Optical Coupling in Atomic Waveguide for Vertically Integrated Photonics.

Integrated 2-dimensional (2D) photonic devices such as monolayer waveguide has generated exceptional interest because of their ultimate thinness. In particular, they potentially permit stereo photonic architecture through bond-free van der Waals integration. However, little is known about the coupling and controlling of the single-atom guided wave to its photonic environment, which governs the design and application of integrated system. Here, we report the optical coupling of atomically guided waves to other photonic modes. We directly probe the mode beating between evanescent waves in a monolayer 2D waveguide and a silicon photonic waveguide, which constitutes a vertically integrated interferometer. The mode-coupling measures the dispersion relation of the guided wave inside the atomic waveguide and unveils it strongly modifies matter's electronic states, manifesting by the formation of a propagating polariton. We also demonstrated light modulating and spectral detecting in this compact nonplanar interferometer. These findings provide a generalizable and versatile platform toward monolithic 3-dimensional integrated photonics.

Probing the interlayer excitation dynamics in WS2/WSe2 heterostructures with broadly tunable pump and probe energies.

van der Waals heterostructures based on transition metal dichalcogenides (TMDs) provide a fascinating platform for exploring new physical phenomena and novel optoelectronic functionalities. Revealing the energy-dependence of photocarrier population dynamics in heterostructures is key for developing optoelectronic or valleytronic devices. Here, the broadband transient dynamics of interlayer excitation of a nearly-aligned WS2/WSe2 heterostructure is investigated by using energy-dependent pump-probe spectroscopy at cryogenic temperatures. Interestingly, WS2/WSe2 interlayer excitation, herein comprising a mixture of intra- and inter-layer excitons, exhibits largely constant lifetimes of a few hundred picoseconds across a broad energy range, in stark contrast to the salient energy-dependent dynamics of intralayer excitons in monolayer WSe2. While the PL emission of the WS2/WSe2 heterostructure is found to be strongly affected by electrostatic doping, the lifetimes of interlayer excitation show negligible changes. Our work elaborates the signatures of ultrafast dynamics introduced by intra- and interlayer co-existing excitonic species and enriches the understanding of interlayer couplings in van der Waals heterostructures.

Gate Controlled Photocurrent Generation Mechanism in Air-Grown Organic Single Crystals for High-Speed Multiband Imaging.

Organic semiconductors herald new opportunities for fabricating high-performance flexible and wearable optoelectronic devices owing to their intrinsic mechanical flexibility, excellent optical absorption, and cool-free operation. The photocurrent generation mechanisms are of multiple physical origins, including photoconductive, photovoltaic, and photogating effects, and the influence of individual effects on the device figures-of-merit is still not well understood. Here we fabricated a high-performance pentacene single-crystal transistor employing graphene electrodes and demonstrated the modulation from the photogating mechanism to the photoconduction effect by controlling gate bias. Control experiments indicate that the calculation based on transfer curves tends to overestimate the responsivity due to nearby trap states. Using a high frequency-modulated light signal to suppress the trapping process, we successfully measured its intrinsic -3 dB bandwidth of 75 kHz. Finally, high-resolution and UV-NIR high-speed imaging capability was demonstrated. Our work provides new guidelines for understanding the photophysical process and intrinsic performances of organic devices and also confirms the potential of organic single crystals in high-speed imaging applications.

Optical-fiber-integrated high-speed organic phototransistor with broadband imaging capacity.

Fiber optic communication is becoming the central pillar of modern high-speed communication technology, which involves the abundant fiber components. Currently, most of photodetectors are fabricated on the silicon chip, so mass fiber-to-chip interfaces increase the complexity of advanced optoelectronic system, and also grow the risk of optical information loss. Here, we report an all-fiber organic phototransistor by employing rubrene single crystal and few-layer graphene to realize the "plug-to-play" operation. The device shows a broadband photoresponse from the ultraviolet to visible range, with fast response times of approximately 130/170 µs and reasonable specific detectivity of 6 × 109 Jones, which is close to the level of commercial on-chip device. Finally, several imaging applications are successfully demonstrated by deploying this all-fiber device. Our work provided an efficient strategy for fabricating all-fiber organic devices, and confirmed their significant potential in future optical fiber optoelectronics.

Quantum criticality of excitonic Mott metal-insulator transitions in black phosphorus.

Quantum phase transition refers to the abrupt change of ground states of many-body systems driven by quantum fluctuations. It hosts various intriguing exotic states around its quantum critical points approaching zero temperature. Here we report the spectroscopic and transport evidences of quantum critical phenomena of an exciton Mott metal-insulator-transition in black phosphorus. Continuously tuning the interplay of electron-hole pairs by photo-excitation and using Fourier-transform photo-current spectroscopy as a probe, we measure a comprehensive phase diagram of electron-hole states in temperature and electron-hole pair density parameter space. We characterize an evolution from optical insulator with sharp excitonic transition to metallic electron-hole plasma phases featured by broad absorption and population inversion. We also observe strange metal behavior that resistivity is linear in temperature near the Mott transition boundaries. Our results exemplify an ideal platform to investigating strongly-correlated physics in semiconductors, such as crossover between superconductivity and superfluity of exciton condensation.

Ultrafast and Sensitive Self-Powered Photodetector Based on Graphene/Pentacene Single Crystal Heterostructure with Weak Light Detection Capacity.

Organic materials exhibit efficient light absorption and low-temperature, large-scale processability, and have stimulated enormous research efforts for next-generation optoelectronics. While, high-performance organic devices with fast speed and high responsivity still face intractable challenges, due to their intrinsic limitations including finite carrier mobility and high exciton binding energy. Here an ultrafast and highly sensitive broadband phototransistor is demonstrated by integrating high-quality pentacene single crystal with monolayer graphene. Encouragingly, the -3 dB bandwidth can reach up to 26 kHz, which is a record-speed for such sensitized organic phototransistors. Enormous absorption, long exciton diffusion length of pentacene crystal, and efficient interfacial charge transfer enable a high responsivity of >105  A W-1  and specific detectivity of >1011  Jones. Moreover, self-powered weak-light detection is realized using a simple asymmetric configuration, and the obvious zero-bias photoresponses can be displayed even under 750 nW cm-2  light intensity. Excellent response speed and photoresponsivity enable high-speed image sensor capability in UV-Vis ranges.  The results offer a practical strategy for constructing high-performance self-powered organic hybrid photodetectors, with strong applicability in wireless, weak-light detection, and video-frame-rate imaging applications.

Probing the mode-locking pattern in the parameter space of a Figure-9 laser.

Due to the many available cavity configurations, a generalized approach for identifying the optimal operating state of a Figure-9 mode-locked laser has proved a challenge. In this Letter, we probe the output pulsation states of an exemplar Figure-9 laser by meticulously scanning its parameter space. Regions corresponding to mode-locked operations are identified periodically in the map of the output states. We correlate these regions to a set of band-like cavity transmission functions that fundamentally allow ultra-short pulse formation. Interestingly, a clear correlation between the mode-locking pattern and the cavity configuration is observed. For example, with the decrease of the fiber loop symmetry in the cavity, half of the solutions in the mode-locking pattern are found to transit to forbidden states. Numerical calculations based on the Jones matrix are used to explain the experimental observations. In addition, the dynamic change of the map of output states is illustrated by using a setup with an automatic algorithm. Our results provide a visually-rich yet simple way for evaluating and optimizing a Figure-9 laser.

Hysteresis of a passively mode-locked fiber laser: effects from cavity dispersion.

Hysteresis is a common phenomenon in passively mode-locked lasers and refers to the effect where the thresholds marking transitions between different pulsation states are not the same for an increasing or decreasing pump power. Despite wide presence in experimental observations, the general dynamics of hysteresis remains elusive, largely due to the challenge to acquire the full hysteresis dynamics of a given mode-locked laser. In this Letter, we overcome this technical bottleneck by fully characterizing an exemplar figure-9 fiber laser cavity, which exhibits well-defined mode-locking patterns in its parameter space or "primitive cell." We varied the net cavity dispersion and observed the salient change of hysteresis characteristics. Specifically, transiting from an anomalous to a normal cavity dispersion is found to consistently increase the likelihood of the single-pulse mode-locking regime. To the best of our knowledge, this is the first time that a laser's hysteresis dynamic is fully probed and related to fundamental cavity parameters.

Highly Sensitive and Ultrafast Organic Phototransistor Based on Rubrene Single Crystals.

Rubrene single crystals have received a lot of attention for their great potential in electronic and wearable nanoelectronics due to their high carrier mobility and excellent flexibility. While they exhibited remarkable electrical performances, their intrinsic potential as photon detectors has not been fully exploited. Here, we fabricate a sensitive and ultrafast organic phototransistor based on rubrene single crystals. The device covers the ultraviolet to visible range (275-532 nm), and the responsivity and detectivity can reach up to ∼4000 A W-1 and 1011 jones at 532 nm, respectively. Furthermore, the response times are highly gate-tunable down to sub-90 µs, and the cutoff frequency is ∼4 kHz, which is one of the fastest organic material-based phototransistors reported so far. Equally important is that the fabricated device exhibits stable light detection ability even after 8 months, indicating great long-term stability and excellent environmental robustness. The results suggest that the high-quality rubrene single crystal may be a promising material for future flexible optoelectronics with its intrinsic mechanical flexibility.

10†GHz regeneratively mode-locked thulium fiber laser with a stabilized repetition rate.

GHz pulsed thulium-doped fiber laser with stabilized repetition rate can enable a wide range of applications. By employing regenerative mode-locking and cavity stabilization technique, we have for the first time demonstrated a 10 GHz polarization-maintaining thulium-doped fiber laser, which has a long-term repetition-rate stabilization and picosecond timing-jitter. In our experiment, a RF circuitry is designed to extract the 10 GHz longitudinal clock signal so that stable regenerative mode-locking is achieved. A piezo actuator-based phase-lock-loop is used to lock the regeneratively mode-locked pulses to a local reference synthesizer. The regeneratively mode-locked pulses with picosecond pulse width exhibit a high super-mode suppression ratio of 60 dB. In addition, the repetition rate of the laser shows good long-term stability with a variation of 8 Hz in 8 hours, corresponding to a cavity free spectral range fluctuation of less than 16 mHz. Meanwhile, the Allan deviation of the stabilized 10 GHz regeneratively mode-locked pulses is measured to be as low as 2 × 10-12 over 1000 s average time, which is only limited by the stability of the reference synthesizer. Such an ultra-stable 10 GHz pulsed thulium fiber laser may find potential application in 2 µm optical communication, material processing and spectroscopy.

High energy (>40 nJ), sub-100 fs, 950 nm laser for two-photon microscopy.

Compact and high-energy femtosecond fiber lasers operating around 900-950 nm are desirable for multiphoton microscopy. Here, we demonstrate a >40 nJ, sub-100 fs, wavelength-tunable ultrafast laser system based on chirped pulse amplification (CPA) in thulium-doped fiber and second-harmonic generation (SHG) technology. Through effective control of the nonlinear effect in the CPA process, we have obtained 92-fs pulses at 1903 nm with an average power of 0.89 W and a pulse energy of 81 nJ. By frequency doubling, 95-fs pulses at 954 nm with an average power of 0.46 W and a pulse energy of 42 nJ have been generated. In addition, our system can also achieve tunable wavelength from 932 nm to 962 nm (frequency doubled from 1863 nm to 1919 nm). A pulse width of ∼100 fs and sufficient pulse energy are ensured over the entire tuning range. Finally, we applied the laser in a two-photon microscope and obtained superior imaging results. Due to a relatively low repetition rate (∼ 10 MHz), similar imaging quality can be achieved at significantly reduced average power compared with a commercial 80 MHz laser system. At the same time, the lower average power is helpful in limiting the thermal load to the samples. It is believed that such a setup, with its well-balanced optical characteristics and compact footprint, provides an ideal source for two-photon microscopy.

Pushing Optical Switch into Deep Mid-Infrared Region: Band Theory, Characterization, and Performance of Topological Semimetal Antimonene.

The existing pulsed laser technologies and devices are mainly in the infrared spectral region below 3 µm so far. However, longer-wavelength pulsed lasers operating in the deep mid-infrared region (3-20 µm) are desirable for atmosphere spectroscopy, remote sensing, laser lidar, and free-space optical communications. Currently, the lack of reliable optical switches is the main limitation for developing pulsed lasers in the deep mid-infrared region. Here, we demonstrate that topological semimetal antimonene possesses an ultrabroadband optical switch characteristic covering from 2 µm to beyond 10 µm. Especially, the topological semimetal antimonene shows a very low saturable energy fluence (only 3-15 nJ cm-2 beyond 3 µm) and an ultrafast recovery time of ps level. We also demonstrate stable Q-switching in fiber lasers at 2 and 3.5 µm by using topological semimetal antimonene as passive optical switches. Combined with the high environmental stability and easy fabrication, topological semimetal antimonene offers a promising optical switch that extends pulsed lasers into deep mid-infrared region.

Modulation of photocarrier relaxation dynamics in two-dimensional semiconductors.

Due to strong Coulomb interactions, two-dimensional (2D) semiconductors can support excitons with large binding energies and complex many-particle states. Their strong light-matter coupling and emerging excitonic phenomena make them potential candidates for next-generation optoelectronic and valleytronic devices. The relaxation dynamics of optically excited states are a key ingredient of excitonic physics and directly impact the quantum efficiency and operating bandwidth of most photonic devices. Here, we summarize recent efforts in probing and modulating the photocarrier relaxation dynamics in 2D semiconductors. We classify these results according to the relaxation pathways or mechanisms they are associated with. The approaches discussed include both tailoring sample properties, such as the defect distribution and band structure, and applying external stimuli such as electric fields and mechanical strain. Particular emphasis is placed on discussing how the unique features of 2D semiconductors, including enhanced Coulomb interactions, sensitivity to the surrounding environment, flexible van der Waals (vdW) heterostructure construction, and non-degenerate valley/spin index of 2D transition metal dichalcogenides (TMDs), manifest themselves during photocarrier relaxation and how they can be manipulated. The extensive physical mechanisms that can be used to modulate photocarrier relaxation dynamics are instrumental for understanding and utilizing excitonic states in 2D semiconductors.

Ultrafast lattice and electronic dynamics in single-walled carbon nanotubes.

Understanding the photoinduced ultrafast structural transitions and electronic dynamics in single-walled carbon nanotubes (SWCNTs) is important for the development of SWCNT-based optoelectronic devices. In this study, we conducted femtosecond-resolved electron diffraction and electron energy-loss spectroscopy (EELS) measurements on SWCNTs using ultrafast transmission electron microscopy. The experimental results demonstrated that dominant time constants of the dynamic processes were ∼1.4 ps for electron-driven lattice expansion, ∼17.4 ps for thermal phonon-driven lattice expansion associated with electron-phonon coupling. The time-resolved EELS measurements clearly revealed a notable red shift of plasmon peaks by ∼100 meV upon femtosecond laser excitation. Different features of charge carrier excitation and relaxation were carefully discussed in correlation with the lattice dynamics and photoinduced absorption signals of SWCNTs. Our results provide a comprehensive understanding of the ultrafast dynamics in SWCNTs and powerful techniques to characterize the dynamics of low-dimensional structures.

Graphene Hybrid Structures for Integrated and Flexible Optoelectronics.

Graphene (Gr) has many unique properties including gapless band structure, ultrafast carrier dynamics, high carrier mobility, and flexibility, making it appealing for ultrafast, broadband, and flexible optoelectronics. To overcome its intrinsic limit of low absorption, hybrid structures are exploited to improve the device performance. Particularly, van der Waals heterostructures with different photosensitive materials and photonic structures are very effective for improving photodetection and modulation efficiency. With such hybrid structures, Gr hybrid photodetectors can operate from ultraviolet to terahertz, with significantly improved R (up to 109 A W-1 ) and bandwidth (up to 128 GHz). Furthermore, integration of Gr with silicon (Si) complementary metal-oxide-semiconductor (CMOS) circuits, the human body, and soft tissues is successfully demonstrated, opening promising opportunities for wearable sensors and biomedical electronics. Here, the recent progress in using Gr hybrid structures toward high-performance photodetectors and integrated optoelectronic applications is reviewed.

Fast Photoelectric Conversion in the Near-Infrared Enabled by Plasmon-Induced Hot-Electron Transfer.

Interfacial charge transfer is a fundamental and crucial process in photoelectric conversion. If charge transfer is not fast enough, carrier harvesting can compromise with competitive relaxation pathways, e.g., cooling, trapping, and recombination. Some of these processes can strongly affect the speed and efficiency of photoelectric conversion. In this work, it is elaborated that plasmon-induced hot-electron transfer (HET) from tungsten suboxide to graphene is a sufficiently fast process to prevent carrier cooling and trapping processes. A fast near-infrared detector empowered by HET is demonstrated, and the response time is three orders of magnitude faster than that based on common band-edge electron transfer. Moreover, HET can overcome the spectral limit of the bandgap of tungsten suboxide (≈2.8 eV) to extent the photoresponse to the communication band of 1550 nm (≈0.8 eV). These results indicate that plasmon-induced HET is a new strategy for implementation of efficient and high-speed photoelectric devices.

Slowing down photocarrier relaxation in Dirac semimetal Cd3As2 via Mn doping.

In this Letter, we successfully introduce a long-lived non-radiative photocarrier decay component in a Dirac semimetal Cd3As2 thin film via Mn doping. The long-lived decay component is found to vary between 200 ps and 2.8 ns with different Mn concentrations and probing wavelengths. Most remarkably, the elongated transients persist over the important mid-infrared wavelengths (observed up to 4 µm). Saturable absorption measurement reveals stronger modulation effects for long-width pulses (∼80 ps) from the Mn-doped samples. Our results provide new insights into the effect of transition-metal doping on the ultrafast optical properties of Dirac semimetal Cd3As2 and establish Cd3As2 as a highly amendable material for mid-infrared photonic applications.

InAs-Nanowire-Based Broadband Ultrafast Optical Switch.

Due to their tunable optical properties with various shapes, sizes, and compositions, nanowires (NWs) have been regarded as a class of semiconductor nanostructures with great potential for photodetectors, light-emitting diodes, gas sensors, microcavity lasers, optical modulators, and converters. Indium arsenide (InAs), an attractive III-V semiconductor NW with the advantages of narrow bandgap and large electron mobility, has attracted considerable interest in infrared optoelectronic and photonic devices. Here, we studied the ultrafast carrier dynamics and nonlinear optical responses of InAs NWs ranging from 1.0 to 2.8 µm and demonstrated the InAs-NW-based ultrafast broadband optical switch for passively Q-switching in all-solid-state laser systems. Furthermore, we achieved ultrafast optical modulation for laser mode-locking at 1.0 µm, paving the way for their applications in the field of ultrafast optics. These exotic optical properties indicate that InAs NWs have significant potential for various optoelectronic and photonic devices, especially in the mid-infrared wavelength range.

Dirac semimetal saturable absorber with actively tunable modulation depth.

In this Letter, we demonstrate an electrically contacted saturable absorber (SA) device based on topological Dirac semimetal Cd3As2. With a current-induced temperature change in the range of 297-336 K, the modulation depth of the device is found to be significantly altered from 33% to 76% (under the irradiation of a 1560 nm femtosecond laser). The broad tuning of the modulation depth is attributed to the strong temperature dependence of the carrier concentration close to room temperature. The simple tuning mechanism uncovered here, together with the compatibility with III-V compounds substrate, such as GaAs, points to the potential of fabricating broadband, electrically tunable, SESAM-like devices based on emerging bulk Dirac materials.

Nanotube mode-locked, wavelength and pulsewidth tunable thulium fiber laser.

Mode-locked oscillators with highly tunable output characteristics are desirable for a range of applications. Here, with a custom-made tunable filter, we demonstrate a carbon nanotube (CNT) mode-locked thulium fiber laser with widely tunable wavelength, spectral bandwidth, and pulse duration. The demonstrated laser's wavelength tuning range reached 300 nm (from 1733 nm to 2033 nm), which is the widest-ever that was reported for rare-earth ion doped fiber oscillators in the near-infrared. At each wavelength, the pulse duration can be regulated by changing the filter's bandwidth. For example, at ~1902 nm, the pulse duration can be adjusted from 0.9 ps to 6.4 ps (the corresponding output spectral bandwidth from 4.3 nm to 0.6 nm). Furthermore, we experimentally and numerically study the spectral evolution of the mode-locked laser in presence of a tunable filter, a topic that has not been thoroughly investigated for thulium-doped fiber lasers. The detailed dynamical change of the mode-locked spectra is presented and we observed gradual suppression of the Kelly sidebands as the filter's bandwidth is reduced. Further, using the polarization-maintaiing (PM) cavity ensures that the laser is stable and the output laser's polarization extinction ratio is measured to exceed 20 dB.