Quantitative gas pressure measurement by molecular spectroscopy using chip-based supercontinuum in the mid-infrared.

We demonstrate the quantitative pressure measurement of gas molecules in the mid-infrared using chip-based supercontinuum and cepstrum analysis without additional measurements for baseline normalization. A supercontinuum generated in an on-chip waveguide made of chalcogenide glass having high nonlinearity passes through CO gas and provides a transmission spectrum. The gas absorption information is deconvoluted from the original supercontinuum spectral information containing temporal fluctuation by cepstrum analysis and extracted simply by applying a bandpass filter in the temporal domain. The gas pressure estimated from the extracted absorption information is consistent with the value measured by a pressure gauge within a difference of 1.25%, despite spectral fluctuations in the supercontinuum baseline comparable to the spectral depth of the gas absorption lines.

Design of High-Performance Organic Nonlinear Optical and Terahertz Crystals by Controlling the van der Waals Volume.

In the development of new organic crystals for nonlinear optical and terahertz (THz) applications, it is very challenging to achieve the essentially required non-centrosymmetric molecular arrangement. Moreover, the resulting crystal structure is mostly unpredictable due to highly dipolar molecular components with complex functional substituents. In this work, new organic salt crystals with top-level macroscopic optical nonlinearity by controlling the van der Waals volume (VvdW ), rather than by trial and error, are logically designed. When the VvdW of molecular ionic components varies, the corresponding crystal symmetry shows an observable trend: change from centrosymmetric to non-centrosymmetric and back to centrosymmetric. All non-centrosymmetric crystals exhibit an isomorphic P1 crystal structure with an excellent macroscopic second-order nonlinear optical response. Apart from the top-level macroscopic optical nonlinearity, new organic crystals introducing highly electronegative fluorinated substituents with strong secondary bonding ability show excellent performance in efficient and broadband THz wave generation, high crystal density, high thermal stability, and good bulk crystal growth ability.

Ultrafast formation of quantized interlayer vibrations in Bi2Se3 by photoinduced strain waves.

This study comprehensively investigated the coherent lattice dynamics in Bi2Se3 by ultrafast optical pump-probe spectroscopy with tunable near-infrared probe pulses. Sample-thickness- and probe-wavelength-dependent experiments revealed the key role of Bi2Se3 optical property in the generation and detection of photoinduced strain waves, whose confinement initiated coherent interlayer vibrations. Furthermore, the frequency and lifetime of the interlayer vibrations could be quantitatively explained with a modified linear chain and an acoustic mismatch model considering elastic coupling at sample-substrate interfaces. The results of this work provide insights for analyzing and interpreting, through ultrafast optical spectroscopy, nanomechanical interactions in layered materials.

Observation of spin-glass-like characteristics in ferrimagnetic TbCo through energy-level-selective approach.

Rare earth (RE)-transition metal (TM) ferrimagnetic alloys are gaining increasing attention because of their potential use in the field of antiferromagnetic spintronics. The moment from RE sub-lattice primarily originates from the 4f-electrons located far below the Fermi level (EF), and the moment from TM sub-lattice arises from the 3d-electrons across the EF. Therefore, the individual magnetic moment configurations at different energy levels must be explored to clarify the microscopic mechanism of antiferromagnetic spin dynamics. Considering these issues, here we investigate the energy-level-selective magnetic moment configuration in ferrimagnetic TbCo alloy. We reveal that magnetic moments at deeper energy levels are more easily altered by the external magnetic field than those near the EF. More importantly, we find that the magnetic moments at deeper energy levels exhibit a spin-glass-like characteristics such as slow dynamics and magnetic moment freezing whereas those at EF do not. These unique energy-level-dependent characteristics of RE-TM ferrimagnet may provide a better understanding of ferrimagnet, which could be useful in spintronic applications as well as in spin-glass studies.

Phonon-Suppressing Intermolecular Adhesives: Catechol-Based Broadband Organic THz Generators.

Solid-state molecular phonons play a crucial role in the performance of diverse photonic and optoelectronic devices. In this work, new organic terahertz (THz) generators based on a catechol group that acts as a phonon suppressing intermolecular adhesive are developed. The catechol group is widely used in mussel-inspired mechanical adhesive chemistry. Newly designed organic electro-optic crystals consist of catechol-based nonlinear optical 4-(3,4-dihydroxystyryl)-1-methylpyridinium (DHP) cations and 4-(trifluoromethyl)benzenesulfonate anions (TFS), which both have multiple interionic interaction capability. Interestingly, compared to benchmark organic crystals for THz generators, DHP-TFS crystals concomitantly achieve top level values of the lowest void volume and the highest crystal density, resulting in an exceptionally small amplitude of solid-state molecular phonons. Simultaneously achieving small molecular phonon amplitude, large optical nonlinearity and good phase matching at infrared optical pump wavelengths, DHP-TFS crystals are capable of generating broadband THz waves of up to 16 THz with high optical-to-THz conversion efficiency; one order of magnitude higher than commercial inorganic THz generators.

Coherent control of interlayer vibrations in Bi2Se3 van der Waals thin-films.

Interlayer vibrations with discrete quantized modes in two-dimensional (2D) materials can be excited by ultrafast light due to the inherent low dimensionality and van der Waals force as a restoring force. Controlling such interlayer vibrations in layered materials, which are closely related to fundamental nanomechanical interactions and thermal transport, in spatial- and time-domain provides an in-depth understanding of condensed matters and potential applications for advanced phononic and photonics devices. The manipulation of interlayer vibrational modes has been implemented in a spatial domain through material design to develop novel optoelectronic and phononic devices with various 2D materials, but such control in a time domain is still lacking. We present an all-optical method for controlling the interlayer vibrations in a highly precise manner with Bi2Se3 as a promising optoelectronic and thermoelasticity material in layered structures using a coherently controlled pump and probe scheme. The observed thickness-dependent fast interlayer breathing modes and substrate-induced slow interfacial modes can be exactly explained by a modified linear chain model including coupling effect with substrate. In addition, the results of coherent control experiments also agree with the simulation results based on the interference of interlayer vibrations. This investigation is universally applicable for diverse 2D materials and provides insight into the interlayer vibration-related dynamics and novel device implementation based on an ultrafast timescale interlayer-spacing modulation scheme.

SWCNT-SA mode-locked Tm,Ho:LCLNGG laser.

Sub-100 fs pulse generation from a passively mode-locked Tm,Ho-codoped cubic multicomponent disordered garnet laser at ∼2 µm is demonstrated. A single-walled carbon nanotube saturable absorber is implemented to initiate and stabilize the soliton mode-locking. The Tm,Ho:LCLNGG (lanthanum calcium lithium niobium gallium garnet) laser generated pulses as short as 63 fs at a central wavelength of 2072.7 nm with an average output power of 63 mW at a pulse repetition rate of ∼102.5 MHz. Higher average output power of 121 mW was obtained at the expense of longer pulse duration (96 fs) at 2067.6 nm using higher output coupling. To the best of our knowledge, this is the first report on mode-locked operation of the Tm,Ho:LCLNGG crystal.

Real-time ultrafast oscilloscope with a relativistic electron bunch train.

The deflection of charged particles is an intuitive way to visualize an electromagnetic oscillation of coherent light. Here, we present a real-time ultrafast oscilloscope for time-frozen visualization of a terahertz (THz) optical wave by probing light-driven motion of relativistic electrons. We found the unique condition of subwavelength metal slit waveguide for preserving the distortion-free optical waveform during its propagation. Momentary stamping of the wave, transversely travelling inside a metal slit, on an ultrashort wide electron bunch enables the single-shot recording of an ultrafast optical waveform. As a proof-of-concept experiment, we successfully demonstrated to capture the entire field oscillation of a THz pulse with a sampling rate of 75.7 TS/s. Owing to the use of transversely-wide and longitudinally-short electron bunch and transversely travelling wave, the proposed "single-shot oscilloscope" will open up new avenue for developing the real-time petahertz (PHz) metrology.

Sub-100 fs mode-locked Tm:CLTGG laser.

We report on the first sub-100 fs mode-locked laser operation of a Tm3+-doped disordered calcium lithium tantalum gallium garnet (Tm:CLTGG) crystal. Soliton mode-locking was initiated and stabilized by a transmission-type single-walled carbon nanotube saturable absorber. Pulses as short as 69 fs were achieved at a central wavelength of 2010.4 nm with an average power of 28 mW at a pulse repetition rate of ∼87.7 MHz. In the sub-100 fs regime, the maximum average output power amounted to 103 mW.

Interlayer Coupling and Ultrafast Hot Electron Transfer Dynamics in Metallic VSe2/Graphene van der Waals Heterostructures.

Atomically thin vanadium diselenide (VSe2) is a two-dimensional transition metal dichalcogenide exhibiting attractive properties due to its metallic 1T phase. With the recent development of methods to manufacture high-quality monolayer VSe2 on van der Waals materials, the outstanding properties of VSe2-based heterostructures have been widely studied for diverse applications. Dimensional reduction and interlayer coupling with a van der Waals substrate lead to its distinguishable characteristics from its bulk counterparts. However, only a few fundamental studies have investigated the interlayer coupling effects and hot electron transfer dynamics in VSe2 heterostructures. In this work, we reveal ultrafast and efficient interlayer hot electron transfer and interlayer coupling effects in VSe2/graphene heterostructures. Femtosecond time-resolved reflectivity measurements showed that hot electrons in VSe2 were transferred to graphene within a 100 fs time scale with high efficiency. Besides, coherent acoustic phonon dynamics indicated interlayer coupling in VSe2/graphene heterostructures and efficient thermal energy transfer to three-dimensional substrates. Our results provide valuable insights into the intriguing properties of metallic transition metal dichalcogenide heterostructures and motivate designing optoelectronic and photonic devices with tailored properties.

Efficient perovskite solar cells via improved carrier management.

Metal halide perovskite solar cells (PSCs) are an emerging photovoltaic technology with the potential to disrupt the mature silicon solar cell market. Great improvements in device performance over the past few years, thanks to the development of fabrication protocols1-3, chemical compositions4,5 and phase stabilization methods6-10, have made PSCs one of the most efficient and low-cost solution-processable photovoltaic technologies. However, the light-harvesting performance of these devices is still limited by excessive charge carrier recombination. Despite much effort, the performance of the best-performing PSCs is capped by relatively low fill factors and high open-circuit voltage deficits (the radiative open-circuit voltage limit minus the high open-circuit voltage)11. Improvements in charge carrier management, which is closely tied to the fill factor and the open-circuit voltage, thus provide a path towards increasing the device performance of PSCs, and reaching their theoretical efficiency limit12. Here we report a holistic approach to improving the performance of PSCs through enhanced charge carrier management. First, we develop an electron transport layer with an ideal film coverage, thickness and composition by tuning the chemical bath deposition of tin dioxide (SnO2). Second, we decouple the passivation strategy between the bulk and the interface, leading to improved properties, while minimizing the bandgap penalty. In forward bias, our devices exhibit an electroluminescence external quantum efficiency of up to 17.2 per cent and an electroluminescence energy conversion efficiency of up to 21.6 per cent. As solar cells, they achieve a certified power conversion efficiency of 25.2 per cent, corresponding to 80.5 per cent of the thermodynamic limit of its bandgap.

Non-resonant power-efficient directional Nd:YAG ceramic laser using a scattering cavity.

Non-resonant lasers exhibit the potential for stable and consistent narrowband light sources. Furthermore, non-resonant lasers do not require well-defined optics, and thus has considerably diversified the available types of laser gain materials including powders, films, and turbid ceramics. Despite these intrinsic advantages, the practical applications of non-resonant lasers have been limited so far, mainly because of their low power efficiency and omnidirectional emission. To overcome these limitations, here we propose a light trap design for non-resonant lasers based on a spherical scattering cavity with a small entrance. Using a porous Nd3+:YAG ceramic, directional laser emission could be observed with significant enhancements in the slope efficiency and linewidth (down to 32 pm). A theoretical model is also developed to describe and predict the operation characteristics of proposed non-resonant laser.

Single-walled carbon-nanotube saturable absorber assisted Kerr-lens mode-locked Tm:MgWO4 laser.

We demonstrate sub-100-fs Kerr-lens mode-locking of a Tm:MgWO4 laser emitting at ∼2µm assisted by a single-walled carbon-nanotube saturable absorber. A maximum average output power of 100 mW is achieved with pulse duration of 89 fs at a pulse repetition rate of ∼86MHz. The shortest pulse duration derived from frequency-resolved optical gating amounts to 76 fs at 2037 nm, corresponding to nearly bandwidth-limited pulses. To the best of our knowledge, these are the shortest pulses generated from any Tm-doped tungstate crystal and the first report on saturable absorber assisted Kerr-lens mode-locking of a Tm laser at ∼2µm.

Organic Broadband THz Generators Optimized for Efficient Near-Infrared Optical Pumping.

New organic THz generators are designed herein by molecular engineering of the refractive index, phonon mode, and spatial asymmetry. These benzothiazolium crystals simultaneously satisfy the crucial requirements for efficient THz wave generation, including having nonlinear optical chromophores with parallel alignment that provide large optical nonlinearity; good phase matching for enhancing the THz generation efficiency in the near-infrared region; strong intermolecular interactions that provide restraining THz self-absorption; high solubility that promotes good crystal growth ability; and a plate-like crystal morphology with excellent optical quality. Consequently, the as-grown benzothiazolium crystals exhibit excellent characteristics for THz wave generation, particularly at near-infrared pump wavelengths around 1100 nm, which is very promising given the availability of femtosecond laser sources at this wavelength, where current conventional THz generators deliver relatively low optical-to-THz conversion efficiencies. Compared to a 1.0-mm-thick ZnTe crystal as an inorganic benchmark, the 0.28-mm-thick benzothiazolium crystal yields a 19 times higher peak-to-peak THz electric field with a broader spectral bandwidth (>6.5 THz) when pumped at 1140 nm. The present work provides a valuable approach toward realizing organic crystals that can be pumped by near-infrared sources for efficient THz wave generation.

Spectroscopy and diode-pumped laser operation of transparent Tm:Lu3Al5O12 ceramics produced by solid-state sintering.

A transparent Tm:Lu3Al5O12 ceramic is fabricated by solid-state reactive sintering at 1830 °C for 30 h using commercial α-Al2O3 and Lu2O3/Tm2O3 powders and sintering aids - MgO and TEOS. The ceramic belongs to the cubic system and exhibits a close-packed structure (mean grain size: 21 µm). The in-line transmission at ∼1 µm is 82.6%, close to the theoretical limit. The spectroscopic properties of the ceramic are studied in detail. The maximum stimulated-emission cross-section is 2.37×10-21 cm2 at 1749nm and the radiative lifetime of the 3F4 state is about 10 ms. The modified Judd-Ofelt theory accounting for configuration interaction is applied to determine the transition probabilities of Tm3+, yielding the intensity parameters Ω2 = 2.507, Ω4 = 1.236, Ω6 = 1.340 [10-20 cm2] and α = 0.196×10-4 cm. The effect of excited configurations on lower-lying interconnected states with the same J quantum number is discussed. First laser operation is achieved under diode-pumping at 792 nm. A 4 at.% Tm:Lu3Al5O12 ceramic laser generated 3.12 W at 2022-2035nm with a slope efficiency of 60.2%. The ceramic is promising for multi-watt lasers at >2 µm.

Transition of pulsed operation from Q-switching to continuous-wave mode-locking in a Yb:KLuW waveguide laser.

We report on the diverse pulsed operation regimes of a femtosecond-laser-written Yb:KLuW channel waveguide laser emitting near 1040 nm. By the precise position tuning of a carbon-nanotube-coated saturable absorber (SA) mirror, the transition of the pulsed operation from Q-switching, Q-switched mode-locking and finally sub-GHz continuous-wave mode-locking are obtained based on the interplay of dispersion and mode area control. The Q-switched pulses exhibit typical fast SA Q-switched pulse characteristics depending on absorbed pump powers. In the Q-switched mode-locking, amplitude modulations of the mode-locked pulses on the Q-switched envelope are observed. The radio-frequency spectrum represents the coexistence of Q-switching and mode-locking signals. In the purely mode-locked operation, the waveguide laser generates 2.05-ps pulses at 0.5 GHz.

MHz-repetition-rate, sub-mW, multi-octave THz wave generation in HMQ-TMS.

We demonstrate the first megahertz (MHz) repetition-rate, broadband terahertz (THz) source based on optical rectification in the organic crystal HMQ-TMS driven by a femtosecond Yb:fibre laser. Pumping at 1035 nm with 30 fs pulses, we achieve few-cycle THz emission with a smooth multi-octave spectrum that extends up to 6 THz at -30 dB, with conversion efficiencies reaching 10-4 and an average output power of up to 0.38 mW. We assess the thermal damage limit of the crystal and conclude a maximum fluence of ∼1.8 mJ·cm-2 at 10 MHz with a 1/e2 pump beam diameter of 0.10 mm. We compare the performance of HMQ-TMS with the prototypical inorganic crystal gallium phosphide (GaP), yielding a tenfold electric field increase with a peak on-axis field strength of 7 kV·cm-1 and almost double the THz bandwidth. Our results further demonstrate the suitability of organic crystals in combination with fibre lasers for repetition-rate scaling of broadband, high-power THz sources for time-domain spectroscopic applications.

Laser-micromachined zebra-patterned graphene as a mode locker with adjustable loss.

In this Letter, we describe a novel, to the best of our knowledge, device based on micro-structured graphene, referred to as zebra-patterned graphene saturable absorber (ZeGSA), which can be used as a saturable absorber with adjustable loss to initiate femtosecond pulse generation. Femtosecond laser micro-machining was employed to ablate monolayer graphene on an infrasil substrate in the form of stripes with a different duty cycle, resulting in the formation of regions with variable insertion loss in the 0.21%-3.12% range. The mode-locking performance of the device was successfully tested using a ${{\rm Cr}^{4 {+} }}{:}\,{\rm forsterite}$Cr4+:forsterite laser, operating near 1250 nm. In comparison with mode locking using non-ablated graphene, the ZeGSA device with regions of decreasing graphene, enabled improved power performance where the mode-locked output power increased from 68 mW to 114 mW, and the corresponding pulse duration decreased from 62 to 48 fs at the same incident pump power of 6.3 W. These experiments indicate that ZeGSA shows great potential as a laser mode locker with adjustable loss and that it should find applications in the development of femtosecond lasers over a broad spectral range.

Graphene mode-locked operation of Tm3+:YLiF4 and Tm3+:KY3F10 lasers near 2.3 µm.

We report experimental demonstration of graphene mode-locked operation of ${{\rm Tm}^{3 + }}\!:\!{{\rm YLiF}_4}$Tm3+:YLiF4 (YLF) and ${{\rm Tm}^{3 + }}\!:\!{{\rm KY}_3}{{\rm F}_{10}}$Tm3+:KY3F10 (KYF) lasers near 2.3 µm. To scale up the intracavity pulse energy, the cavity was extended, and double-end pumping was employed with a continuous-wave, tunable ${{\rm Ti}^{3 + }}\!:\!{\rm sapphire}$Ti3+:sapphire laser delivering up to 1 W near 780 nm. The extended ${{\rm Tm}^{3 + }}\!:\!{\rm KYF}$Tm3+:KYF laser cavity was purged with dry nitrogen to eliminate pulsing instabilities due to atmospheric absorption lines, but this was not needed in the case of the ${{\rm Tm}^{3 + }}\!:\!{\rm YLF}$Tm3+:YLF laser. Once initiated by graphene, stable uninterrupted mode-locked operation could be maintained with both lasers. With the extended cavity ${{\rm Tm}^{3 + }}\!:\!{\rm YLF}$Tm3+:YLF laser, 921 fs pulses were generated at a repetition rate of 17.2 MHz at 2304 nm. 739 fs pulses were obtained at the repetition rate of 54 MHz from the ${{\rm Tm}^{3 + }}\!:\!{\rm KYF}$Tm3+:KYF laser at 2340 nm. The corresponding pulse energy and peak power were 2.4 nJ and 2.6 kW for the ${{\rm Tm}^{3 + }}\!:\!{\rm YLF}$Tm3+:YLF laser, and 1.2 nJ and 1.6 kW for the ${{\rm Tm}^{3 + }}\!:\!{\rm KYF}$Tm3+:KYF laser. We foresee that it should be possible to generate shorter pulses at higher pump levels.

Measurement of bending-induced birefringence in a hollow-core photonic crystal fiber.

We report the measurement of bending-induced birefringence in the presence of large intrinsic birefringence in a hollow-core photonic crystal fiber (HC-PCF). The fast axis of bending-induced birefringence was found to be normal to the bending plane, in contrast to the conventional fiber case. The dependence of the induced birefringence on the bending radius was also different from the typical inverse square law. Possibilities and design criteria for polarization controllers using bending-induced birefringence in HC-PCFs are presented.