Search

Low frequency Raman spectroscopy resolves the slow vibrations resulting from collective motions of molecular structures. This frequency region is extremely challenging to access via other multidimensional methods such as 2D-IR. In this paper, we describe a new scheme which measures 2D Raman spectra in the low frequency regime. We separate the pulse into a spectrally shaped pump and a transform-limited probe, which can be distinguished by their polarization states. Low frequency 2D Raman spectra in liquid tetrabromoethane are presented, revealing coupling dynamics at frequencies as low as 115 cm -1 . The experimental results are supported by numerical simulations which replicate the key features of the measurement. This method opens the door for the deeper exploration of vibrational energy surfaces in complex molecular structures.

Solid-state high-harmonic generation (HHG) by an intense infra-red (IR) laser field offers a new route to generate coherent attosecond light pulses in the extreme ultraviolet regime. The propagation of the IR driving field in the dense solid medium is accompanied by non-linear processes which shape the generating waveform. In this work, we introduce a monolithic scheme in which we both exploit the non-linear propagation to manipulate a two color driving field, as well as generate high harmonics within a single crystal. We show that the resulting non-commensurate, bi-chromatic, generating field provides precise control over the periodicity of the HHG process. This control enables us to manipulate the spectral positions of the discrete harmonic peaks. Our method advances solid-state HHG spectroscopy, and offers a simple route towards tunable, robust XUV sources.

High-harmonic generation (HHG) is a powerful tool to generate coherent attosecond light pulses in the extreme ultraviolet. However, the low conversion efficiency of HHG at the single atom level poses a significant practical limitation for many applications. Enhancing the efficiency of the process defines one of the primary challenges in the application of HHG as an advanced XUV source. In this work, we demonstrate a new mechanism, which in contrast to current methods, enhances the HHG conversion efficiency purely on a single particle level. We show that using a bichromatic driving field, sub-optical-cycle control and enhancement of the tunnelling ionization rate can be achieved, leading to enhancements in HHG efficiency by up to two orders of magnitude. Our method advances the perspectives of HHG spectroscopy, where isolating the single particle response is an essential component, and offers a simple route toward scalable, robust XUV sources.

Phase measurement is a long-standing challenge in a wide range of applications, from X-ray imaging to astrophysics and spectroscopy. While in some scenarios the phase is resolved by an interferometric measurement, in others it is reconstructed via numerical optimization, based on some a-priori knowledge about the signal. The latter commonly use iterative algorithms, and thus have to deal with their convergence, stagnation, and robustness to noise. Here we combine these two approaches and present a new scheme, termed double blind Fourier holography, providing an efficient solution to the phase problem in two dimensions, by solving a system of linear equations. We present and experimentally demonstrate our approach for the case of lens-less imaging.

Ultrafast science is inherently, due to the lack of fast enough detectors and electronics, based on nonlinear interactions. Typically, however, nonlinear measurements require significant powers and often operate in a limited spectral range. Here we overcome the difficulties of ultraweak ultrafast measurements by precision time-domain localization of spectral components. We utilize this for linear self-referenced characterization of pulse trains having ∼ 1 photon per pulse, a regime in which nonlinear techniques are impractical, at a temporal resolution of ∼ 10 fs. This technique does not only set a new scale of sensitivity in ultrashort pulse characterization, but is also applicable in any spectral range from the near-infrared to the deep UV.