Short-wavelength excitation two-photon intravital microscopy of endogenous fluorophores.

The noninvasive two-photon excitation autofluorescence imaging of cellular and subcellular structure and dynamics in live tissue could provide critical in vivo information for biomedical studies. However, the two-photon microscopy of short-wavelength endogenous fluorophores, such as tryptophan and hemoglobin, is extremely limited due to the lack of suitable imaging techniques. In this study, we developed a short-wavelength excitation time- and spectrum-resolved two-photon microscopy system. A 520-nm femtosecond fiber laser was used as the excitation source, and a time-correlated single-photon counting module connected with a spectrograph was used to provide time- and spectrum-resolved detection capability. The system was specially designed for measuring ultraviolet and violet-blue fluorescence signals and thus was very suitable for imaging short-wavelength endogenous fluorophores. Using the system, we systematically compared the fluorescence spectra and fluorescence lifetimes of short-wavelength endogenous fluorophores, including the fluorescent molecules tyrosine, tryptophan, serotonin (5-HT), niacin (vitamin B3), pyridoxine (vitamin B6), and NADH and the protein group (keratin, elastin, and hemoglobin). Then, high-resolution three-dimensional (3D) label-free imaging of different biological tissues, including rat esophageal tissue, rat oral cheek tissue, and mouse ear skin, was performed in vivo or ex vivo. Finally, we conducted time-lapse imaging of leukocyte migration in the lipopolysaccharide injection immunization model and a mechanical trauma immunization model. The results indicate that the system can specifically characterize short-wavelength endogenous fluorophores and provide noninvasive label-free 3D visualization of fine structures and dynamics in biological systems. The microscopy system developed here can empower more flexible imaging of endogenous fluorophores and provide a novel method for the 3D monitoring of biological events in their native environment.

Direct mapping of bending and torsional dynamics in individual nanostructures.

Investigating coherent acoustic vibrations in nanostructured materials provides fundamental insights into optomechanical responses and microscopic energy flow. Extensive measurements of vibrational dynamics have been performed for a wide variety of nanoparticles and nanoparticle assemblies. However, virtually all of them show that only the dilation modes are launched after laser excitations, and the acoustic bending and torsional motions, which are commonly observed in photoexcited chemical bonds, are absent. Unambiguous identification and refined characterization of these "missing" modes have been a long-standing issue. In this report, we investigated the acoustic vibrational dynamics of individual Au nanoprisms on free-standing graphene substrates using an ultrafast high-sensitivity dark-field imaging approach in four-dimensional transmission electron microscopy. Following optical excitations, we observed low-frequency multiple-mode oscillations and higher superposition amplitudes at nanoprism corners and edges on the subnanoparticle level. In combination with finite-element simulations, we determined that these vibrational modes correspond to out-of-plane bending and torsional motions, superimposed by an overall tilting effect of the nanoprisms. The launch and relaxation processes of these modes are highly pertinent to substrate effects and nanoparticle geometries. These findings contribute to the fundamental understanding about acoustic dynamics of individual nanostructures and their interaction with substrates.

Bessel Beam Coherent Anti-Stokes Raman Scattering Spectroscopy for Turbulent Flow Diagnosis.

Coherent anti-Stokes Raman scattering (CARS) spectroscopy plays an important role in chemical analysis for transient flow dynamics. Due to the turbulent ambient conditions, the CARS spectrum often suffers from a poor signal-to-noise ratio (SNR) and cannot provide a convincing measurement. Here, we report on a CARS spectroscopic method using a Bessel beam to enhance the spectral fidelity and SNR in a quasi-turbulent environment. Compared with traditional CARS, the measurement accuracy is significantly improved by taking advantage of the anti-scattering and self-healing characteristics of the Bessel beam. Our preliminary results indicate that Bessel beam CARS could be a promising method for high precision turbulent flow measurement fields.

Single-Lens Light-Sheet Fluorescence Microscopy Based on Micro-Mirror Array.

Conventional light sheet fluorescence microscopy (LSFM) utilizes two perpendicularly arranged objective lenses for optical excitation and detection, respectively. Such a configuration often limits the use of high-numerical-aperture (NA) objectives or requires specially designed long-working-distance objectives. Here, a LSFM based on a micro-mirror array (MMA) to enable light sheet imaging with a single objective lens is reported. The planar fluorescent emission excited by the light sheet illumination is collected by the same objective, relayed onto an MMA and detected by a side-view camera. The proposed scheme makes LSFM compatible to single objective imaging system and shows promising candidacy for high spatiotemporal imaging.

New soliton dynamics revealed in the normal dispersion region.

Birefringence-involved phase matching is demonstrated to be a novel mechanism to generate transform limited solitary pulses in an ultrafast mode-locking fiber laser cavity with normal dispersion.

A protocol for single-source dual-pulse stimulated emission depletion setup with Bessel modulation.

STimulated Emission Depletion (STED) microscopy attains super-resolution in biological imaging beyond the diffraction limit. Here, we give a concise protocol to construct a dual-pulse STED setup with one super-continuum laser. Moreover, a flexible and dismountable Bessel modulation module is introduced for potential 2D-stack STED imaging. Experiments and notices are introduced in detail, with discussion on some important check-points for STED, such as detector saturation. Finally, the results validate the system working.

Differential fluorescence microscopy by using a dynamic cylindrical-vector field.

Fluorescence emission difference (FED) microscopy, as an emerging super-resolution imaging modality, uses double-exposure and subtraction between double-exposed fluorescence images to achieve high spatial resolution beyond the diffraction limit. Here we report on a new FED imaging approach with a single-exposure scheme based on dynamic cylindrical-vector fields, where the fluorescence excitation beam can be switched between radial and azimuthal polarization states at a designated high radio frequency. Lateral spatial resolution of ${\sim} \lambda/4$ is achieved. Being able to integrate with lock-in amplifier detection, the proposed method will find promising applications for high-speed fluorescence imaging with improved signal-to-noise ratio.

In vivo label-free two-photon excitation autofluorescence microscopy of microvasculature using a 520 nm femtosecond fiber laser.

Observing microvasculature in its native environment provides invaluable information to understand the initiation and development of microcirculatory related diseases. However, the lack of a high-resolution three-dimensional (3D) imaging technique hinders in vivo investigation of the microvasculature. Recently, we found that the red blood cells can emit autofluorescence signals with short-wavelength two-photon excitation. In this study, we exploited this property and developed a time-resolved two-photon excitation microscopy system using a homemade 520 nm femtosecond fiber laser as the excitation source. Using this system, we could achieve intravital high-resolution 3D imaging of a microvascular network noninvasively. In a mouse tumor model, tumorous blood vessels could be observed and distinguished clearly from the normal vessels.

Super-resolution fluorescence-assisted diffraction computational tomography reveals the three-dimensional landscape of the cellular organelle interactome.

The emergence of super-resolution (SR) fluorescence microscopy has rejuvenated the search for new cellular sub-structures. However, SR fluorescence microscopy achieves high contrast at the expense of a holistic view of the interacting partners and surrounding environment. Thus, we developed SR fluorescence-assisted diffraction computational tomography (SR-FACT), which combines label-free three-dimensional optical diffraction tomography (ODT) with two-dimensional fluorescence Hessian structured illumination microscopy. The ODT module is capable of resolving the mitochondria, lipid droplets, the nuclear membrane, chromosomes, the tubular endoplasmic reticulum, and lysosomes. Using dual-mode correlated live-cell imaging for a prolonged period of time, we observed novel subcellular structures named dark-vacuole bodies, the majority of which originate from densely populated perinuclear regions, and intensively interact with organelles such as the mitochondria and the nuclear membrane before ultimately collapsing into the plasma membrane. This work demonstrates the unique capabilities of SR-FACT, which suggests its wide applicability in cell biology in general.

Size-Dependent Phase Transition in Perovskite Nanocrystals.

The complex structure of halide and oxide perovskites strongly affects their physical properties. Here, the effect of dimensions reduced to the nanoscale has been investigated by a combination of single-dot optical experiments with a phase transition theory. Methylammonium lead bromide (CH3NH3PbBr3) nanocrystals with two average particle sizes of ∼2 and ∼4 nm with blue and green photoluminescence, respectively, were spectrally and temporally probed on a single-particle level from 5 to 295 K. The results show that the abrupt blue shift of the photoluminescence spectra and lifetimes at ∼150 K can be attributed to the cubic-to-tetragonal phase transition in the large 4 nm nanocrystals, while this phase transition is completely absent for the small 2 nm particles in the investigated temperature range. Theoretical calculations based on Landau theory reveal a strong size-dependent effect on temperature-induced phase transitions in individual CH3NH3PbBr3 nanocrystals, corroborating experimental observations. This effect should be considered in structure-property analysis of ultrasmall perovskite crystals.

Pattern-assisted stacking colloidal quantum dots for photonic integrated circuits.

In photonic integrated circuits (PICs), on-chip light sources and other photonic devices are usually made of different materials. The complexity and compatibility brought about by different materials and various structures in a single chip considerably increase the fabrication and integration difficulties. Here, we propose to stack the same nanoscale building blocks [colloidal quantum dots (CQDs) with both large gains and high refractive indices] in predefined trench patterns to address the fabrication and integration problems of PICs. By employing this simple approach of using the same material (CdSe/ZnS CQDs), the on-chip integration of more than 10 CQD-based photonic components (including the laser, low-noise amplifier, bending waveguide, Y-splitter, Mach-Zehnder interferometer, and grating) is experimentally demonstrated. In particular, the integrated low-noise amplifier (net gain coefficient >600 cm-1) addresses the absorption loss problem brought about by the utilization of the same material. Moreover, the little influence of the CQD layer on the CQD nanophotonic components facilitates the fabrication and is beneficial for large-scale integration. This simple fabrication approach with a flexible integration strategy may provide a possible platform to construct functional PICs.

Direct observation of ultrafast plasmonic hot electron transfer in the strong coupling regime.

Achieving strong coupling between plasmonic oscillators can significantly modulate their intrinsic optical properties. Here, we report the direct observation of ultrafast plasmonic hot electron transfer from an Au grating array to an MoS2 monolayer in the strong coupling regime between localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs). By means of femtosecond pump-probe spectroscopy, the measured hot electron transfer time is approximately 40 fs with a maximum external quantum yield of 1.65%. Our results suggest that strong coupling between LSPs and SPPs has synergetic effects on the generation of plasmonic hot carriers, where SPPs with a unique nonradiative feature can act as an 'energy recycle bin' to reuse the radiative energy of LSPs and contribute to hot carrier generation. Coherent energy exchange between plasmonic modes in the strong coupling regime can further enhance the vertical electric field and promote the transfer of hot electrons between the Au grating and the MoS2 monolayer. Our proposed plasmonic strong coupling configuration overcomes the challenge associated with utilizing hot carriers and is instructive in terms of improving the performance of plasmonic opto-electronic devices.

A Tunable Optofluidic Microlaser in a Photostable Conjugated Polymer.

The optofluidic laser has become an important platform for biological sensing and medical diagnosis. To date, fluorescent dyes and proteins have been widely utilized as gain materials for biological analysis due to their good biocompatibility, but the limited photostability restricts their reliability and sensitivity. Here, an optofluidic microlaser with an ultralow threshold down to 7.8 µJ cm-2 in the ultrahigh-Q whispering-gallery microcavity, which is filled with a biocompatible conjugated polymer, is demonstrated. This conjugated polymer exhibits a significant enhancement in the lasing stability compared with a typical laser dye (Nile red). In the experiment, after 20 min of illumination with the excitation intensity of 23.2 MW cm-2 , the lasing intensity of the conjugated polymer experiences a decrease of less than 10%, while the lasing feature of Nile red completely disappears. Additionally, by mechanically stretching the resonator, the lasing frequency can be fine-tuned with the range of about 2 nm, exceeding the free spectral range of the resonator.

Ultrafast Broadband Charge Collection from Clean Graphene/CH3NH3PbI3 Interface.

Photocarrier generation in a material, transportation to the material surface, and collection at the electrode interface are of paramount importance in any optoelectronic and photovoltaic device. In the last collection process, ideal performance comprises ultrafast charge collection to enhance current conversion efficiency and broadband collection to enhance energy conversion efficiency. Here, for the first time, we demonstrate ultrafast broadband charge collection achieved simultaneously at the clean graphene/organic-inorganic halide perovskite interface. The clean interface is realized by directly growing perovskite on graphene surface without polymer contamination. The tunable two-color pump-probe spectroscopy, time-resolved photoluminescence spectroscopy, and time-dependent density functional theory all reveal that the clean-interfacial graphene collects band-edge photocarriers of perovskite in an ultrashort time of ∼100 fs, with a current collection efficiency close to 99%. In addition, graphene can extract deep-band hot carriers of perovskite within only ∼50 fs, several orders faster than hot carrier relaxation and cooling in perovskite itself, due to the unique Dirac linear band structure of graphene, indicating a potential high energy conversion efficiency exceeding the Shockley-Queisser limit. Adding other graphene superiority of good transparency, high carrier mobility, and extreme flexibility, clean-interfacial graphene provides an ideal charge collection layer and electrode candidate for future optoelectronic and photovoltaic applications in two dimensions.

Configurable Integration of On-Chip Quantum Dot Lasers and Subwavelength Plasmonic Waveguides.

The integration of on-chip dielectric lasers and subwavelength plasmonic waveguides has attracted enormous attention because of the combination of both the advantages of the high performances of the small dielectric lasers and the subwavelength plasmonic waveguides. However, the configurable integration is still a challenge owing to the complexity of the hybrid structures and the damageability of the gain media in the multistep micro/nanofabrications. By employing the dark-field optical imaging technique with a position uncertainty of about 21 nm and combining the high-resolution electron beam lithography, the small colloidal quantum dot (CQD) lasers without any damages are accurately aligned with the silver nanowires. As a result, the integration of the CQD lasers and the silver nanowires can be flexibly configured on chips. In the experiment, the tangential coupling, radial coupling, and complex coupling between the high-performance CQD lasers and the subwavelength silver nanowires are demonstrated. Because of the subwavelength field confinements of the silver nanowires, the deep-subwavelength coherent sources (multimode, one-color single-mode, or two-color single-mode) with a mode area of only 0.008λ2 are output from these hybrid structures. This configurable on-chip integration with high flexibility and controllability will greatly facilitate the developments of the complex functional hybrid photonic-plasmonic circuits.

Time-of-flight detection of femtosecond laser pulses for precise measurement of large microelectronic step height.

We propose and demonstrate a new method which employs time-of-flight detection of femtosecond laser pulses for precise height measurement of large steps. By using time-of-flight detection with fiber-loop optical-microwave phase detectors, precise measurement of large step height is realized. The proposed method shows uncertainties of 15 nm and 6.5 nm at sampling periods of 40 ms and 800 ms, respectively. This method employs only one free-running femtosecond mode-locked laser and requires no scanning of laser repetition rate, making it easier to operate. Precise measurements of 6 µm and 0.5 mm step heights have been demonstrated, which show good functionality of this method for measurement of step heights.

Robust Stacking-Independent Ultrafast Charge Transfer in MoS2/WS2 Bilayers.

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS2/WS2 bilayer with various stacking configurations, by optical two-color ultrafast pump-probe spectroscopy. Surprisingly, we found that the charge transfer is robust against varying interlayer twist angles and interlayer coupling strength, in time scale of ∼90 fs. Our observation, together with atomic-resolved transmission electron characterization and time-dependent density functional theory simulations, reveals that the robust ultrafast charge transfer is attributed to the heterogeneous interlayer stretching/sliding, which provides additional channels for efficient charge transfer previously unknown. Our results elucidate the origin of transfer rate robustness against interlayer stacking configurations in optical devices based on 2D heterostructures, facilitating their applications in ultrafast and high-efficient optoelectronic and photovoltaic devices in the near future.

High-precision multi-node clock network distribution.

A high precision multi-node clock network for multiple users was built following the precise frequency transmission and time synchronization of 120 km fiber. The network topology adopts a simple star-shaped network structure. The clock signal of a hydrogen maser (synchronized with UTC) was recovered from a 120 km telecommunication fiber link and then was distributed to 4 sub-stations. The fractional frequency instability of all substations is in the level of 10-15 in a second and the clock offset instability is in sub-ps in root-mean-square average.

Ultrasensitive, high-dynamic-range and broadband strain sensing by time-of-flight detection with femtosecond-laser frequency combs.

Ultrahigh-resolution optical strain sensors provide powerful tools in various scientific and engineering fields, ranging from long-baseline interferometers to civil and aerospace industries. Here we demonstrate an ultrahigh-resolution fibre strain sensing method by directly detecting the time-of-flight (TOF) change of the optical pulse train generated from a free-running passively mode-locked laser (MLL) frequency comb. We achieved a local strain resolution of 18 pε/Hz1/2 and 1.9 pε/Hz1/2 at 1 Hz and 3 kHz, respectively, with large dynamic range of >154 dB at 3 kHz. For remote-point sensing at 1-km distance, 80 pε/Hz1/2 (at 1 Hz) and 2.2 pε/Hz1/2 (at 3 kHz) resolution is demonstrated. While attaining both ultrahigh resolution and large dynamic range, the demonstrated method can be readily extended for multiple-point sensing as well by taking advantage of the broad optical comb spectra. These advantages may allow various applications of this sensor in geophysical science, structural health monitoring, and underwater science.

Ultra-broadband enhancement of nonlinear optical processes from randomly patterned super absorbing metasurfaces.

Broadband light trapping and field localization is highly desired in enhanced light-matter interaction, especially in harmonic generations. However, due to the limited resonant bandwidth, most periodic plasmonic nanostructures cannot cover both fundamental excitation wavelength and harmonic generation wavelength simultaneously. Therefore, most previously reported plasmonic nonlinear optical processes are low in conversion efficiency. Here, we report a strong enhancement of second harmonic generation based on a three-layered super absorbing metasurface structure consisting of a dielectric spacer layer sandwiched by an array of random metallic nanoantennas and a metal ground plate. Intriguingly, the strong light trapping band (e.g. >80%) was realized throughout the entire visible to near-infrared spectral regime (i.e., from 435 nm to 1100 nm), enabling plasmonically enhanced surface harmonic generation and frequency mixing across a broad range of excitation wavelengths, which cannot be achieved with narrow band periodic plasmonic structures. By introducing hybrid random antenna arrays with small metallic nanoparticles and ultra-thin nonlinear optical films (e.g. TiO2) into the nanogaps, the nonlinear optical process can be further enhanced. This broadband light-trapping metastructure shows its potential as a building block for emerging nonlinear optical meta-atoms.