Pulsed Optical Excitation Research Articles

Heat transfer from nanoparticles for targeted destruction of infectious organisms

Whereas the application of optically or magnetically heated nanoparticles to destroy tumours is now well established, the extension of this concept to target pathogens has barely begun. Here we examine the challenge of targeting pathogens by this means and, in particular, explore the issues of power density and heat transfer. Depending on the rate of heating, either hyperthermia or thermoablation may occur. This division of the field is fundamental and implies very different sources of excitation and heat transfer for the two modes, and different strategies for their clinical application. Heating by isolated nanoparticles and by agglomerates of nanoparticles is compared: hyperthermia is much more readily achieved with agglomerates and for large target volumes, a factor which favours magnetic excitation and moderate power densities. In contrast, destruction of planktonic pathogens is best achieved by localised thermoablation and very high power density, a scenario that is best delivered by pulsed optical excitation.

CsPbBr3 Perovskite Quantum Dot Vertical Cavity Lasers with Low Threshold and High Stability

All-inorganic cesium lead bromide (CsPbBr3) perovskite quantum dots (QDs) have recently emerged as highly promising solution-processed materials for next-generation light-emitting applications. They combine the advantages of QD and perovskite materials, which makes them an attractive platform for achieving high optical gain with high stability. Here, we report an ultralow lasing threshold (0.39 μJ/cm2) from a hybrid vertical cavity surface emitting laser (VCSEL) structure consisting of a CsPbBr3 QD thin film and two highly reflective distributed Bragg reflectors (DBRs). Temperature dependence of the lasing threshold and long-term stability of the device were also characterized. Notably, the CsPbBr3 QDs provide superior stability and enable stable device operation over 5 h/1.8 × 107 optical pulse excitations under ambient conditions. This work demonstrates the significant potential of CsPbBr3 perovskite QD VCSELs for highly reliable lasers, capable of operating in the short-pulse (femtosecond) and quasi-co...

Laser-Induced Focused Ultrasound for Cavitation Treatment: Toward High-Precision Invisible Sonic Scalpel.

Beyond the implementation of the photoacoustic effect to photoacoustic imaging and laser ultrasonics, this study demonstrates a novel application of the photoacoustic effect for high-precision cavitation treatment of tissue using laser-induced focused ultrasound. The focused ultrasound is generated by pulsed optical excitation of an efficient photoacoustic film coated on a concave surface, and its amplitude is high enough to produce controllable microcavitation within the focal region (lateral focus <100 µm). Such microcavitation is used to cut or ablate soft tissue in a highly precise manner. This work demonstrates precise cutting of tissue-mimicking gels as well as accurate ablation of gels and animal eye tissues.

Ab initio dynamical exchange interactions in frustrated antiferromagnets

The ultrafast response to an optical pulse excitation of the spin-spin exchange interaction in transition metal anti-ferromagnets is studied within the framework of the time-dependent spin-density functional theory. We propose a formulation for the purely dynamical exchange interaction, which is non-local in space, and it is derived starting from {\it ab initio} arguments. Then, we investigate the effect of the laser pulse on the onset of the dynamical process. It is found that we can distinguish two types of excitations, both activated immediately after the action of the laser pulse. While the first one can be associated to a Stoner-like excitation and involves the transfer of spin from one site to another, the second one is related to the ultrafast modification of a Heisenberg-like exchange interaction and can trigger the formation of spin waves in the first few hundred femtoseconds of the time evolution.

Relaxation Oscillations and Ultrafast Emission Pulses in a Disordered Expanding Polariton Condensate

Semiconductor microcavities are often influenced by structural imperfections, which can disturb the flow and dynamics of exciton-polariton condensates. Additionally, in exciton-polariton condensates there is a variety of dynamical scenarios and instabilities, owing to the properties of the incoherent excitonic reservoir. We investigate the dynamics of an exciton-polariton condensate which emerges in semiconductor microcavity subject to disorder, which determines its spatial and temporal behaviour. Our experimental data revealed complex burst-like time evolution under non-resonant optical pulsed excitation. The temporal patterns of the condensate emission result from the intrinsic disorder and are driven by properties of the excitonic reservoir, which decay in time much slower with respect to the polariton condensate lifetime. This feature entails a relaxation oscillation in polariton condensate formation, resulting in ultrafast emission pulses of coherent polariton field. The experimental data can be well reproduced by numerical simulations, where the condensate is coupled to the excitonic reservoir described by a set of rate equations. Theory suggests the existence of slow reservoir temporarily emptied by stimulated scattering to the condensate, generating ultrashort pulses of the condensate emission.

Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency.

Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow ultrafast dynamics to be characterized in materials. However, the pursuit of simultaneous ultimate spatial and temporal resolution of microscopy and spectroscopy is largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. Field-driven photoemission from metal tips provides high light-phase synchronization, but suffers large electron energy spreads (3-100 eV) as driven by a long wavelength laser (>800 nm). Here, ultrafast electron emission from carbon nanotubes (≈1 nm radius) excited by a 410 nm femtosecond laser is realized in the field-driven regime. In addition, the emitted electrons have great monochromaticity with energy spread as low as 0.25 eV. This great performance benefits from the extraordinarily high field enhancement and great stability of carbon nanotubes, superior to metal tips. The new nanotube-based ultrafast electron source opens exciting prospects for extending current characterization to sub-femtosecond temporal resolution as well as sub-nanometer spatial resolution.

Charge carrier kinetics in GeSi/Si quantum dots probed by mid-infrared radiation

The mid-infrared photo-induced absorption relaxation kinetics of the self-assembled array of GeSi quantum dots in Si matrix was studied in the conditions of short pulsed interband optical excitation. The measured absorption decay curves directly show the temporal evolution of the population of the QD ground states. The analysis of the experimental data allowed us to estimate characteristic recombination and capture times, and the electron localization energy in the vicinity of QD.

Long-term mutual phase locking of picosecond pulse pairs generated by a semiconductor nanowire laser

The ability to generate phase-stabilized trains of ultrafast laser pulses by mode-locking underpins photonics research in fields, such as precision metrology and spectroscopy. However, the complexity of conventional mode-locked laser systems has hindered their realization at the nanoscale. Here we demonstrate that GaAs-AlGaAs nanowire lasers are capable of emitting pairs of phase-locked picosecond laser pulses with a repetition frequency up to 200 GHz when subject to incoherent pulsed optical excitation. By probing the two-pulse interference spectra, we show that pulse pairs remain mutually coherent over timescales extending to 30 ps, much longer than the emitted laser pulse duration (≤3 ps). Simulations performed by solving the optical Bloch equations produce good quantitative agreement with experiments, revealing how the phase information is stored in the gain medium close to transparency. Our results open the way to phase locking of nanowires integrated onto photonic circuits, optical injection locking and applications, such as on-chip Ramsey comb spectroscopy.

Retraction of "Transient Photothermal Spectra of Plasmonic Nanobubbles".

The photothermal efficacy of near-infrared gold nanoparticles (NP), nanoshells, and nanorods was studied under pulsed high-energy optical excitation in plasmonic nanobubble (PNB) mode as a function of the wavelength and duration of the excitation laser pulse. PNBs, transient vapor nanobubbles, were generated around individual and clustered overheated NPs in water and living cells. Transient PNBs showed two photothermal features not previously observed for NPs: the narrowing of the spectral peaks to 1 nm and the strong dependence of the photothermal efficacy upon the duration of the laser pulse. Narrow red-shifted (relative to those of NPs) near-infrared spectral peaks were observed for 70 ps excitation laser pulses, while longer sub- and nanosecond pulses completely suppressed near-infrared peaks and blue shifted the PNB generation to the visual range. Thus, PNBs can provide superior spectral selectivity over gold NPs under specific optical excitation conditions.

Ultrafast Charge Transfer between Light Absorber and Co3O4 Water Oxidation Catalyst across Molecular Wires Embedded in Silica Membrane.

The mechanism of visible light-induced hole transfer from a molecular light absorber, in the form of a free-base porphyrin, coupled to a Co3O4 nanoparticle catalyst for water oxidation by a molecular wire (p-oligo(phenylenevinylene) featuring three aryl units) is investigated by transient absorption spectroscopy. The wires are covalently anchored on the Co3O4 surface and embedded in a dense, yet ultrathin (2 nm), silica layer that separates light absorber and catalyst. The porphyrin is electrostatically adsorbed on the silica surface, and aqueous colloidal solutions of the core-shell particles are used for transient optical measurements. Pulsed optical excitation of the porphyrin results in rapid injection of the photogenerated hole onto the molecular wire and concurrent formation of reduced light absorber in less than 1 picosecond (ps). Ultrafast charge separation was monitored by transient absorption of the wire radical cation, which is given by bands in the 500 to 600 nm region and at 1130 nm, while formation of reduced porphyrin was characterized by absorption at 700 nm. Forward transfer of the hole to Co3O4 catalyst proceeds in 255 ± 23 ps. Ultrafast transfer of positive charge from the molecular assembly to a metal oxide nanoparticle catalyst for water oxidation is unprecedented. Holes on Co3O4 recombined with electrons of the reduced sensitizer with biphasic kinetics on a much longer time scale of ten to several hundred nanoseconds. The unusually efficient hole transfer coupling of a molecular light absorber with an Earth-abundant metal oxide catalyst by silica-embedded p-oligo(phenylenevinylene) offers an approach for integrated artificial photosystems featuring product separation on the nanoscale.

Optically pumped lasing in solution-processed perovskite semiconducting materials: Self-assembled Fabry–Pérot microcavity

Optically pumped lasing has been observed in solution-processed perovskite semiconducting materials, CH3NH3PbX3 (X = Cl, Br, I). Self-assembled Fabry–Pérot (FP) cavities have been easily obtained by using a simple “cast-capping method”, where we can obtain single-crystal-like optical cavities. The observed spectra show clear multimode lasing of the FP cavities under pulsed optical excitation. The mode intervals are well explained by the optical constants with large dispersions of the materials. The obtained refractive index around the lasing area coincides with the results in the previous reports.

Stationary Phonon Squeezing by Optical Polaron Excitation.

We demonstrate that a stationary squeezed phonon state can be prepared by a pulsed optical excitation of a semiconductor quantum well. Unlike previously discussed scenarios for generating squeezed phonons, the corresponding uncertainties become stationary after the excitation and do not oscillate in time. The effect is caused by two-phonon correlations within the excited polaron. We demonstrate by quantum kinetic simulations and by a perturbation analysis that the energetically lowest polaron state comprises two-phonon correlations which, after the pulse, result in an uncertainty of the lattice momentum that is continuously lower than in the ground state of the semiconductor. The simulations show the dynamics of the polaron formation process and the resulting time-dependent lattice uncertainties.

Acousto-optic modulation and opto-acoustic gating in piezo-optomechanical circuits.

Acoustic wave devices provide a promising chip-scale platform for efficiently coupling radio frequency (RF) and optical fields. Here, we use an integrated piezo-optomechanical circuit platform that exploits both the piezoelectric and photoelastic coupling mechanisms to link 2.4 GHz RF waves to 194 THz (1550 nm) optical waves, through coupling to propagating and localized 2.4 GHz acoustic waves. We demonstrate acousto-optic modulation, resonant in both the optical and mechanical domains, in which waveforms encoded on the RF carrier are mapped to the optical field. We also show opto-acoustic gating, in which the application of modulated optical pulses interferometrically gates the transmission of propagating acoustic pulses. The time-domain characteristics of this system under both pulsed RF and pulsed optical excitation are considered in the context of the different physical pathways involved in driving the acoustic waves, and modelled through the coupled mode equations of cavity optomechanics.

Low-threshold room-temperature AlGaAs/GaAs nanowire/single-quantum-well heterostructure laser

Near-infrared nanowire lasers are promising as ultrasmall, low-consumption light emitters in on-chip optical communications and computing systems. Here, we report on a room-temperature near-infrared nanolaser based on an AlGaAs/GaAs nanowire/single-quantum-well heterostructure grown by Au-catalyzed metal organic chemical vapor deposition. When subjects to pulsed optical excitation, the nanowire exhibits lasing, with a low threshold of 600 W/cm2, a narrow linewidth of 0.39 nm, and a high Q factor of 2000 at low temperature. Lasing is observed up to 300 K, with an ultrasmall temperature dependent wavelength shift of 0.045 nm/K. This work paves the way towards ultrasmall, low-consumption, and high-temperature-stability near-infrared nanolasers.

Ultrafast Structure Switching through Nonlinear Phononics.

We describe a mechanism by which nonlinear phononics allows ultrafast coherent and directional control of transient structural distortions. With ErFeO_{3} as a model system, we use density functional theory to calculate the structural properties as input into an anharmonic phonon model that describes the response of the system to a pulsed optical excitation. We find that the trilinear coupling of two orthogonal infrared-active phonons to a Raman-active phonon causes a transient distortion of the lattice. In contrast to the quadratic-linear coupling that has been previously explored, the direction of the distortion is determined by the polarization of the exciting light, introducing a novel mechanism for nonlinear phononic switching. Since the occurrence of the coupling is determined by the symmetry of the system we propose that it is a universal feature of orthorhombic and tetragonal perovskites.

Ultrafast demagnetizing fields from first principles

Starting from the continuity equation for the magnetization in time-dependent spin-density functional theory, we derive an expression for the effective time-dependent magnetic fields driving the out-of-equilibrium spin dynamics in magnetic systems. We evaluate these, so called, kinetic magnetic fields in the ultrafast demagnetization response to optical pulse excitations of ferromagnetic iron-based materials, namely Fe$_6$ cluster and bulk bcc Fe. We identify spatial "hot spots" where the demagnetization is particularly enhanced as a result of the increased kinetic torque.

A versatile implementation of pulsed optical excitation in scanning tunneling microscopy.

We present a combination of pulsed optical excitation and scanning tunneling microscopy with a highly flexible pulse generation method. A high frequency arbitrary wave generator drives a gigahertz electro-optical modulator, which processes a continuous-wave laser beam of a low-noise laser diode into the desired wave shape. For pump-probe excitation we generate optical pulse series in an all-electronic way. Thereby we can easily adapt parameters like pulse amplitude, width, or repetition cycle to the demands of the experiment. This setup is used to study different dynamic processes at the GaAs(110) surface. Separating thermally induced effects from electrically induced effects allows us to quantify the thermal contribution of the optical excitation in STM experiments. Time-resolved decay spectra of the photo-generated electron-hole pairs demonstrate the nanoscale spatial resolution.

Polarization-dependent exciton linewidth in semiconductor quantum wells: A consequence of bosonic nature of excitons

The exciton coherent signal decay rate in GaAs quantum wells, as measured in four-wave mixing experiments, depends on the polarization of the excitation pulses. Using polarization-dependent two-dimensional coherent spectroscopy, we show that this behavior is due to the bosonic character of excitons. Interference between two different quantum mechanical pathways results in a smaller decay rate for cocircular and colinear polarization of the optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a larger decay rate. Our result shows that the bosonic nature of excitons must be considered when interpreting ultrafast spectroscopic studies of exciton dephasing in semiconductors. This behavior should be considered while interpreting results of ultrafast spectroscopy experiments involving bosonlike excitations.

Lasing in Bose-Fermi mixtures.

Light amplification by stimulated emission of radiation, well-known for revolutionising photonic science, has been realised primarily in fermionic systems including widely applied diode lasers. The prerequisite for fermionic lasing is the inversion of electronic population, which governs the lasing threshold. More recently, bosonic lasers have also been developed based on Bose-Einstein condensates of exciton-polaritons in semiconductor microcavities. These electrically neutral bosons coexist with charged electrons and holes. In the presence of magnetic fields, the charged particles are bound to their cyclotron orbits, while the neutral exciton-polaritons move freely. We demonstrate how magnetic fields affect dramatically the phase diagram of mixed Bose-Fermi systems, switching between fermionic lasing, incoherent emission and bosonic lasing regimes in planar and pillar microcavities with optical and electrical pumping. We collected and analyzed the data taken on pillar and planar microcavity structures at continuous wave and pulsed optical excitation as well as injecting electrons and holes electronically. Our results evidence the transition from a Bose gas to a Fermi liquid mediated by magnetic fields and light-matter coupling.

Anisotropic lattice response induced by a linearly-polarized femtosecond optical pulse excitation in interfacial phase change memory material.

Optical excitation of matter with linearly-polarized femtosecond pulses creates a transient non-equilibrium lattice displacement along a certain direction. Here, the pump and probe pulse polarization dependence of the photo-induced ultrafast lattice dynamics in (GeTe)2/(Sb2Te3)4 interfacial phase change memory material is investigated under obliquely incident conditions. Drastic pump polarization dependence of the coherent phonon amplitude is observed when the probe polarization angle is parallel to the c–axis of the sample, while the pump polarization dependence is negligible when the probe polarization angle is perpendicular to the c–axis. The enhancement of phonon oscillation amplitude due to pump polarization rotation for a specific probe polarization angle is only found in the early time stage (≤2 ps). These results indicate that the origin of the pump and probe polarization dependence is dominantly attributable to the anisotropically-formed photo-excited carriers which cause the directional lattice dynamics.