical microlaser at low and high intensity regimes of non-polarized UV irradiation, respectively. If the DDCLC microdroplet is subjected to weak UV irradiation, azo-chiral molecules may transform to the bent cis state at a low concentration rate. The effect can slightly decrease the local order of LCs and thus the helical twisting power of the CLC in the microdroplet. As a result, the CLC pitch may become slightly elongated, which will cause the gradual red-shift of both omnidirectional PBG and lasing emission of the DDCLC spherical microdroplet. In contrast, when the microdroplet is subjected to strong UV irradiation, numerous azo-chiral molecules may simultaneously change to bent cis-isomers to seriously disarrange the helical texture of the CLC, which will quickly deform the PBG and deactivate the lasing emission of the microdroplet. Prolonged irradiation of a blue beam after strong UV irradiation may cause the cis azo-chiral molecules quickly convert back rod-like trans-isomers, which may then regenerate the CLC Bragg onion and PBG structures and reactivate the lasing emission of the microdroplet. Optical control of the DDCLC spherical microlaser is realized on a scale of seconds and minutes when UV irradiation is strong and weak, respectively. The 3D DDCLC spherical microlaser is a highly promising controllable 3D micro-light source or microlaser (e.g., all-optical 3D single photon microlaser) for applications of 3D all-optical integrated photonics, laser displays, and biomedical imaging and therapy, and as a 3D UV microdosagemeter or microsensor.

Optically controllable and focus-tunable Fresnel lens in azo-dye-doped liquid crystals using a Sagnac interferometer.

This study demonstrates a tunable Fresnel lens in an azo-dye-doped liquid crystal (ADDLC) film using an interference technique. One Fresnel-patterned green beam using a Sagnac interferometer irradiated the UV-illuminated ADDLC cell, yielding a concentric zone plate distribution with homeotropic and isotropic structures in bright and dark regions of the green interference pattern. The proposed Fresnel lens is polarization independent, focus tunable, and the focusing efficiency of the device can be optically controlled.

Electrically controllable liquid crystal random lasers below the Fréedericksz transition threshold.

This investigation elucidates for the first time electrically controllable random lasers below the threshold voltage in dye-doped liquid crystal (DDLC) cells with and without adding an azo-dye. Experimental results show that the lasing intensities and the energy thresholds of the random lasers can be decreased and increased, respectively, by increasing the applied voltage below the Fréedericksz transition threshold. The below-threshold-electric-controllability of the random lasers is attributable to the effective decrease of the spatial fluctuation of the orientational order and thus of the dielectric tensor of LCs by increasing the electric-field-aligned order of LCs below the threshold, thereby increasing the diffusion constant and decreasing the scattering strength of the fluorescence photons in their recurrent multiple scattering. This can result in the decrease in the lasing intensity of the random lasers and the increase in their energy thresholds. Furthermore, the addition of an azo-dye in DDLC cell can induce the range of the working voltage below the threshold for the control of the random laser to reduce.

All-optically controllable random laser based on a dye-doped liquid crystal added with a photoisomerizable dye.

This study investigates, for the first time, an all-optically controllable random laser based on a dye-doped liquid crystal (DDLC) cell added with a photoisomerizable dye. Experimental results indicate that the lasing intensity of this random laser can be all-optically controlled to decrease and increase sequentially with a two-step exposure of one UV and then one green beam. All-optically reversible controllability of the random lasing emission is attributed to the isothermal nematic(N)-->isotropic(I) and I-->N phase transitions for LCs due to the UV-beam-induced trans-->cis and green-beam-induced cis-->trans back isomerizations of the photoisomerizable dye, respectively. The former and the latter can decrease and increase the spatial fluctuations of the order and thus of the dielectric tensor of LCs, respectively, subsequently increasing and decreasing the diffusion constant (or transport mean free path), respectively, and thus decaying and rising the scattering strength for the fluorescence photons in their recurrent multi-scattering process, respectively. The consequent decrease and increase of the lasing intensity for the random laser and thus the rise and descent of its energy threshold are generated, respectively.

Photoerasable and photorewritable spatially-tunable laser based on a dye-doped cholesteric liquid crystal with a photoisomerizable chiral dopant.

This study investigates, for the first time, a photoerasable and photorewritable spatially-tunable laser using a dye-doped cholesteric liquid crystal (DDCLC) with a photoisomerizable chiral dopant (AzoM). UV illumination via a photomask with a transmittance-gradient can create a pitch gradient in the cell such that the lasing wavelength can be spatially tuned over a wide band of 134nm. The pitch gradient is generated by the UV-irradiation-induced gradient of the cis-AzoM concentration and therefore the induced gradient of the cell HTP value, resulting in the spatial tunability of the laser. Furthermore, the laser has advantages of photoerasability and photorewritability. The spatial tunability of the laser can undergo more than 100 cycles of photoerasing and photorewriting processes without decay or damage.

Photoinduced two-dimensional gratings based on dye-doped cholesteric liquid crystal films.

This work elucidates photoinduced two-dimensional (2D) gratings in dye-doped cholesteric liquid crystal films. The helical pitch is increased by green-beam-induced trans-cis isomerization and a concomitant thermal effect. Two-dimensional gratings appear when the green beam is turned off. Grating formation results from elastic instability caused by restored strain arising from helical pitch reduction. Grating lifetime increases as green beam intensity increases and declines under irradiation with a strong red beam. Variation in grating spacing with green intensity with various pitches is also examined.

Nonlinear optical property of azo-dye doped liquid crystals determined by biphotonic Z-scan technique.

This work investigates the optical Kerr property of azo-dye doped nematic liquid crystal films using the biphotonic Z-scan technique. The results indicate that the nonlinear effect measured using the Z-scan technique with a red light can be modulated or switched with the simultaneous application of a green light, because of photoisomerization and thermal effects, as determined by dynamic measurements. The former dominates in the early stage when the green light is applied, while the latter dominates in the later stage.