Valleytronics in bulk MoS2 with a topologic optical field.

The valley degree of freedom1-4 of electrons in materials promises routes towards energy-efficient information storage with enticing prospects for quantum information processing5-7. Current challenges in utilizing valley polarization are symmetry conditions that require monolayer structures8,9 or specific material engineering10-13, non-resonant optical control to avoid energy dissipation and the ability to switch valley polarization at optical speed. We demonstrate all-optical and non-resonant control over valley polarization using bulk MoS2, a centrosymmetric material without Berry curvature at the valleys. Our universal method utilizes spin angular momentum-shaped trefoil optical control pulses14,15 to switch the material's electronic topology and induce valley polarization by transiently breaking time and space inversion symmetry16 through a simple phase rotation. We confirm valley polarization through the transient generation of the second harmonic of a non-collinear optical probe pulse, depending on the trefoil phase rotation. The investigation shows that direct optical control over the valley degree of freedom is not limited to monolayer structures. Indeed, such control is possible for systems with an arbitrary number of layers and for bulk materials. Non-resonant valley control is universal and, at optical speeds, unlocks the possibility of engineering efficient multimaterial valleytronic devices operating on quantum coherent timescales.

Field-resolved infrared spectroscopy of biological systems.

The proper functioning of living systems and physiological phenotypes depends on molecular composition. Yet simultaneous quantitative detection of a wide variety of molecules remains a challenge1-8. Here we show how broadband optical coherence opens up opportunities for fingerprinting complex molecular ensembles in their natural environment. Vibrationally excited molecules emit a coherent electric field following few-cycle infrared laser excitation9-12, and this field is specific to the sample's molecular composition. Employing electro-optic sampling10,12-15, we directly measure this global molecular fingerprint down to field strengths 107 times weaker than that of the excitation. This enables transillumination of intact living systems with thicknesses of the order of 0.1 millimetres, permitting broadband infrared spectroscopic probing of human cells and plant leaves. In a proof-of-concept analysis of human blood serum, temporal isolation of the infrared electric-field fingerprint from its excitation along with its sampling with attosecond timing precision results in detection sensitivity of submicrograms per millilitre of blood serum and a detectable dynamic range of molecular concentration exceeding 105. This technique promises improved molecular sensitivity and molecular coverage for probing complex, real-world biological and medical settings.

Few-cycle mid-infrared pulses from BaGa2GeSe6.

BaGa2GeSe6 (BGGSe) is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold. A numerical study shows the material's capacity for octave-spanning mid-infrared pulse generation up to 18 µm. In a first experiment, we show that a long crystal length of 2.6 mm yields a pulse energy of 21 pJ at 100 MHz with a spectral bandwidth covering 5.8 to 8.5 µm. The electric field of the carrier-envelope-phase stable pulse is directly measured with electro-optical sampling and reveals a pulse duration of 91 fs, which corresponds to sub-four optical cycles, thus confirming some of the prospects of the material for ultrashort pulse generation and mid-infrared spectroscopy.

Interferometric delay tracking for low-noise Mach-Zehnder-type scanning measurements.

Precise delay control is of paramount importance in optical pump-probe measurements. Here, we report on a high-precision delay tracking technique for mechanical scanning measurements in a Mach-Zehnder interferometer configuration. The setup employs a 1.55-µm continuous-wave laser beam propagating along the interferometer arms. Sinusoidal phase modulation at 30 MHz, and demodulation of the interference signal at the fundamental frequency and its second harmonic, enables delay tracking with sampling rates of up to 10 MHz. At an interferometer arm length of 1 m, root-mean-square error values of the relative delay tracking below 10 attoseconds for both stationary and mechanically scanned (0.2 mm/s) operation are demonstrated. By averaging several scans, a precision of the delay determination better than 1 as is reached. We demonstrate this performance with a mechanical chopper periodically interrupting one of the interferometer arms, which opens the door to the combination of high-sensitivity lock-in detection with (sub-)attosecond-precision relative delay determination.

High-power, 1-ps, all-Yb:YAG thin-disk regenerative amplifier.

We report a 100 W, 20 mJ, 1-ps, all-Yb:YAG thin-disk regenerative amplifier seeded by a microjoule-level Yb:YAG thin-disk Kerr-lens mode-locked oscillator. The regenerative amplifier is implemented in a chirped pulse amplification system and operates at an ambient temperature in air, delivering ultrastable output pulses at a 5 kHz repetition rate and with a root mean square power noise value of less than 0.5%. Second harmonic generation of the amplifier's output in a 1.5 mm-thick BBO crystal results in more than 70 W at 515 nm, making the system an attractive source for pumping optical parametric chirped pulse amplifiers in the visible and near-infrared spectral ranges.