We present single-molecule and macroscopic calculations showing that laser-induced Stark shifts contribute significantly to the phase of high-order harmonics from polar molecules. This is important for orbital tomography, where phases of field-free dipole matrix elements are needed in order to reconstruct molecular orbitals. We derive an analytical expression that allows the first-order Stark phase to be subtracted from experimental measurements.
The strong-field approximation for high-harmonic generation in near-infrared and infrared laser pulses is formulated in the accelerated Kramers-Henneberger frame. The accompanying physical picture is discussed and the nature of the leading-order term is contrasted with that of the three-step model following the strong-field-approximation formulation in the length or velocity gauges. The theory is illustrated by high-harmonic generation spectra for atomic hydrogen.
Quantum-mechanical investigation is presented to study single attosecond pulse generation by gating high-order harmonic emission from H$_2^+$ molecule in intense laser pulses with time-dependent ellipticity. The high-order harmonic generation from H$_2^+$ molecule in superposition of a left and a right-hand circularly polarized Gaussian pulse is studied and the effect of time duration and carrier-envelope phase of laser field on single attosecond pulse generation is investigated. Using laser field formed by combination of a left and a right-hand elliptically polarized Gaussian pulse, the effec…
High-order harmonic generation (HHG) from molecular ion HeH$^{2+}$ in two initial states of $1sσ$ (ground state) and $2pσ$ (first excited state) is investigated theoretically, in homogeneous and plasmonic-enhanced laser fields. The electron ionization and the enhancement of HHG yield in ground and first excited states, as the initial states, is studied and a strong orientation effect for ionization of electron in $2pσ$ state is discovered, that it can be used to reach a longer lifetime for the electron in the first excited state, which is responsible for the enhancement in HHG yield, during th…
The coherent radiation spectrum of two-level polar molecules with UV transition is studied at the multiphoton resonant excitation by a moderately strong laser field. The spectrum corresponding to harmonic generation and low-frequency radiation is investigated both analytically and numerically. Specifically, a mechanism for generation of intense smoothly tunable terahertz radiation by two-level molecular configurations (with dynamic Stark shifts) possessing permanent dipole moments, is considered.
In strong field laser physics it is a common practice to use the high-order harmonic cutoff to estimate the laser intensity of the pulse that generates the harmonic radiation. Based on the semiclassical arguments it is possible to find a direct relationship between the maximum value of the photon energy and the laser intensity. This approach is only valid if the electric field driving HHG is spatially homogenous. In laser-matter processes driven by plasmonics fields, the enhanced fields present a spatial dependence that strongly modifies the electron motion and consequently the laser driven ph…
High-order harmonic generation by a bicircular field, which consists of two coplanar counter-rotating circularly polarized fields of frequency $rω$ and $sω$ ($r$ and $s$ are integers), is investigated for a polyatomic molecule. This field possesses dynamical symmetry, which can be adjusted to the symmetry of the molecular Hamiltonian and used to investigate the molecular symmetry. For polyatomic molecules having the $C_{r+s}$ symmetry only the harmonics $n=q(r+s)\pm r$, $q=1,2,\ldots$, are emitted having the ellipticity $\varepsilon_n=\pm 1$. We illustrate this using the example of the planar …
High-order harmonic generation (HHG) by hydrogenlike atoms/ions in the uniform periodic electric field, formed by the two linearly polarized counterpropagating laser beams of relativistic intensities, is studied. The relativistic quantum theory of HHG in such fields, at which the impeding factor of relativistic magnetic drift of a strong wave can be eliminated, is presented arising from the Dirac equation. Specifically, a scheme of HHG in underdense plasma with the copropagating ultraintense laser and fast ion beams is proposed.
Two different induced effects of a laser falling edge on high-order harmonic generation are resolved by solving numerically full-dimensional electronic time-dependent Schrödinger equation beyond the Born-Oppenheimer approximation. The harmonic spectrum of H$_2^+$ and T$_2^+$ isotopes are compared to see the effects of a 4-cycle falling edge of a 800 nm, 15-cycle trapezoidal laser pulse of $I=$3 $\times 10^{14}$ Wcm$^{-2}$ intensity on harmonic emission spectrum. The harmonic emission at the laser falling part is negligible for H$_2^+$ due to ionization suppression, but considerable for T$_2^+$…
We investigate a single laser driven atom trapped in a non-harmonic potential. We present the performance of ground-state laser cooling and Doppler cooling and the signatures of the center-of-mass motion in the power spectrum of the scattered light. In order to illustrate the results we provide two explicit examples for the confining potential: the infinite square well and the Morse potential.
We investigate laser-driven vibronic transitions of a single two-level atomic ion in harmonic and hard wall traps. In the Lamb-Dicke regime, for tuned or detuned lasers with respect to the internal frequency of the ion, and weak or strong laser intensities, the vibronic transitions occur at well isolated "Rabi Resonances", where the detuning-adapted Rabi frequency coincides with the level spacing of the vibrational modes. These vibronic resonances are characterized as avoided crossings of the dressed levels (eigenvalues of the full Hamiltonian). Their peculiarities due to symmetry constraints …
The Quantum Polariton Hamiltonian that Reproduces the Same Mean Acceleration High-Harmonic Generation Spectra as the Classical Hamiltonian in Strong Laser Fields
A laser model is formulated in terms of quantum harmonic oscillators. Emitters in the low lasing states are usual harmonic oscillators, and emitters in the upper states are inverted harmonic oscillators. Diffusion coefficients, consistent with the model and necessary for solving quantum nonlinear laser equations analytically, are found. Photon number fluctuations of the lasing mode and fluctuations of the population of the lasing states are calculated. Collective Rabi splitting peaks are predicted in the intensity fluctuation spectra of the superradiant lasers. Population fluctuation mechanism…
Chiral discrimination with high harmonic generation (cHHG method) has been introduced in the recent work by R. Cireasa et al ( Nat. Phys. 11, 654 - 658, 2015). In its original implementation, the cHHG method works by detecting high harmonic emission from randomly oriented ensemble of chiral molecules driven by elliptically polarized field, as a function of ellipticity. Here we discuss future perspectives in the development of this novel method, the ways of increasing chiral dichroism using tailored laser pulses, new detection schemes involving high harmonic phase measurements, and concentratio…
Quantum-optical spectrometry is a recently developed shot-to-shot photon correlation-based method, namely using a quantum spectrometer (QS), that has been used to reveal the quantum optical nature of intense laser-matter interactions and connect the research domains of quantum optics (QO) and strong laser-field physics (SLFP). The method provides the probability of absorbing photons from a driving laser field towards the generation of a strong laser-field interaction product, such as high-order harmonics. In this case, the harmonic spectrum is reflected in the photon number distribution of the…
Non Born-Oppenheimer quantum dynamics of H$_{2}^{+}$ excited by shaped one-cycle laser pulses linearly polarized along the molecular axis have been studied by the numerical solution of the time-dependent Schrödinger equation within a %three-body three-dimensional model, including the internuclear separation, $R$, and the electron coordinates $z$ and $ρ$. Laser carrier frequencies corresponding to the wavelengths $λ_{l}=25$~nm through $λ_{l}=400$~nm were used and the amplitudes of the pulses were chosen such that the energy of H$_{2}^{+}$ was close to its dissociation threshold at the end of an…
