Chirped Laser Pulses Research Articles

High brightness betatron x-ray source driven by chirped laser pulses

We demonstrate high brightness betatron x-ray generation from a chirped laser pulses driven plasma accelerator. It is shown that positively chirped laser pulse leads to the initiation and enhancement of collective oscillations of electrons inside plasma bubbles, due to associated pulse front tilt (PFT). The PFT causes transverse drift of the bubbles with respect to the laser axis, which results in high brightness x-ray generation. At an optimum chirp, enhanced x-ray emission of >108 photons/pulse/sr in 0.1% BW with a critical energy of ∼18 keV was observed by a factor >2 in comparison to the case of no chirp. The role of collective oscillation in enhancing x-ray emission is also validated in the Geant4 simulations.

Multiwavelength highly transient stimulated Raman scattering on dual Raman modes in Sr(MoO4)0.8(WO4)0.2 and Sr(MoO4)0.4(WO4)0.6.

For the first time to our knowledge, multiwavelength, highly transient, single-pass stimulated Raman scattering with a low wavelength spacing on dual (stretching and bending) Raman modes in Sr(MoO4)0.8(WO4)0.2 and Sr(MoO4)0.4(WO4)0.6 solid solutions in a range of 1000-1300 nm (transparence window of biological tissue) under ultrafast chirped pulse laser pumping is comparatively investigated in the interests of multicolor two-photon imaging of a living tissue. For both the solid solutions, the optimum range (1-5 ps) of chirped pump pulse durations for multiwavelength Raman conversion on dual Raman modes was wider than for SrMoO4 (2-3 ps) due to the higher integral cross section of the bending Raman mode. Higher efficient SRS conversion took place at negative chirping of the pump pulse with its stretching from 0.25 ps up to 5 ps due to the compensation of a positive chirp caused by nonlinear phase modulation with total Raman conversion efficiency of up to 36% for Sr(MoO4)0.8(WO4)0.2 and 49% for Sr(MoO4)0.4(WO4)0.6. The highest number (five) of Stokes components in the desired range (1000-1300 nm) was observed in the optimum Sr(MoO4)0.4(WO4)0.6 solid solution, which has the Raman modes with comparable intensities.

Cooling positronium to ultralow velocities with a chirped laser pulse train

When laser radiation is skilfully applied, atoms and molecules can be cooled1–3, allowing the precise measurements and control of quantum systems. This is essential for the fundamental studies of physics as well as practical applications such as precision spectroscopy4–7, ultracold gases with quantum statistical properties8–10 and quantum computing. In laser cooling, atoms are slowed to otherwise unattainable velocities through repeated cycles of laser photon absorption and spontaneous emission in random directions. Simple systems can serve as rigorous testing grounds for fundamental physics—one such case is the purely leptonic positronium11,12, an exotic atom comprising an electron and its antiparticle, the positron. Laser cooling of positronium, however, has hitherto remained unrealized. Here we demonstrate the one-dimensional laser cooling of positronium. An innovative laser system emitting a train of broadband pulses with successively increasing central frequencies was used to overcome major challenges posed by the short positronium lifetime and the effects of Doppler broadening and recoil. One-dimensional chirp cooling was used to cool a portion of the dilute positronium gas to a velocity distribution of approximately 1 K in 100 ns. A major advancement in the field of low-temperature fundamental physics of antimatter, this study on a purely leptonic system complements work on antihydrogen13, a hadron-containing exotic atom. The successful application of laser cooling to positronium affords unique opportunities to rigorously test bound-state quantum electrodynamics and to potentially realize Bose–Einstein condensation14–18 in this matter–antimatter system.

Effect of laser chirping on third harmonic generation in anharmonic clusters with ripple on cluster density

A proposed model delves into the resonant enhancement of third harmonic generation (THG) by a short-pulse laser inside nanoclustered plasma under the influence of density ripple. An intense chirped laser pulse incident on a clustered plasma of argon gas displaces the electrons of the medium and produces a restoring force. This force is considered to vary nonlinearly with electron displacement, leading to the anharmonic response of the electron clouds of the cluster. The nonlinear current at the third harmonic frequency arises from the perturbation of the electron density of the cluster by the ponderomotive force exerted on them by the incident laser pulse. Applying ripple in cluster density and electron density of surrounding plasma enables the phase-matching criteria for THG to be satisfied, which leads to enhanced harmonic output. An anharmonic structure of clusters exhibits strong optical nonlinearities, resulting in the plasmon resonance broadening and producing harmonics with greater efficiency. Numerical analysis shows that the chirp parameter of the laser pulse and ripple on cluster density enhance system nonlinearity causing the generation of a third harmonic of enhanced amplitude. The study explores how different factors such as laser intensity, cluster size, ripple parameter, chirp parameter, and electron excursion influence the efficiency of THG.

Optimized terahertz generation in BNA organic crystals with chirped Ti:sapphire laser pulses.

We report on the efficient generation of intense terahertz radiation from the organic crystal N-benzyl-2-methyl-4-nitroaniline pumped by chirped Ti:sapphire femtosecond laser pulses. The THz energy and spectrum as a function of the pump fluence and duration of the chirped laser pulses are studied systematically. For the appropriate positively chirped pump pulses, a significant boost in the THz generation efficiency by a factor of around 2.5 is achieved, and the enhancement of high-frequency components (>1 THz) shortens the THz pulse duration. Via complete characterization of THz properties and transmitted laser spectra, this nonlinear behavior is attributed to the extended effective interaction length for phase matching as a result of the self-phase modulation of the intense pump laser pulses. Numerical calculations well reproduce the experimental observation. Our results demonstrate a robust, efficient, strong-field (up to several MV/cm) THz source using the common sub-10 mJ and sub-100 fs Ti:sapphire laser systems without optical parametric amplifiers.

Unveiling Ultrafast-Weak-Field Coherent Control of Indirect Dissociation Reactions.

Coherent control of molecular photodissociation through one-photon transitions has become a topic of interest in physical chemistry. Previous studies have shown that modulating the spectral phase of a single ultrafast laser pulse while keeping its spectral amplitude constant does not affect the dissociation yield of reactions originating from a pure eigenstate of the ground electronic state. Here, we explore the indirect photodissociation reaction of NaI molecules using theoretical and numerical methods. Our findings show that, in contrast to the outcomes achieved with negatively chirped pulses, time-dependent population of the eigenstates of the excited adiabatic potential induced by positively chirped laser pulses, acting as intermediates in the reaction, cannot be periodically restored to that caused by the unchirped pulse. This gives rise to an intriguing phenomenon: the sign of the pulse's chirp rate influences the distribution of dissociation fragments in coordinate and momentum space over extended periods. This work highlights the potential of using spectral-phase modulated pulses to manipulate indirect photodissociation reactions, offering a way to modify the transient photofragment distributions by controlling reaction intermediates.

Modulation of H atom photoelectron momentum distribution by chirped laser pulses of different wavelengths

The wavelength dependence of the holographic interference structure in the photoelectron momentum distribution (PMD) of hydrogen atoms under a few-cycle chirped laser field is investigated using a two-dimensional (2D) semiclassical two-step (SCTS) model. Under the constraint of a fixed chirp parameter, we observe an amplification in the impact of the chirp parameter on the laser field waveform as the wavelength increases. This enhancement facilitates effective modulation of the ionization time window. As the wavelength reaches a certain threshold, the double-slit interference pattern undergoes an observable expansion towards the left. Furthermore, based on the variations in X-axis momentum (Px) concerning ionization time at different wavelengths and the corresponding distribution of classical electron trajectories at those wavelengths, we present a more comprehensive explanation for the expansion of interference patterns. This expansion can be attributed to changes in wavelength, which result in modifications to the laser field’s waveform, consequently leading to a significant acceleration of ionized electrons when exposed to chirped laser pulses. It is worth noting that by tuning the negative chirp parameter, the leftward expansion of the double-slit interference pattern can also be achieved, particularly when shorter wavelengths of chirped laser pulses are employed.

Chirped Laser Pulse Control of Vibronic Wavepackets and Energy Transfer in Phycocyanin 645.

Photosynthetic organisms use light-harvesting complexes to increase the spectrum of light that they absorb from solar photons. Recent ultrafast spectroscopic studies have revealed that efficient (sub-ps) energy transfer is mediated by vibronic coherence in the phycobiliprotein phycocyanin 645 (PC645). Here, we report studies that employ broadband pump-probe spectroscopy with linearly chirped excitation pulses to further investigate the relationship between vibronic state preparation and energy transfer dynamics in PC645. Negatively chirped pulse excitation is found to enhance wavepackets of a high-frequency mode (1580 cm-1) and increase the rate of downhill energy transfer, while on the other hand, positively chirped pulses suppress these oscillatory features and decrease this rate. Model calculations incorporating the influence of the chirped pump pulse are used to understand its effect on initial state preparation. These results provide mechanistic insight into how the overall nonequilibrium rate of energy transfer is influenced by initial state preparation.

Nonlinear propagation of chirped laser pulses through a dispersive and turbulent atmosphere

The evolution of ultrashort laser pulses in dispersive, turbulent, nonlinear, and dissipative media is discussed in connection with nonlinear self-focusing collapse and the onset of laser filamentation. In quiescent air, a laser pulse propagating with a peak power greater than a critical power for self-focusing will undergo a catastrophic, transverse collapse until the intensity is large enough for photoionization. At this point, self-focusing is arrested and balanced by plasma refraction, forming a laser filament. By applying an appropriate chirp, the dispersive properties of the medium can be used to enhance this process and control its onset, and to counter dissipative effects such as molecular absorption and atmospheric scattering. This paper presents an analysis of the effect of atmospheric turbulence on the propagation of nonlinear pulses with dispersion compensation (chirp). The analytical results are compared with wave optics simulations and found to be in reasonable agreement as long as the pulse maintains a near-Gaussian spatiotemporal profile.

Ouroboros-pattern-like electron spirals by synchronous crossed chirped laser pulses

Ouroboros-pattern-like electron spirals by synchronous crossed chirped laser pulses

Spatiotemporal control of high-intensity laser pulses with a plasma lens

Spatiotemporal control encompasses a variety of techniques for producing laser pulses with dynamic intensity peaks that move independently of the group velocity. This controlled motion of the intensity peak offers a new approach to optimizing laser-based applications and enhancing signatures of fundamental phenomena. Here, we demonstrate spatiotemporal control with a plasma optic. A chirped laser pulse focused by a plasma lens exhibits a moving focal point, or “flying focus,” that can travel at an arbitrary, predetermined velocity. Unlike currently used conventional or adaptive optics, a plasma lens can be located close to the interaction region and can operate at an orders of magnitude higher, near-relativistic intensity. Published by the American Physical Society 2024

Robust parallel laser driving of quantum dots for multiplexing of quantum light sources

Deterministic sources of quantum light (i.e. single photons or pairs of entangled photons) are required for a whole host of applications in quantum technology, including quantum imaging, quantum cryptography and the long-distance transfer of quantum information in future quantum networks. Semiconductor quantum dots are ideal candidates for solid-state quantum emitters as these artificial atoms have large dipole moments and a quantum confined energy level structure, enabling the realization of single photon sources with high repetition rates and high single photon purity. Quantum dots may also be triggered using a laser pulse for on-demand operation. The naturally-occurring size variations in ensembles of quantum dots offers the potential to increase the bandwidth of quantum communication systems through wavelength-division multiplexing, but conventional laser triggering schemes based on Rabi rotations are ineffective when applied to inequivalent emitters. Here we report the demonstration of the simultaneous triggering of >10 quantum dots using adiabatic rapid passage. We show that high-fidelity quantum state inversion is possible in a system of quantum dots with a 15 meV range of optical transition energies using a single broadband, chirped laser pulse, laying the foundation for high-bandwidth, multiplexed quantum networks.

Field-free orientation of 7LiH steered by a few-cycle nonlinearly chirped pulse

We demonstrate theoretically that an efficient field-free molecular orientation of 7LiH molecule steered by a few-cycle nonlinearly chirped laser pulse with frequency in the terahertz regime can be achieved. The frequency modulation parameter β plays an important role in the molecular orientation, the maximum molecular orientation |〈cosθ〉|max is 0.848 and the orientation duration is 150 fs when β=7.25. In the range of electric-field peak intensity E0=[0.1,4.0] MV/cm, we can find the maximum orientation degree in both positive and negative directions. Compared to the scheme steered by a normal laser pulse, we can find that a more efficient molecular orientation and a smaller difference in population between the adjacent states can be realized by using the nonlinearly chirped laser pulse under the same near-single-period conditions. In addition, at the same temperature, a higher molecular orientation and a smaller decrease rate of orientation with temperature can be obtained by the nonlinearly chirped laser pulse.

Control of the spider-like interference structure in photoelectron momentum distributions of a helium atom in a few-cycle nonlinear chirped laser pulse.

We investigate theoretically the photoelectron momentum distributions (PMDs) of the helium atom in the few-cycle nonlinear chirped laser pulse. The numerical results show that the direction of the spider-like interference structure in PMDs exhibits periodic variations with the increase of the chirp parameter. It is illustrated that the direction of the spider-like interference structure is related to the direction of the electron motion by tracking the trajectories of the electrons. We also demonstrate that the carrier-envelope phase can precisely control the opening of the ionization channel. In addition, we investigate the PMDs when a chirp-free second harmonic (SH) laser pulse is added to the chirped laser field, the numerical results show that the interference patterns can change from only spider-like interference structure to both spider-like and ring-like interference structures.

Chirped Pulses Meet Quantum Dots: Innovations, Challenges, and Future Perspectives

AbstractShaped laser pulses have been remarkably effective in investigating various aspects of light–matter interactions spanning a broad range of research. Chirped laser pulses exhibiting a time‐varying frequency, or quadratic spectral phase, form a crucial category in the group of shaped laser pulses. This type of pulses have made a ubiquitous presence from spectroscopic applications to developments in high‐power laser technology, and from nanophotonics to quantum optical communication, ever since their introduction. In the case of quantum technologies recently, substantial efforts are being invested toward achieving a truly scalable architecture. Concurrently, it is important to develop methods to produce robust photon sources. In this context, semiconductor quantum dots hold great potential, due to their exceptional photophysical properties and on‐demand operating nature. Concerning the scalability aspect of semiconductor quantum dots, it is advantageous to develop a simple, yet robust method to generate photon states from it. Chirped pulse excitation has been widely demonstrated as a robust and efficient state preparation scheme in quantum dots, thereby boosting its applicability as a stable photon source in a real‐world scenario. Despite the rapid growth and advancements in laser technologies, the generation and control of chirped laser pulses can be demanding. Here, an overview of a selected few approaches is presented to tailor and characterize chirped pulses for the efficient excitation of a quantum dot source. By taking the chirped‐pulse‐induced adiabatic rapid passage process in quantum dot as an example, numerical design examples are presented along with experimental advantages and challenges in each method and conclude with an outlook on future perspectives.

A Scalable, High-Efficiency, Low-Energy-Spread Laser Wakefield Accelerator Using a Tri-Plateau Plasma Channel.

The emergence of multi-petawatt laser facilities is expected to push forward the maximum energy gain that can be achieved in a single stage of a laser wakefield acceleration (LWFA) to tens of giga-electron volts, which begs the question-is it likely to impact particle physics by providing a truly compact particle collider? Colliders have very stringent requirements on beam energy, acceleration efficiency, and beam quality. In this article, we propose an LWFA scheme that can for the first time simultaneously achieve hitherto unrealized acceleration efficiency from the laser to the electron beam of >20% and a sub-1% energy spread using a stepwise plasma structure and a nonlinearly chirped laser pulse. Three-dimensional high-fidelity simulations show that the nonlinear chirp can effectively mitigate the laser waveform distortion and lengthen the acceleration distance. This, combined with an interstage rephasing process in the stepwise plasma, can triple the beam energy gain compared to that in a uniform plasma for a fixed laser energy, thereby dramatically increasing the efficiency. A dynamic beam loading effect can almost perfectly cancel the energy chirp that arises during the acceleration, leading to the sub-percent energy spread. This scheme is highly scalable and can be applied to petawatt LWFA scenarios. Scaling laws are obtained, which suggest that electron beams with parameters relevant for a Higgs factory could be reached with the proposed high-efficiency, low-energy-spread scheme.

Theoretical study of influence of laser pulse chirp on terahertz emission characteristics of gas induced by two-color laser field

With the development of terahertz (THz) wave research, the demand for controllable THz sources is increasing. How to obtain the regulated THz waves has been one of the research hotspots and key problem in the field of THz science. There have been researches in which the resulting THz wave is modulated by changing the wavelength, relative phase, energy, or chirp of the laser produced by a two-color laser. In this work, we establish a three-dimensional theoretical model of THz wave generation and subsequent propagation induced by two-color laser. And we investigate the influence of chirp modulation of different laser on THz wave by chirp modulation of the fundamental wave (FW) and the second harmonic wave (SHW) of two-color laser, including THz wave amplitude, THz wave center frequency and spectrum width, and analyze the physical mechanism of related phenomena. At the same time, the effects of different orders of magnitudes of laser chirp parameters (femtosecond and picosecond) and initial phase of laser pulse on THz wave parameters are also studied. The results are shown below. 1) In the two-color laser, the chirp of FW mainly affects the shape of THz wave when the initial phase is unchanged. The chirp modulation of SHW can cause the amplitude of THz wave to change significantly, and affect the center frequency and spectrum width of THz waves. 2) In the case of laser pulse width of femtosecond order, 40 fs is taken as an example. When the chirp parameter is of femtosecond magnitude, the chirp parameter has a great influence on the THz wave generation efficiency of two-color laser filament. At the picosecond magnitude, the chirp parameter has a weak effect on the THz wave energy and mainly affects the phase of the THz wave. 3) The initial phase of the two-color laser can aid in chirp modulation of THz wave to optimize the energy generated. 4) The initial phase of two-color laser can assist in the process of chirped laser modulation of terahertz waves to optimize the energy generated. Our research shows that the chirp modulation, as a controllable parameter, has multiple regulation effect on the properties of radiated THz waves. The related research results provide a new idea and basis for studying the generation and regulation of THz waves.

Relativistic cross-focusing of two chirped laser pulses in thermal quantum plasma

Relativistic cross-focusing of two chirped laser pulses in thermal quantum plasma

Compact chirped fiber Bragg gratings for single-photon generation from quantum dots

A scalable source of single photons is a key constituent of an efficient quantum photonic architecture. To realize this, it is beneficial to have an ensemble of quantum emitters that can be collectively excited with high efficiency. Semiconductor quantum dots hold great potential in this context due to their excellent photophysical properties. Spectral variability of quantum dots is commonly regarded as a drawback introduced by the fabrication method. However, this is beneficial to realize a frequency-multiplexed single-photon platform. Chirped pulse excitation, relying on the so-called adiabatic rapid passage, is the most efficient scheme to excite a quantum dot ensemble due to its immunity to individual quantum dot parameters. Yet, the existing methods of generating chirped laser pulses to excite a quantum emitter are bulky, lossy, and mechanically unstable, which severely hampers the prospects of a quantum dot photon source. Here, we present a compact, robust, and high-efficiency alternative for chirped pulse excitation of solid-state quantum emitters. Our simple plug-and-play module consists of chirped fiber Bragg gratings, fabricated via femtosecond inscription, to provide high values of dispersion in the near-infrared spectral range, where the quantum dots emit. We characterize and benchmark the performance of our method via chirped excitation of a GaAs quantum dot, establishing high-fidelity single-photon generation. Our highly versatile chirping module coupled to a photon source is a significant milestone toward realizing practical quantum photonic devices.

Retaining terahertz intensity modulation at second harmonic generation of a chirped pulse

Terahertz modulation of chirped laser pulse intensity was achieved with phase-only spectral modulation. Preservation of this modulation during second harmonic generation together with almost 30% conversion efficiency was demonstrated employing noncollinear frequency mixing of 60-µJ oppositely chirped laser pulses.