Haiyun Dong

Broadband Tunable Microlasers Based on Controlled Intramolecular Charge-Transfer Process in Organic Supramolecular Microcrystals

Wavelength tunable micro/nanolasers are indispensable components for various photonic devices. Here, we report broadband tunable microlasers built by incorporating a highly polarized organic intramolecular charge-transfer (ICT) compound with a supramolecular host. The spatial confinement of the ICT dye generates an optimized energy level system that favors controlled population distribution between the locally excited (LE) state and the twisted intramolecular charge-transfer (TICT) state, which is beneficial for significantly broadening the tailorable gain region. As a result, we realized a wide tuning of lasing wavelength in the organic supramolecular microcrystals based on temperature-controlled population transfer from the LE to TICT state. The results will provide a useful enlightenment for the rational design of miniaturized lasers with desired performances.

Wavelength-Tunable Microlasers Based on the Encapsulation of Organic Dye in Metal-Organic Frameworks.

A wavelength-tunable microlaser is realized based on the controlled intramolecular charge transfer (ICT) process in dye-encapsulated metal-organic framework (MOF) material. The confinement effect of the MOFs is beneficial for low-threshold lasing. By effectively controlling the polarity of the MOF pores, the population distribution between the locally excited and ICT states is continuously modulated, thus achieving broadband tunable MOF-based microlasers.

Dual-Wavelength Switchable Vibronic Lasing in Single-Crystal Organic Microdisks

Wavelength switchable micro/nanoscale laser is essential to construct various ultracompact photonic devices. However, traditional semiconductors as the gain media generally provide only monochromatic laser output due to their continuous energy band structures. For luminescent conjugated molecules, the broad emission band usually contains a series of vibronic peaks, which is very helpful for extending the lasing spectrum to several different wavelengths. Here we propose a novel strategy to realize wavelength switchable lasers based on the controlled competition of dual-wavelength vibronic lasing in single-component organic microcrystals. The vibrationally structured fluorescence property of the single-crystal organic microdisks brings dual-wavelength lasing at different vibronic bands. Their relative optical gain intensity was modulated by controlling the population on the certain vibronic level of the ground state with varied temperature, which consequently enabled the reversible switching of the dual-wavelength vibronic lasing. The results point out a promising route to the rational design of miniaturized lasers and other photonic elements with desired performances.

Dual-color single-mode lasing in axially coupled organic nanowire resonators

Dual-color single-mode nanolasers were experimentally achieved in axially coupled organic nanowire heterogeneous resonators. Miniaturized lasers with multicolor output and high spectral purity are of crucial importance for yielding more compact and more versatile photonic devices. However, multicolor lasers usually operate in multimode, which largely restricts their practical applications due to the lack of an effective mode selection mechanism that is simultaneously applicable to multiple wavebands. We propose a mutual mode selection strategy to realize dual-color single-mode lasing in axially coupled cavities constructed from two distinct organic self-assembled single-crystal nanowires. The unique mode selection mechanism in the heterogeneously coupled nanowires was elucidated experimentally and theoretically. With each individual nanowire functioning as both the laser source and the mode filter for the other nanowire, dual-color single-mode lasing was successfully achieved in the axially coupled heterogeneous nanowire resonators. Furthermore, the heterogeneously coupled resonators provided multiple nanoscale output ports for delivering coherent signals with different colors, which could greatly contribute to increasing the integration level of functional photonic devices. These results advance the fundamental understanding of the lasing modulation in coupled cavity systems and offer a promising route to building multifunctional nanoscale lasers for high-level practical photonic integrations.

Polymorph-Dependent Electrogenerated Chemiluminescence of Low-Dimensional Organic Semiconductor Structures for Sensing

A sensitive electrogenerated chemiluminescence (ECL) sensor with an organic semiconductor as active material for detecting trace amounts of molecules has been highly desired. However, the crystal structure responses of the ECL properties of the organic semiconductor materials, that is, structure-property relationship, is not clear, which limits the development of the sensitive ECL sensors. Herein, for the first time, we reported a novel concept for molecular-stacking-arrangement-dependent electrogenerated chemiluminescence properties of organic semiconductor rubrene microstructures. The rubrene 1D microwires and 2D hexagonal plates with different polymorphs (triclinic and monoclinic) were controllably constructed with the reprecipitation method. The supersaturation of the rubrene molecules plays an important role in the thermodynamically and kinetically dominated process of growth, which affects not only the polymorphs but also the morphology of the obtained microstructures. These microstructures show good optoelectronic properties, which are used as active ECL materials for the construction of ECL sensors. The ECL sensors exhibited distinct electrogenerated chemiluminescence properties, probably related to different inherent crystal-structure-dependent triplet-triplet annihilation rate and charge-transfer rate. The sensors manifested electrogenerated chemiluminescence responses in broad linear range for the monitoring of creatinine molecules.

Wavelength‐Controlled Organic Microlasers Based on Polymorphism‐Dependent Intramolecular Charge‐Transfer Process

Wavelength-tunable micro/nanoscale lasers are particularly attractive as indispensible building blocks for various ultracompact photonic devices. Polymorphic organic materials display distinct emission colors in different crystal forms, providing the potential possibility in tailoring the lasing wavelength. Here we report wavelength-controlled microlasers based on the polymorphism-dependent intramolecular charge-transfer (ICT) process in organic microcrystals. With different solution-phase self-assembly methods, three kinds of microstructures were prepared from the same organic ICT compound, where the different crystal structures offer completely distinct molecular environments, having a significant influence on the excited-state ICT process and therefore the emission wavelength. As a result, we realized three different color lasing actions in these three kinds of organic ICT microcystals under two-photon pumping. The results demonstrated here provide useful insights for the rational design of miniaturized lasers with desired performances.

Host–guest composite organic microlasers

Organic microlasers are miniaturized coherent light sources with great promise for advancing the field of optoelectronics. Recently, host–guest composite organic microlasers, where the host materials provide spatial confinement for the organic gain materials, have captured much research interest because the host–guest composite material systems endow the organic microlasers with improved lasing performances, such as low threshold, high stability, and excellent tunability. In this Review, we explore the latest advancements in the development of host–guest composite organic microlasers, and offer our perspective on future improvements and trends. Special emphasis is put on the construction strategies and the unique laser properties of the organic microlasers based on host–guest confinement systems. The comprehensive understanding of the relationship between laser performances and the synergistic interactions of the host and guest materials would provide a useful guidance for the design and fabrication of novel organic microlasers.

Covert Photonic Barcodes Based on Light Controlled Acidichromism in Organic Dye Doped Whispering‐Gallery‐Mode Microdisks

Photonic barcodes with a small footprint have demonstrated a great value for multiplexed high-throughput bioassays and tracking systems. Attempts to develop coding technology tend to focus on the generation of featured barcodes both with high coding capacity and accurate recognition. In this work, a strategy to design photonic barcodes is proposed based on whispering-gallery-mode (WGM) modulations in dye-doped microdisk resonant cavities, where each modulated photoluminescence spectrum constitutes the fingerprint of a corresponding microdisk. The WGM-based barcodes can achieve infinite encoding capacity through tuning the dimensions of the microdisks. These photonic barcodes can be well disguised and decoded based on the light controlled proton release and acidichromism of the organic materials, which are essential to fulfill the functions of anti-counterfeiting, information security, and so on. The results will pave an avenue to new types of flexible WGM-based components for optical data recording and security labels.

Organic Microcrystal Vibronic Lasers with Full‐Spectrum Tunable Output beyond the Franck–Condon Principle

The very broad emission bands of organic semiconductor materials are, in theory, suitable for achieving versatile solid-state lasers; however, most of organic materials only lase at short wavelength corresponding to the 0-1 transition governed by the Franck-Condon (FC) principle. A strategy is developed to overcome the limit of FC principle for tailoring the output of microlasers over a wide range based on the controlled vibronic emission of organic materials at microcrystal state. For the first time, the output wavelength of organic lasers is tailored across all vibronic (0-1, 0-2, 0-3, and even 0-4) bands spanning the entire emission spectrum.

Stimulated Emission-Controlled Photonic Transistor on a Single Organic Triblock Nanowire

In this work, we demonstrate a stimulated emission-controlled photonic transistor on a single organic triblock nanowire composed of alternate energy donor and acceptor. The population of acceptor excitons was engineered by energy transfer to achieve enhanced fluorescence, which was further amplified by the stimulated emission of the donor and the optical feedback in the nanowire microcavities, yielding a remarkable nonlinear amplification of the acceptor emission. On this basis, a prototype of photonic transistor with high nonlinear gain at very low pump energy was achieved. The results will provide a useful enlightenment for the rational design of novel all-optical switches with desired performances.