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A temporal boundary refers to a specific time at which the properties of an optical medium are abruptly changed. When light interacts with the temporal boundary, its spectral content can be redistributed due to the breaking of continuous time-translational symmetry of the medium where light resides. In this work, we use this principle to demonstrate, at terahertz (THz) frequencies, the resonance-enhanced spectral funneling of light coupled to a Fabry–Perot resonator with a temporal boundary mirror. To produce a temporal boundary effect, we abruptly increase the reflectance of a mirror constituting the Fabry–Perot resonator and, correspondingly, its quality factor in a step-like manner. The abrupt increase in the mirror reflectance leads to a trimming of the coupled THz pulse that causes the pulse to broaden in the spectral domain. Through this dynamic resonant process, the spectral contents of the input THz pulse are redistributed into the modal frequencies of the high-Q Fabry–Perot resonator formed after the temporal boundary. An energy conversion efficiency of up to 33% was recorded for funneling into the fundamental mode with a Fabry–Perot resonator exhibiting a sudden Q-factor change from 4.8 to 48. We anticipate that the proposed resonance-enhanced spectral funneling technique could be further utilized in the development of efficient mechanically tunable narrowband terahertz sources for diverse applications.

Generating high stability ultrafast pulse laser using constituents of the most powerful biomolecules in nature (Adenine, Guanine, Cytosine, and Thymine).

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., A travelling wave inside a metal slit can reveal its own waveform by probing deflecting motions of charged particles. Here, a real-time THz oscilloscope was demonstrated by utilizing the relativistic electrons and the subwavelength slit waveguide.

This study comprehensively investigated the coherent lattice dynamics in Bi

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.

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.

In this study, an organic nonlinear optical salt crystal, 4-(4-methoxystyryl)-1-methylpyridinium 4-bromobenzenesulfonate (MOS-BBS), is newly reported. MOS-BBS crystals exhibit perfectly parallel molecular ordering of 4-(4-methoxystyryl)-1-methylpyridinium (MOS) cationic chromophores with noncentrosymmetric P1 space group symmetry, which provides an optimal configuration for maximizing the macroscopic second-order optical nonlinearity. The macroscopic optical nonlinearity of the MOS-BBS crystals is very large, with the diagonal effective first hyperpolarizability of 160 × 10−30 esu. Furthermore, the MOS-BBS crystals exhibit a high thermal crystal-phase stability. The lowest phase transition temperature of the MOS-BBS crystals is 265°C, which is ~90°C higher than that of previously reported MOS-based crystals.

Controllable graphene Q-switching in an Yb:YAG fs-laser-written beam-splitter-type waveguide laser is demonstrated by tunable beam-splitting ratio and varying pump power. Desired channels are regulated to generate Q-switched pulses separately or simultaneously with a single pumping.

Long-wave multiphonon-assisted emission of rare-earth ions provides broadband gain which is essential for the generation of few-optical-cycle pulses. A phonon-terminated Kerr-lens mode-locked Tm,Ho:CALGO laser generates 37-fs pulses with an ultrabroadband spectrum (1870 - 2337 nm).

We report on a Kerr-lens mode-locked Tm,Ho:CALGO laser delivering 46-fs pulses at ~2.06 μm with an average power of 110 mW. The maximum average power reached 423 mW for a pulse duration of 53 fs.

Stroboscopic visualization of nuclear or electron dynamics in atoms, molecules or solids requires ultrafast pump and probe pulses and a close to perfect synchronization between the two. We have developed a 3 MeV ultrafast electron diffraction (UED) probe technology that nominally reduces the electron bunch duration and the arrival time jitter to the subfemtosecond level. This simple configuration uses a radiofrequency photogun and a 90° achromatic bend and is designed to provide effectively jitter-free conditions. Terahertz streaking measurements reveal an electron bunch duration of 25 fs, even for a charge as high as 0.6 pC, and an arrival time jitter of 7.8 fs, the latter limited by only the measurement accuracy. From pump–probe measurements of photoexcited bismuth films, the instrument response function was determined to be 31 fs. This pioneering jitter-free technique paves the way towards UED of attosecond phenomena in atomic, molecular and solid-state dynamics. An ultrafast electron diffraction facility with an overall temporal resolution of 31 fs root mean square is developed. Even for a charge as high as 0.6 pC, the electron bunch duration and timing jitter are 25 fs and less than 10 fs, respectively.

We report a new π-conjugated cationic chromophore based on phenolic N-pyrimidinyl stilbazolium and its corresponding non-centrosymmetric crystals. The new cationic chromophore, HPR (4-(4-hydroxy-3-methoxystyryl)-1-(pyrimidin-2-yl)pyridin-1-ium), consists of a strong electron donor, the 4-hydroxy-3-methoxyphenyl group based on two electron-donating groups, and a strong electron acceptor, the N-pyrimidinyl pyridinium group based on two electron-withdrawing groups. The HPR chromophore possesses large molecular optical nonlinearity with first hyperpolarizability of up to 264 × 10−30 esu, which is significantly larger than that of the benchmark stilbazolium chromophores. In solution, the HPR chromophore showed co-existence of phenol- and phenolate-like forms with two absorption bands (∼460 and ∼610 nm, respectively). In the crystalline state, all HPR-based derivatives with three different counter anions, N2S (naphthalene-2-sulfonate), VBS (4-vinylbenzenesulfonate), and NBS (3-nitrobenzenesulfonate), exhibit a macroscopic second-order nonlinear optical response. HPR-N2S crystals exhibit non-centrosymmetric monoclinic Pn space group symmetry and large off-diagonal effective macroscopic optical nonlinearity (94 × 10−30 esu), which is approximately four times higher than that of the benchmark stilbazolium crystals. Therefore, the newly developed HPR-based crystals are highly promising materials for second-order nonlinear optical applications.

International audience; 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.

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 Bi

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.

We demonstrate multi-gigahertz continuous-wave mode-locking of a Yb:KLuW waveguide laser. A femtosecond-laser-inscribed Yb:KLuW channel waveguide in an extended laser cavity delivers a fundamentally mode-locked laser near 1030 nm. A tunable few-centimeter-long cavity containing a single-walled carbon nanotube saturable absorber as mode-locker generates self-starting femtosecond pulses with average output powers exceeding 210 mW at repetition rates of 2.27, 2.69, and 3.55 GHz. The laser cavity, which includes a wedged waveguide, is extended by using a lens pair that controls the laser fluence on the saturable absorber for reliable mode-locked operation without instability. The presented laser performance, mode-locked up to 3.55 GHz, highly suggests the potential of crystalline Yb:KLuW waveguides for realizing high-power ultrafast lasers with higher GHz repetition rates in a quasi-monolithic cavity.

This work reports a series of new organic electro-optic salt crystals possessing unusual orthogonal dipole-coupling assembly that act as dimple-free THz generators. In the new crystals, optically anisotropic aromatic anions introducing highly electronegative fluorinated substituents are orthogonally assembled with optically anisotropic nonlinear optical benzothiazolium cations. These orthogonal cation–anion assembled crystals exhibit strong suppression of intrinsic THz phonon modes along the polar axis, which results in a wide THz absorption-free range from 1.5 to 4.0 THz without substantial absorption peaks. This is sharply in contrast to previous benchmark crystals with parallel cation–anion assembly; for example, in analogous crystals, several strong absorption peaks appear in this frequency range. This absence of strong absorption peaks is attributed to the orthogonal cation–anion dipole coupling assembly, the formation of fluorinate-induced strong interionic interactions, and a high packing ability of uniaxial anions. With top-level macroscopic optical nonlinearity, new orthogonal-dipole assembled crystals make dimple-free THz wave generation possible in the range of about 1.5–4.0 THz, which is very beneficial for characterizing signature peaks related to molecular phonon motions of analytes in THz spectroscopy. Therefore, orthogonal molecular assembly of optically highly anisotropic molecules provides an efficient way to substantially reduce and control intrinsic THz phonon modes.

Supercontinuum generation (SCG) is an attractive method to generate broadband optical sources in that it covers more than hundreds of nm bandwidths. In virtue of the advances in nanoscale designs of the nonlinear waveguides, their spectral coverages are allowed in ultraviolet (UV) to mid-infrared (MIR) regions and their bandwidths also extended more than 1 octaves. Since the ro-vibrational bands of the many sorts of gases reside in the infrared regions, there have been advances in absorption spectroscopies, which were demonstrated by transmitting SCG into gas cells [1] , [2] . To extract absorption data of specific gas molecules, it is essential to subtract background signals such as the envelope of the SCG and the effect of optical components, from the cell-transmitted signal. Extra measurement of N 2 cell transmission, linear fitting, and polynomial fitting have been implemented for it. Here, by applying an appropriate high-pass filter, we achieved a clear distinction of the absorption band of CO gas from the SCG transmitted through 400 Torr, 121 mm CO gas cell.

Next-generation solar cells, such as dye-sensitized solar cells (DSSCs) and perovskite solar cells (PSCs), are fabricated in a configuration where light absorbers are located between the electron transporting layer (ETL) and the hole transporting layer (HTM). Although the most efficient DSSCs and PSCs have been fabricated using TiO2 as the ETL, TiO2 exhibits inherently low electron mobility with difficulty controlling the energy levels (i.e., conduction and valence bands) as it possesses a single phase of two components. Here, we report the synthesis of Sr-substituted BaSnO3 (BSSO) by a low-temperature solution process as a new alternative to TiO2 for both PSCs and DSSCs. The energy-level tailoring by Sr incorporation into BaSnO3 minimizes the open-circuit voltage (VOC) loss at the interfaces of ETL/perovskite and ETL/electrolyte in the PSCs and DSSCs, thereby leading to an improved VOC from 0.65 to 0.72 V in DSSC and 1.07 to 1.13 V in PSCs. Additionally, the BSSO ETL-based PSC shows improved photostability compared to the TiO2 analog. Our results show that energy-level tuned BSSO can be applied as a universal ETL for improving efficiency in both PSCs and DSSCs.

We demonstrate diverse pulsed operation regimes adjustable from Q-switching to sub-GHz continuous-wave mode-locking in a Yb:KLuW channel waveguide laser based on the interplay of dispersion and mode area managements.

We report on a power-scalable sub-100-fs laser in the 2-μm spectral range using a Tm3+-doped ‘mixed’ (Lu,Sc)2O3 sesquioxide ceramic as an active medium. Pulses as short as 58 fs at 2076 nm with an average output power of 114 mW at a pulse repetition rate of approximately 82.9 MHz are generated by employing single-walled carbon nanotubes as a saturable absorber. A higher average power of 350 mW at 2075 nm is obtained at the expense of the pulse duration (65 fs). A maximum average power of 486 mW is achieved for a pulse duration of 98 fs and an optical conversion efficiency of 22.3%, representing the highest value ever reported from sub-100-fs mode-locked Tm lasers.

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 VSe 2 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 VSe 2 were transferred to graphene within a 100-fs timescale 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., Comment: 30 pages, 5 figures, supplementary information(7 pages, 5 figures)

Organic π-conjugated crystals with second-order optical nonlinearity are considerably attractive materials for diverse terahertz (THz) wave photonics. An overview of the research of organic nonlinear optical (NLO) crystals for THz wave generation, detection, and applications is provided here. First, the status of organic NLO crystals compared to other alternative THz materials is described. Second, the basic theory and requirements for organic THz generators and detectors are explained. Third, with a primary focus on the organic NLO crystals that have been developed during the last decade, various molecular engineering approaches are discussed from the perspective of THz photonics. Finally, various types of high-power broadband coherent THz sources and their applications in THz nonlinear optics are discussed.

We report on the first passively mode-locked Tm3+-doped calcium tantalum gallium garnet laser generating 69-fs pulses at 2010.4 nm with an average power of 28 mW at a pulse repetition rate of ~87.7 MHz.

We demonstrate sub-100-fs Kerr-lens mode-locking of a

We demonstrate 1.4 milliwatt average power, broadband terahertz generation extending up to 6 THz at 10 MHz repetition rate through optical rectification in the organic crystal HMQ-TMS. The pump source is based on a simple external pulse compression scheme for the generation of ultra-short pulses using compact Yb:fiber laser technology.

We present an overview of our recent achievements on fabrication, characterization and CW and passively Q-switched laser operation of Thulium and Holmium depressed-cladding waveguide lasers operating at ~2 μm and inscribed in anisotropic crystals by femtosecond direct laser writing. Variable waveguide geometries (buried and surface guides; circular, rectangular and hexagonal channels; Y-splitters) are described.

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., Organic crystals, which are designed through molecular engineering of the refractive index, phonon mode, and spatial asymmetry, simultaneously satisfy the crucial requirements for efficient and broadband THz wave generation, particularly at near‐infrared pump wavelengths near 1100 nm.

A transparent Tm:Lu

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., National Research Foundation of Korea (2018H1A2AA1061480, 2019R1A2C3003504, 2020R1A4A2002828); Spanish Government (FIS2017-87970-R, MAT2016-75716-C2-1-R (AEI/FEDER,UE)); Junta de Castilla y León (SA287P18); Generalitat de Catalunya (2017SGR755).

We report new organic nonlinear optical salt crystals comprising bis(head-to-tail) complementary cation–anion assembly that results in extremely efficient THz wave generation. In the new salt crystals, each of the ends of the molecular anion, 4-(trifluoromethyl)benzenesulfonate, possesses bis(hydrogen-bond acceptors), while each of the ends of the nonlinear optical molecular cationic chromophore, 2-(4-(4-(hydroxymethyl)piperidin-1-yl)styryl)-3-methylbenzothiazol-3-ium, possesses bis(hydrogen-bond donors). The resulting assembly fulfills the requirements for efficient broadband THz wave generation, namely, perfectly parallel alignment of the nonlinear optical cationic chromophores for maximizing the optical nonlinearity as well as strong interionic binding interactions for reducing self-absorption of the generated THz waves. The new benzothiazolium crystals provide extremely high optical-to-THz conversion efficiency with a broad THz spectral bandwidth of 8 THz, where the peak-to-peak THz electric field amplitude is 36 times higher than that of the benchmark inorganic 1.0 mm-thick ZnTe crystal when pumped at 1300 nm and also notably higher than those of benchmark organic analogous crystals.

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.

Interlayer coupling in van der Waals heterostructures exhibits unique physical properties and presents a new pathway for diverse applications in materials science and photonics. Interestingly, photo-responsivity of graphene with semiconducting transition metal dichalcogenide (TMD) can be enhanced in the UV-visible range by interlayer charge/energy transfer. However, such an effect has been studied only for semiconducting materials. In this work, we will discuss ultrafast hot-electron transfer in atomically thin metallic-layer VSe2/graphene heterostructures investigated by time-resolved pump-probe spectroscopy. Our experimental finding extends the concepts of conventional two-dimensional heterostructures to metallic-layer and can provide a new degree of freedom for designing novel functionalized materials and devices.