High-efficiency near-infrared optical parametric amplifier for intense, narrowband THz pulses tunable in the 4 to 19 THz region.

Dynamic control of material properties using strong-field, narrowband THz sources has drawn attention because it allows selective manipulation of quantum states on demand by coherent excitation of specific low-energy modes in solids. Yet, the lack of powerful narrowband lasers with frequencies in the range of a few to a few tens of THz has restricted the exploration of hidden states in condensed matter. Here, we report the optimization of an optical parametric amplifier (OPA) and the efficient generation of a strong, narrowband THz field. The OPA has a total conversion efficiency of > 55%, which is the highest value reported to date, with an excellent energy-stability of 0.7% RMS over 3 h. We found that the injection of a high-energy signal beam to a power amplification stage in an OPA leads to high-efficiency and a super-Gaussian profile. By difference-frequency generation of two chirped OPA signal pulses in an organic nonlinear crystal, we obtained a THz pulse with an energy of 3.2 µJ, a bandwidth of 0.5 THz, and a pulse duration of 860 fs tunable between the 4 and 19 THz regions. This corresponds to an internal THz conversion efficiency of 0.4% and a THz field strength of 6.7 MV/cm. This approach demonstrates an effective way to generate narrow-bandwidth, intense THz fields.

Time-Dependent Unitary Transformation Method in the Strong-Field-Ionization Regime with the Kramers-Henneberger Picture.

Time evolution operators of a strongly ionizing medium are calculated by a time-dependent unitary transformation (TDUT) method. The TDUT method has been employed in a quantum mechanical system composed of discrete states. This method is especially helpful for solving molecular rotational dynamics in quasi-adiabatic regimes because the strict unitary nature of the propagation operator allows us to set the temporal step size to large; a tight limitation on the temporal step size (δt<<1) can be circumvented by the strict unitary nature. On the other hand, in a strongly ionizing system where the Hamiltonian is not Hermitian, the same approach cannot be directly applied because it is demanding to define a set of field-dressed eigenstates. In this study, the TDUT method was applied to the ionizing regime using the Kramers-Henneberger frame, in which the strong-field-dressed discrete eigenstates are given by the field-free discrete eigenstates in a moving frame. Although the present work verifies the method for a one-dimensional atom as a prototype, the method can be applied to three-dimensional atoms, and molecules exposed to strong laser fields.

Field-free molecular orientation by delay- and polarization-optimized two fs pulses.

Unless the molecular axis is fixed in the laboratory frame, intrinsic structural information of molecules can be averaged out over the various rotational states. The macroscopic directional properties of polar molecules have been controlled by two fs pulses with an optimized delay. In the method, the first one-color laser pulse provokes molecular alignment. Subsequently, the molecular sample is irradiated with the second two-color laser pulse, when the initial even-J states are aligned, and the odd-J states are anti-aligned in the thermal ensemble. The second pulse selectively orients only the aligned even-J states in the same direction, which results in significant enhancement of the net degree of orientation. This paper reports the results of simulations showing that the two-pulse technique can be even more powerful when the second pulse is cross-polarized. This study shows that the alignment and orientation can be very well synchronized temporally because the crossed field does not disturb the preformed alignment modulation significantly, suggesting that the molecules are very well confined in the laboratory frame. This cross-polarization method will serve as a promising technique for studying ultrafast molecular spectroscopy in a molecule-fixed frame.

Path integral formulation of light propagation in a static collisionless plasma, and its application to dynamic plasma.

In many studies on the laser impinging on a plasma surface, an assumption is made that the reflection of a laser pulse propagating to a plasma surface takes place only at the turning point, at which the plasma density exceeds the critical one. A general reflection amplitude of light R from an arbitrary inhomogeneous medium can be obtained by solving a Riccati-type integral equation, which can be solved analytically in low-reflection conditions, i.e., |R|2 ≪ 1. In this work, we derive an intuitive analytic solution for the reflection amplitude of light R from a plasma surface by integrating all possible reflection paths given by the Fresnel equation. In the low-reflection condition, reflection paths having only one reflection event can be used. By considering the higher-order reflection paths, our analytic expression can describe reflection in the high-reflection condition. We show the results of a one-dimensional particle-in-cell simulation to support our discussions. Since our model derived for static plasmas is well corroborated by the simulation results, it can be a useful tool for analyzing light reflection from dynamically varying plasmas.

Development of a plasma shutter applicable to 100-mJ-class, 10-ns laser pulses and the characterization of its performance.

For the purpose of preparing a sample of aligned and oriented molecules in the laser-field-free condition, we developed a plasma shutter, which enables laser pulses with 100-mJ-class, 10-ns pulse durations to be rapidly turned off within ∼150 fs. Inthis work, the residual field intensity after the rapid turn off is carefully examined by applying the shaped laser pulse to OCS molecules in the rotational ground state. Based on the comparison between the observation of alignment revivals of the OCS molecules and the results of numerical simulations, we demonstrate that the residual field intensity is actually negligible (below 0.4% of the peak intensity) and, if any, does not influence the alignment and orientation dynamics at all.