arXiv subjects

Pengfei Lan

Publications and source records attributed to Pengfei Lan.

At least 37 records · Page 2Linked to original sources

arXiv2020

Energy scaling of water window high-order harmonic generation for single-shot soft X-ray spectroscopy and live-cell imaging

Full coherent soft X-ray attosecond pulses are now available through high-order harmonic generation (HHG); however, its insufficient output energy hinders various applications, such as attosecond-scale soft X-ray nonlinear experiments, the seeding of soft X-ray free-electron lasers, attosecond-pump-attosecond-probe spectroscopies, and single-shot imaging. In this paper, towards the implementation of these exciting studies, we demonstrate a soft X-ray harmonic beam that is more than two orders of magnitudes stronger up to the water window region compared to previous works. This was achieved by combining a newly developed TW class mid-infrared femtosecond laser and a loosely focusing geometry for HHG in the mid-infrared region for the first time. Thanks to a loosely focusing geometry with a neutral medium target, we achieve a high conversion efficiency, a low beam divergence, and a significantly reduced medium gas pressure. As the first application of our nano-joule level water window soft X-ray harmonic source, we demonstrate near edge X-ray absorption fine structure (NEXAFS) experiments with clear fine absorption spectra near the K- and L-edges observed in various samples. The systematic study of a robust energy scaling method on HHG opens the door for demonstrating single-shot absorption spectrum and live cell imaging with a femtosecond time resolution.

physics.optics↗

arXiv2020

Fully stabilized multi-TW optical waveform synthesizer for gigawatt soft-x-ray isolated attosecond pulses

A stable 50 mJ three-channel optical waveform synthesizer is demonstrated and used to reproducibly generate a high-order harmonics supercontinuum in the soft-x-ray region. This synthesizer is composed of pump pulses from a 10-Hz-repetition-rate Ti:sapphire pump laser and signal and idler pulses from an infrared two-stage optical parametric amplifier driven by this pump laser. With the full active stabilization of all relative time delays, relative phases, and the carrier-envelope phase, a shot-to-shot stable intense continuum harmonic spectrum is obtained around 60 eV with pulse energy above 0.24 $μ$J. The peak power of the soft-x-ray continuum is evaluated to be beyond 1 GW with a 140 as transform limit duration. Furthermore, we found a characteristic delay dependence of the multi-cycle waveform synthesizer and established its control scheme. Compared with the one-color case, we experimentally observe an enhancement of the cut-off spectrum intensity by one to two orders of magnitude through the three-color waveform synthesis.

physics.optics↗

arXiv2019

All-optical frequency resolved optical gating for isolated attosecond pulse reconstruction

We demonstrate an all-optical approach for precise characterization of attosecond extreme ultraviolet pulses. Isolated attosecond pulse is produced from high order harmonics using intense driving pulse with proper gating technique. When a weak field is synchronized with the driver, it perturbs the harmonics generation process via altering the accumulated phase of the electron trajectories. The perturbed harmonic spectrum can be formulated as a convolution of the unperturbed dipole and a phase gate, implying the validity of complete reconstruction of isolated attosecond pulses using conventional frequency resolved optical gating method. This in situ measurement avoids the central momentum approximation assumed in the widely used attosecond streaking measurement, providing a simple and reliable metrology for isolated attosecond pulse.

physics.optics↗

arXiv2019

Wave-front controlled attosecond time domain interferometry

Interferometry, as the key technique in modern precision measurements, has been used for length diagnosis in the fields of engineering metrology and astronomy. Analogous interferometric technique for time domain precision measurement is a significant complement to the spatial domain applications and requires the manipulation of the interference on the extreme time and energy scale. Here we present an all-optical interferometry for high precision measurement with attosecond temporal and hundreds of meV energy resolution. The interferometer is based on laser driven high order harmonics which provide a robust sequence of attosecond temporal slits. As applications, we reconstruct the waveform of an arbitrarily polarized optical pulse using the time resolving capability, and capture the abnormal character of the transition dipole near a Cooper minimum in argon using the energy resolution provided. This novel attosecond interferometry opens the possibility for high precision measurement in time energy domain using an all-optical approach.

physics.optics↗

arXiv2019

All-optical measurement of high-order fractional molecular echoes by high-order harmonic generation

An all-optical measurement of high-order fractional molecular echoes is demonstrated by using high-order harmonic generation (HHG). Excited by a pair of time-delayed short laser pulses, the signatures of full and high order fractional (1/2 and 1/3) alignment echoes are observed in the HHG signals measured from CO2 molecules at various time delays of the probe pulse. By increasing the time delay of the pump pulses, much higher order fractional (1/4) alignment echo is also observed in N2O molecules. With an analytic model based on the impulsive approximation, the spatiotemporal dynamics of the echo process are retrieved from the experiment. Compared to the typical molecular alignment revivals, high-order fractional molecular echoes are demonstrated to dephase more rapidly, which will open a new route towards the ultrashort-time measurement. The proposed HHG method paves an efficient way for accessing the high-order fractional echoes in molecules.

physics.chem-ph↗

arXiv2019

Determination of Electron Band Structure using Temporal Interferometry

We propose an all-optical method to directly reconstruct the band structure of semiconductors. Our scheme is based on the temporal Young's interferometer realized by high harmonic generation (HHG) with a few-cycle laser pulse. As a time-energy domain interferometric device, temporal interferometer encodes the band structure into the fringe in the energy domain. The relation between the band structure and the emitted harmonic frequencies is established. This enables us to retrieve the band structure from the HHG spectrum with a single-shot measurement. Our scheme paves the way to study matters under ambient conditions and to track the ultrafast modification of band structures.

physics.optics↗

arXiv2019

Photoelectron holographic interferometry to probe the longitudinal momentum offset at the tunnel exit

Laser-induced electron tunneling underlies numerous emerging spectroscopic techniques to probe attosecond electron dynamics in atoms and molecules. The improvement of those techniques requires an accurate knowledge of the exit momentum for the tunneling wave packet. Here we demonstrate a photoelectron interferometric scheme to probe the electron momentum longitudinal to the tunnel direction at the tunnel exit by measuring the photoelectron holographic pattern in an orthogonally polarized two-color laser pulse. In this scheme, we use a perturbative 400-nm laser field to modulate the photoelectron holographic fringes generated by a strong 800-nm pulse. The fringe shift offers a direct experimental access to the intermediate canonical momentum of the rescattering electron, allowing us to reconstruct the momentum offset at the tunnel exit with high accuracy. Our result unambiguously proves the existence of nonzero initial longitudinal momentum at the tunnel exit and provides fundamental insights into the non-quasi-static nature of the strong-field tunneling.

physics.atom-ph↗

arXiv2019

Reciprocal-space-trajectory perspective on high harmonic generation in solids

We revisit the mechanism of high harmonic generation (HHG) from solids by comparing HHG in laser fields with different ellipticities but constant maximum amplitude. It is shown that the cutoff of HHG is strongly extended in a circularly polarized field. Moreover, the harmonic yield with large ellipticity is comparable to or even higher than that in the linearly polarized field. To understand the underlying physics, we develop a reciprocal-space-trajectory method, which explains HHG in solids by a trajectory ensemble from different ionization times and different initial states in the reciprocal space. We show that the cutoff extension is related to an additional pre-acceleration step prior to ionization, which has been overlooked in solids. By analyzing the trajectories and the time-frequency spectrogram, we show that the HHG in solids cannot be interpreted in terms of the classical re-collision picture alone. Instead, the radiation should be described by the electronhole interband polarization, which leads to the unusual ellipticity dependence. We propose a new four-step model to understand the mechanism of HHG in solids.

physics.optics↗

arXiv2019

Molecular rotation movie filmed with high-harmonic generation

Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding information from the harmonic signals is usually painstaking due to the coherent nature of high-harmonic generation (HHG). Here we show that this obstacle can be effectively overcome by exploiting machine learning in HHS. Combining the machine learning with an angle-resolved HHS method, we demonstrate that the rich dynamics of molecular rotational wave packet is fully reconstructed from the angular distributions of HHG measured at various time delays of the probe pulse. The experimental retrievals are in good agreement with the numerical simulations. These findings provide a comprehensive picture of molecular rotation in space and time which will facilitate the development of related researches on molecular dynamics imaging.

physics.optics↗

arXiv2018

High harmonic generation with circularly polarized fields in solid: a quantum trajectory perspective

We investigate the high harmonic generation (HHG) in solids driven by laser fields with different ellipticities. The HHG spectra show a two-plateau structure within the energy gap between the valence band and the first conduction band. These two plateaus depend distinctly on the laser ellipticity. The first plateau is decreased while the second plateau is enhanced with increasing the laser ellipticity. To understand these phenomena, we develop an intuitive Reciprocal-Space- Trajectory (RST) method, with which HHG in solids is explained by a trajectory-ensemble from different initial states and different ionization times in the reciprocal space. In the framework of RST, we can not only quantitatively reproduce the HHG spectra, but also well understand the underlying physics of these phenomena, providing a deep insight into the mechanism of HHG in solids.

physics.optics↗

arXiv2018

Tomography of asymmetric molecular orbitals with one-color inhomogeneous field

We demonstrate to image asymmetric molecular orbitals via high-order harmonic generation in a one-color inhomogeneous field. Due to the broken inversion symmetry of the inhomogeneous field in space, the returning electrons with energy in a broad range can be forced to recollide from only one direction for all the orientation angles of molecules, which therefore can be used to reconstruct asymmetric molecular orbitals. Following the procedure of molecular orbital tomography, the highest occupied molecular orbital of CO is satisfactorily reconstructed with high-order harmonic spectra driven by the inhomogeneous field. This scheme is helpful to relax the requirement of laser conditions and also applicable to other asymmetric molecules.

physics.optics↗

arXiv2017

Scaling law of high harmonic generation in the framework of photon channel

Photon channel perspective on high harmonic generation (HHG) is proposed by quantizing both the driving laser and high harmonics. It is shown that the HHG yield can be expressed as a sum of the contribution of all the photon channels. From this perspective, the contribution of a specific photon channel follows a simple scaling law and the competition between the channels is well interpreted. Our prediction is shown to be in good agreement with the simulations by solving the time-dependent Schrodinger equation. It also can well explains the experimental results of the HHG in the noncollinear two-color field and bicicular laser field.

physics.atom-ph↗

arXiv2017

High-order harmonic generation of doped semiconductor

We investigate the high-order harmonic generation (HHG) in doped semiconductors. The HHG is simulated with the single-electron time-dependent Schrödinger equation (TDSE). The results show that the high-order harmonics in the second plateau generated from the doped semiconductors is about 1 to 3 orders of magnitude higher than those from the undoped semiconductor. The results are explained based on the analysis of the energy band structure and the time-dependent population imaging. Our work indicates that doping can effectively control the HHG in semiconductor.

physics.optics↗

arXiv2017

Attosecond probing of nuclear dynamics with trajectory-resolved high-harmonic spectroscopy

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajec- tories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H2 and D2 are used simultaneously to retrieve the nuclear dynamics on the attosecond and angstrom scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules.

physics.atom-ph↗

arXiv2017

Time-dependent population imaging for solid high harmonic generation

We propose an intuitive method, called time-dependent population imaging (TDPI), to map the dynamical processes of high harmonic generation (HHG) in solids by solving the time-dependent Schrödinger equation (TDSE). It is shown that the real-time dynamical characteristics of HHG in solids, such as the instantaneous photon energies of emitted harmonics, can be read directly from the energy-resolved population oscillations of electrons in the TDPIs. Meanwhile, the short and long trajectories of solid HHG are illustrated clearly from TDPI. By using the TDPI, we also investigate the effects of carrier-envelope phase (CEP) in few-cycle pulses and intuitively demonstrate the HHG dynamics driven by two-color fields. Our results show that the TDPI provides a powerful tool to study the ultrafast dynamics in strong fields for various laser-solid configurations and gain an insight into HHG processes in solids.

physics.atom-ph↗

arXiv2017

Diffractive molecular orbital tomography

High harmonic generation in the interaction of femtosecond lasers with atoms and molecules opens the path to molecular orbital tomography and to probe the electronic dynamics with attosecond-Ångström resolutions. Molecular orbital tomography requires both the amplitude and phase of the high harmonics. Yet the measurement of phases requires sophisticated techniques and represents formidable challenges at present. Here we report a novel scheme, called diffractive molecular orbital tomography, to retrieve the molecular orbital solely from the amplitude of high harmonics without measuring any phase information. We have applied this method to image the molecular orbitals of N$_2$, CO$_2$ and C$_2$H$_2$. The retrieved orbital is further improved by taking account the correction of Coulomb potential. The diffractive molecular orbital tomography scheme, removing the roadblock of phase measurement, significantly simplifies the molecular orbital tomography procedure and paves an efficient and robust way to the imaging of more complex molecules.

physics.optics↗

arXiv2016

Helicity reversion in high harmonic generation driven by bichromatic counterrotating circularly polarized laser fields

We investigate the polarization properties of high harmonics generated with the bichromatic counterrotating circularly polarized (BCCP) laser fields by numerically solving time-dependent Schrödinger equation (TDSE). It is found that, the helicity of the elliptically polarized harmonic emission is reversed at particular harmonic orders. Based on the time-frequency analysis and the classical three-step model, the correspondence between the positions of helicity reversions and the classical trajectories of continuum electrons is established. It is shown that, the electrons ionized at one lobe of laser field can be divided into different groups based on the different lobes they recombine at, and the harmonics generated by adjacent groups have opposite helicities. Our study performs a detailed analysis of high harmonics in terms of electron trajectories and depicts a clear and intuitive physical picture of the HHG process in BCCP laser field.

physics.atom-ph↗

arXiv2016

Quenching effect in below-threshold high harmonic generation

We theoretically demonstrate the quenching effect in below-threshold high harmonic generation (HHG) by using the time-dependent density-functional theory (TDDFT) and solving the time-dependent Schrödinger equation (TDSE). It is shown that the HHG is substantially suppressed in particular harmonic orders in the below-threshold region when multi-electron interaction comes into play. The position of the suppression is determined by the energy gap between the highest occupied orbital and the higher-lying orbital of the target. We show that the quenching effect is due to a new class of multi-electron dynamics involving electron-electron energy transfer, which is analog to the fluorescence quenching owing to the energy transfer between molecules in fluorescent material. This work reveals the important role of the multi-electron interaction on HHG especially in the below-threshold region.

physics.atom-ph↗