Search

External electric fields can be used to manipulate the electronic properties of two-dimensional (2D) materials. 2D InSe semiconductors possess high electron mobility and wide band gap tunability. Therefore, they have been proposed for use in ultrathin electronic devices. Here, using first-principles calculations, we study the charge polarization, structure, electronic structure, and gas adsorption of an InSe monolayer under vertical electric fields. We find that both the structural evolution and charge polarization rely on the directions of the electric fields. The hole effective mass at the valance band maximum can be decreased by fields that offer a possible route to increase mobility. In contrast, the fields have little impact on the effective mass of electrons at the conduction band minimum. Therefore, high electron mobility in InSe is retained under the fields. Besides, electric fields could alter the absorption intensity for gas molecules. Therefore, gas sensors could be an expected application. More importantly, this work systematically points out some key steps for setting up electric-field calculations in the popular VASP code, such as the cancellation of the symmetrisation of the charge density, avoiding electrons spilling out into the vacuum under high fields. [ABSTRACT FROM AUTHOR]

Femtosecond lasers (fs) can cause a disparity between electronic and lattice temperatures in the very short period after irradiation. In this relatively cool lattice regime, the material properties can differ drastically from those under thermal equilibrium. In particular, first-principles calculations reveal two general mechanical effects on semiconductors. Firstly, the excitation can induce a negative pressure on the lattice, causing a ＞10% expansion, even for superhard diamond. Secondly, it induces inhomogeneous local forces on the atoms, for both perfect and distorted lattices. In the case of phase-change-memory for Ge2Sb2Te5 and GeTe alloys, such random forces cause a simultaneous phase transition from crystalline to amorphous, which enables faster data writing. These excitation effects are further supported by the time-dependent density functional theory. This work could be an important step in advancing fs laser techniques for the atomic-level control of structures, rather than relying on traditional melting or ablation approaches which often apply to much larger and non-atomic scales. [ABSTRACT FROM AUTHOR]

In the past few years, organometal halide light-emitting perovskite thin films and colloidal nanocrystals (NCs) have attracted significant research interest in the field of highly purified illuminating applications. However, knowledge of photoluminescence (PL) characteristics, such as amplified spontaneous emission (ASE) of larger-sized perovskite crystals, is still relatively scarce. Here, we presented room-temperature size-dependent spontaneous emission (SE) and ASE of the organometal halide CH3NH3PbBr3 perovskite cubic microcrystals pumped through one-photon-(1P) and two-photon-(2P) excitation paradigms. The results showed that the optical properties of SE and ASE were sensitively dependent on the sizes of perovskite microcrystals irrespective of whether 1P or 2P excitation was used. Moreover, by comparing the spectral results of 1P- and 2P-pumped experiments, 2P pumping was found to be an effective paradigm to reduce thresholds by one order of magnitude. Finally, we carried out fluences-dependent time-resolved fluorescence dynamics experiments to study the underlying effects of these scale-dependent SE and ASE. We found that the photoluminescence (PL) recombination rates sensitively became faster with increasing carriers’ densities, and that the ASE pumped from larger-sized CH3NH3PbBr3 perovskite cubic microcrystals showed faster lifetimes. This work shows that micro-sized perovskite cubic crystals could be the ideal patterns of perovskite materials for realizing ASE applications in the future. [ABSTRACT FROM AUTHOR]

Recently, all-inorganic cesium lead halide perovskites (CsPbX3) quantum dots (QDs) have attracted great attention due to their halogen composition and size tunable band gap engineering, the same physical mechanism that is responsible for excellent performance in light-emitting devices. However, little is known about the time-resolved fluorescence quenching dynamics process of these CsPbX3 QDs. In this article, we present comprehensive contrastive spectral studies on the electron and hole extraction dynamics of CsPbX3 colloidal QDs with and without quencher by time-resolved femtosecond transient absorption (TA) and time-correlated single-photon counting (TCSPC) spectroscopy methods. We have identified that the partial electrons of the conduction band and holes of the valence band of CsPbX3 QDs can be directly extracted by tetracyanoethylene (TCNE) and phenothiazine (PTZ), respectively. Moreover, compared with the CsPbBr3 QDs, the CsPbI3 QDs showed relatively slower charge extraction rates. We also found that the CsPbBr3 QDs with smaller size showed faster carrier recombination rates and photoluminescence (PL) decay lifetime due to the relatively stronger quantum confinement effects. We believe that this study may be useful for realising optimal applications in photovoltaic and light emission devices. [ABSTRACT FROM AUTHOR]

CH3NH3PbI3−xClx perovskite material has been commonly used as the free charge generator and reservoir in highly efficient perovskite-based solid-state solar photovoltaic devices. However, many of the underlying fundamental photophysical mechanisms in this material such as the perovskite transition band structure as well as the dependent relationship between the carrier properties and lattice properties still lack sufficient understanding. Here, we elucidated the fundamental band structure of the pure CH3NH3PbI3−xClx pervoskite lattice, and then reported about the dependent relationship between the free charge carrier characteristic and the different CH3NH3PbI3−xClx pervoskite lattice thin films utilizing femtosecond time-resolved pump–probe technologies. The data demonstrated that the pure perovskite crystal band structure should only have one conduction and one valence band rather than dual valences, and the pure perovskite lattice could trigger more free charge carriers with a slower recombination rate under an identical pump intensity compared with the impurities doped perovskite crystal. We also investigated the perovskite film performance when exposed to moisture and water, the corresponding results gave us a dip in the optimization of the performance of perovskite based devices, and so as a priority this material should be isolated from moisture (water). This work may propose a deeper perspective on the comprehension for this material and it is useful for future optimization of applications in photovoltaic and light emission devices. [ABSTRACT FROM AUTHOR]

Reported here is the fabrication of solvent-tunable polydimethylsiloxane (PDMS) microlenses using the femtosecond laser direct writing (FsLDW) technique. PDMS microlenses with equation-defined profiles, including both spherical microlens and aspheric hyperboloid microlens, have been fabricated according to preprogrammed models. In addition to excellent optical performance derived from the high accuracy and smooth surface, the resultant PDMS microlenses also show unique solvent-tunable properties; the focal length could be dynamically tuned by organic solvents of different solubility parameters. To obtain better control over the tunable property, a PDMS microlens has been flexibly integrated with a microfluidic device. Under the stimulation of different solvents, its tunable imaging performance has been demonstrated in a controlled manner. [ABSTRACT FROM AUTHOR]

The excited state relaxation of two types of azobenzene derivative excited at 350 nm in the short-wavelength (S2(π, π*)) band was studied by transient absorption spectroscopy. We compared the relaxation dynamics and the time-resolved anisotropic relaxation properties of these two molecules in liquid solution and in bulk film. The average relaxation life-time for Azo-2 in bulk film (13.2 ps) is much slower than that of Azo-2 (4.06 ps) and Azo-1(1.31 ps) in liquid solution. The time-resolved polarization anisotropy spectroscopy measurements of these samples also showed significant differences. The value of anisotropy for Azo-2 remained almost constant at about 0.2 in bulk film but decayed slowly from 0.3 in liquid solution. The value for Azo-1 in liquid solution decayed very fast from 0.4 to 0.2 within 6 ps. Our results gave new evidence for the existence of a converted inversion channel. We also concluded that the concerted inversion process and the conventional rotation process govern the relaxation for the photon-induced switches of azobenzene and its derivatives under short-wavelength band excitation. [ABSTRACT FROM AUTHOR]

Reported here is the programmable assembly of CdTe quantum dots (QDs) into various pre-designed microstructures by using a femtosecond laser direct writing (FsLDW) technique. As nanobuilding blocks, CdTe QDs could be driven by a focused femtosecond laser beam to construct arbitrarily-shaped micropatterns with high resolution (∼170 nm). The optical properties of pristine CdTe QDs were well inherited after the FsLDW induced programmable assembly, which has been confirmed by the luminescence spectrum and the high resolution transmission electron microscope (HR-TEM) image of the assemblies. By using this technique, the CdTe QDs microstructures were integrated within microfluidic devices, which showed the capability of qualitative on-chip detection of heavy metal ions. The FsLDW induced assembly of QDs may open up a new way for the designable assembly of QDs towards the flexible fabrication and integration of QDs-based microdevices. [ABSTRACT FROM AUTHOR]

A novel solvent responsive polymer micromachine has been successfully fabricated by two-photon photopolymerization (TPP) of methacrylate-based photoresists. The moving part of the micromachine could be easily driven by interfacial solvent polarity induced swelling and shrinking of the photopolymer networks. Furthermore, the driving performance of the micromachine could be precisely modulated by varying the laser scanning step length during fabrication. [ABSTRACT FROM AUTHOR]

Microfluidic researches are now resorting to advanced micro-nanoprocessing technologies for production of more functional “lab-on-a-chip” systems. However, two-photon polymerization (TPP), a powerful designable micro-nanofabrication approach, has not been put to use on the exciting field, largely due to the difficulties in forming buried channels. Here, we solve the problem by TPP prototyping of nanoshells, for which the usage of the negative tone resin SU-8 is found critical. The fabrication efficiency improved by orders of magnitude, together with the prospect of integration of movable micro-mechanical and optical components into the chip would make TPP a promising enabling tool for the micro-analytical systems. Finally, a 25 μm length functional microvalve in a microfluidic channel was rapidly realized and its “ON” and “OFF” states were tested. [ABSTRACT FROM AUTHOR]

In the past few years, organometal halide light-emitting perovskite thin films and colloidal nanocrystals (NCs) have attracted significant research interest in the field of highly purified illuminating applications. However, knowledge of photoluminescence (PL) characteristics, such as amplified spontaneous emission (ASE) of larger-sized perovskite crystals, is still relatively scarce. Here, we presented room-temperature size-dependent spontaneous emission (SE) and ASE of the organometal halide CH 3 NH 3 PbBr 3 perovskite cubic microcrystals pumped through one-photon-(1P) and two-photon-(2P) excitation paradigms. The results showed that the optical properties of SE and ASE were sensitively dependent on the sizes of perovskite microcrystals irrespective of whether 1P or 2P excitation was used. Moreover, by comparing the spectral results of 1P- and 2P-pumped experiments, 2P pumping was found to be an effective paradigm to reduce thresholds by one order of magnitude. Finally, we carried out fluences-dependent time-resolved fluorescence dynamics experiments to study the underlying effects of these scale-dependent SE and ASE. We found that the photoluminescence (PL) recombination rates sensitively became faster with increasing carriers' densities, and that the ASE pumped from larger-sized CH 3 NH 3 PbBr 3 perovskite cubic microcrystals showed faster lifetimes. This work shows that micro-sized perovskite cubic crystals could be the ideal patterns of perovskite materials for realizing ASE applications in the future.

Recently, all-inorganic cesium lead halide perovskites (CsPbX 3 ) quantum dots (QDs) have attracted great attention due to their halogen composition and size tunable band gap engineering, the same physical mechanism that is responsible for excellent performance in light-emitting devices. However, little is known about the time-resolved fluorescence quenching dynamics process of these CsPbX 3 QDs. In this article, we present comprehensive contrastive spectral studies on the electron and hole extraction dynamics of CsPbX 3 colloidal QDs with and without quencher by time-resolved femtosecond transient absorption (TA) and time-correlated single-photon counting (TCSPC) spectroscopy methods. We have identified that the partial electrons of the conduction band and holes of the valence band of CsPbX 3 QDs can be directly extracted by tetracyanoethylene (TCNE) and phenothiazine (PTZ), respectively. Moreover, compared with the CsPbBr 3 QDs, the CsPbI 3 QDs showed relatively slower charge extraction rates. We also found that the CsPbBr 3 QDs with smaller size showed faster carrier recombination rates and photoluminescence (PL) decay lifetime due to the relatively stronger quantum confinement effects. We believe that this study may be useful for realising optimal applications in photovoltaic and light emission devices.

Recent advancements in nanotechnology have continued to stimulate the development of functional devices based on nanomaterials. However, the controllable assembly of these tiny nanomaterials into functional structures is still a big challenge for further applications; nowhere is this more obvious than in the field of nanodevices. Currently, despite the fact that self-assembly technologies have revealed great potential to reach this end, serious problems with respect to morphology control, designable assembly and even flexible patterning set huge obstacles to the fabrication of functional devices. Nowadays, in addition to self-assembly technologies that make use of interaction forces between different objects, photodynamic assembly (PDA) technology has emerged as a promising route to architect functional materials with the help of optical driving forces towards device fabrication. In this review, we summarize the recent developments in PDA technology for the designable patterning of nanoparticles (NPs). The basic fundamentals of PDA that resort to optical trapping (OT) and typical examples regarding far-field/near-field OT for the PDA of various NPs have been reviewed. In particular, femtosecond laser induced photodynamic assembly (FsL-PDA), which enables the designable patterning of NPs through a direct writing manner, has been introduced. Finally, the current challenges and future prospects of this dynamic field are discussed based on our own opinions.

CH3NH3PbI3-xClx perovskite material has been commonly used as the free charge generator and reservoir in highly efficient perovskite-based solid-state solar photovoltaic devices. However, many of the underlying fundamental photophysical mechanisms in this material such as the perovskite transition band structure as well as the dependent relationship between the carrier properties and lattice properties still lack sufficient understanding. Here, we elucidated the fundamental band structure of the pure CH3NH3PbI3-xClx pervoskite lattice, and then reported about the dependent relationship between the free charge carrier characteristic and the different CH3NH3PbI3-xClx pervoskite lattice thin films utilizing femtosecond time-resolved pump-probe technologies. The data demonstrated that the pure perovskite crystal band structure should only have one conduction and one valence band rather than dual valences, and the pure perovskite lattice could trigger more free charge carriers with a slower recombination rate under an identical pump intensity compared with the impurities doped perovskite crystal. We also investigated the perovskite film performance when exposed to moisture and water, the corresponding results gave us a dip in the optimization of the performance of perovskite based devices, and so as a priority this material should be isolated from moisture (water). This work may propose a deeper perspective on the comprehension for this material and it is useful for future optimization of applications in photovoltaic and light emission devices.

We report the fabrication of three-dimensional periodic metal nickel nanostructures achieved by the combination of femtosecond laser-induced two-photon polymerization and electroless plating technology. We can control the deposition speed of 10 nm per second by adjusting the reaction time. The thermal stability is good under 500 °C for the three-dimensional graphite-lattice polymer structure with 200 nm nickel film. Optical reflectivity and thermal emission measurements under 550 °C showed that the fabricated metallic structure was thermally excited and emitted light at λ = 4.50, 4.95 μm. The emission peak wavelengths agree with the absorption peaks. These data demonstrate that creating metallic photonic crystals by incorporation of metals to laser-fabricated templates is a simple and cost-efficient method. The emitters can work at such low temperatures, which is more important for realistic operation in applications.

Reported here is the design and fabrication of three-dimensional (3D) "overpass" microstructures at the junction of crossed microfluidic channels by femtosecond laser direct writing of photopolymers. The post-integrated overpass could be used for guiding different microfluids across the junction without mixing; therefore it is proposed as an enabler for achieving 3D microfluidic chips based on conventional two-dimensional (2D) microchannels. As representative examples, bi-crossed and tri-crossed microchannels have been equipped with bi-connected and tri-connected overpasses, respectively. Flow tests confirm 3D flowing capability. The integration of such overpass structures at the microchannel junction provides an opportunity to impart 3D capability to conventional 2D microchips, thus the method may hold great promise for both functionalization and miniaturization of Lab-on-a-Chip systems.

We present a facile production approach to highly efficient SERS test strips by physical vapor deposition of silver on paper, which contains natural wrinkle and fibril structures. The SERS test strips open the door to highly sensitive (e.g., 10(-10) M) SERS detection in a convenient fashion.

Composition modification and surface microstructures have been widely utilized in interface science to improve the surface performance. In this paper, we observed a significant improvement of oil contact angle (CA) from 66 ± 2° to 120 ± 4° by introducing a radical silanol group on a flat PDMS surface through oxygen plasma pretreatment. By combining surface microstructures and plasma modification, we produced three kinds of superoleophobic surfaces: 20 μm pitch micropillar arrays, 2.5 μm pitch micropillar arrays and gecko foot-like hierarchical microstructures. Among them, the hierarchical surface with high surface roughness showed extreme underwater superoleophobicity, which featured ultrahigh CA (175 ± 3°) and ultrasmall sliding angle (<1°). Quantitative measurements demonstrated that these superoleophobic surfaces exhibited distinct adhesive behaviors, by which they were interpreted as Wenzel's, Cassie's and the Lotus state, respectively. A microfluidic channel with superoleophobic microstructures was further created by novel curve-assisted imprint lithography, and the characterization based on anti-oil contamination applications was carried out and discussed. We believe that the superoleophobic surfaces will power broad applications in oil microdroplet transportation, anti-oil channels and droplet microfluidic systems.

We report here a facile approach for flexible integration of high efficiency surface enhanced Raman scattering (SERS) monitors in a continuous microfluidic channel. In our work, femtosecond laser direct writing was adopted for highly localizable and controllable fabrication of the SERS monitor through a multi-photon absorption (MPA) induced photoreduction of silver salt solution. The silver substrate could be shaped into designed patterns, and could be precisely located at the desired position of the microchannel bed, giving the feasibility for real-time detection during reactions. SEM and TEM images show that the silver substrates were composed of crystallized silver nanoplates with an average thickness of 50 nm. AFM results reveal that the substrates were about 600 nm in height and the surface was very rough. As representative tests for SERS detection, p-aminothiophenol (p-ATP) and flavin adenine dinucleotide (FAD) were chosen as probing molecules for microfluidic analysis at visible light (514.5 nm) excitation, exhibiting an enhancement factor of ~10(8). In addition, the combination of the SERS substrate with the microfluidic channel allows detection of inactive analytes through in situ microfluidic reactions.

Reported in this paper is two-photon photopolymerization (TPP) fabrication of magnetic microturbines with high surface smoothness towards microfluids mixing. As the key component of the magnetic photoresist, Fe(3)O(4) nanoparticles were carefully screened for homogeneous doping. In this work, oleic acid stabilized Fe(3)O(4) nanoparticles synthesized via high-temperature induced organic phase decomposition of an iron precursor show evident advantages in particle morphology. After modification with propoxylated trimethylolpropane triacrylate (PO(3)-TMPTA, a kind of cross-linker), the magnetic nanoparticles were homogeneously doped in acrylate-based photoresist for TPP fabrication of microstructures. Finally, a magnetic microturbine was successfully fabricated as an active mixing device for remote control of microfluids blending. The development of high quality magnetic photoresists would lead to high performance magnetically controllable microdevices for lab-on-a-chip (LOC) applications.

This paper demonstrates the embellishment of existing microfluidic devices with integrated three dimensional (3D) micronanostructures via femtosecond laser micronanofabrication, which, for the first time, proves two-photon photopolymerization (TPP) to be a powerful technology for chip functionalization. As representative examples, microsieves with various pore shape and adjustable pore size were successfully fabricated inside a conventional glass-based microfluidic channel prepared by wet etching for microparticle separation. Moreover, a fish scale like microfilter was also fabricated and appointed as a one-way valve, which showed excellent performance as we expected. These results indicate that such embellishment of microfluidic devices is simple, low cost, flexible and easy to access. We believe that, combined with TPP, the application of lab-on-chip devices would be further extended.