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Debobrata Rajak

Publications and source records attributed to Debobrata Rajak.

9 recordsLinked to original sources

Carrier-Envelope Phase Control of Orbital Angular Momentum in Solid-State High-Harmonic Generation

High-order harmonic generation (HHG) driven by optical vortices is a powerful route to produce structured light in different spectral regions. The nonlinear process transfers orbital angular momentum (OAM) from the driving field to the emitted harmonics according to the scaling law $l_q = q\times l$, a consequence of the rotational invariance and angular momentum conservation. Here, we show that, in the regime of few-cycle pulses, the topological charge (TC) of the harmonic radiation detected within a finite spectral window is no longer fixed by this scaling law alone, but is governed by the interplay between broken crystal inversion symmetry and carrier-envelope phase (CEP)-sensitive sub-cycle electron dynamics. By driving HHG in a ZnO crystal with few-cycle ($\approx 1.5$ cycles) vortex beams centered at 3.2~$μ$m, we observed that the measured TC becomes strongly CEP-dependent, switching between adjacent integer values, but only when the inversion symmetry is broken and the harmonic emission is CEP-sensitive. The TC switching vanishes when either condition is removed. Numerical analysis reveals that the TC switching originates from a CEP-controlled redistribution of spectral weight among spectrally overlapping harmonic orders, which changes the dominant OAM channel within the detection window. These results identify the CEP as a degree of freedom for tailoring the topological structure of high-harmonic radiation, pointing toward waveform-controlled structured attosecond light sources.

physics.optics

Twisting harmonics: Transfer of orbital angular momentum in solid-state high-harmonic generation

Although solid-state platforms underpin modern electronics, little is known about how intense ultrashort light pulses carrying orbital angular momentum (OAM) interact with solids. This gap persists even though, for more conventional light-matter interactions, the complex underlying electron dynamics can often be confined to a single Brillouin zone and described well within the dipole approximation. Previous studies were restricted to nonlinear, perturbative regimes, largely because the generation of intense ultrashort vortex pulses, particularly in the mid-infrared spectral regime, has remained a long-standing challenge. Consequently, the role of structured light in driving nonlinear, non-perturbative processes in solids, and the associated transfer of angular momentum during these interactions, has not been systematically explored. Here, we investigate solid-state high-harmonic generation (HHG) driven by intense ultrashort structured light using a versatile experimental approach applicable to different materials and geometries. We demonstrate that the OAM of the driving field is coherently transferred to the emitted harmonics. In particular, we show that the OAM is conserved independently of the crystal symmetry, the range of electronic interactions, and the presence of strong spin-orbit coupling. These results establish OAM-resolved HHG as a robust framework for characterizing and controlling angular momentum transfer in solid-state HHG and open new avenues for structured-light-driven quantum technologies and topological materials investigations.

physics.optics

A High Intensity Attosecond Light Source in Compact Geometry at ELI ALPS User Facility

High-order harmonic generation (HHG) has become a standard technique for producing attosecond XUV pulses in the laboratory, yet the high flux necessary for nonlinear XUV photoionization remains accessible to only a few research groups. Here, we introduce the SYLOS Compact high-harmonic beamline at ELI ALPS, specifically designed to provide the flux required for non-linear optics in the XUV. We present a detailed characterization of the beam line demonstrating its capability to generate and utilize both intense attosecond pulse trains and isolated attosecond pulses. We further showcase the two-XUV-photon double ionization of neon (Ne) and argon (Ar), achieved in a user campaign. The results underscore the beamline's capability to support cutting-edge attosecond experiments and investigations of ultrafast electron dynamics on the attosecond scale.

physics.optics

Sculpting ultrafast mid-infrared light for solid-state high harmonic generation

The ability to sculpt light in space, time, and polarization has revolutionized studies of light-matter interaction and enabled breakthroughs in optical communication, imaging, and ultrafast science. Among the many degrees of freedom of light, orbital angular momentum (OAM) further expands these capabilities by unlocking new regimes of control in information encoding, particle trapping and manipulation, and symmetry-driven selection rules. However, exploiting OAM to drive nonlinear, non-perturbative effects in solids remains challenging, especially in the mid-infrared (MIR) spectral regime-a key region for accessing these effects in ambient air, where spatial light modulators do not operate. Here, we circumvent this limitation by generating femtosecond, few-cycle MIR Bessel-Gauss vortex (BGV) and perfect optical vortices (POVs), using a robust, static spatial-shaping strategy. By utilizing these beams to drive nonlinear optical processes such as second-harmonic generation (SHG) and high-harmonic generation (HHG) in various solid-state materials, we show that the resulting harmonic beams faithfully inherit the structural characteristics of the drivers: the constant-intensity ring of the POVs is preserved across harmonic orders, while the BGV harmonic beams retain their intrinsic topological charge-dependent intensity profiles. Furthermore, by verifying the linear OAM up-scaling law, we confirm the conservation of OAM during SHG and HHG in solids. These results establish strong-field HHG in solids as a robust platform for synthesizing ultrafast structured harmonic light with controllable, high-value OAM.

physics.optics

Theory of Non-Dichroic Enantio-Sensitive Chiroptical Spectroscopy

We show that the photoelectron angular distributions produced by elliptical and cross-polarized two-color laser fields interacting with randomly oriented chiral molecules decompose into four irreducible representations of the $D_{2h}$ point group. One of these ($A_u$) corresponds to a non-dichroic enantiosensitive (NoDES) contribution. This NoDES contribution has opposite sign for opposite enantiomers but remains invariant under reversal of the field ellipticity, enabling chirality detection that is robust against variations of the relative phase between orthogonal field components. We propose a protocol to isolate this component using only two velocity-map imaging projections and validate it through numerical simulations. Our calculations, performed in the two-photon resonantly-enhanced ionization, multi-photon, and strong-field ionization regimes with cross-polarized two-color fields show that the NoDES signal reaches about 1\% of the energy-resolved ionization yield, comparable to photoelectron circular dichroism and much larger than standard magnetic-dipole chiroptical effects. NoDES spectroscopy thus provides a symmetry-protected and phase-robust route to probe molecular chirality on the ultrafast time scale. The experimental confirmation of our theory is presented in the companion paper [L. Fede et al., arXiv:2512.19062 (2025)].

physics.chem-ph

Non-Dichroic Enantio-Sensitive Chiroptical Spectroscopy

Chiroptical effects using circularly polarized light produce signals that change sign when switching either molecular handedness (enantiosensitivity) or the light helicity (circular dichroism). Here, we break this enantiosensitive-and-dichroic paradigm by measuring a new type of chiroptical signal which is enantiosensitive but not dichroic. We photoionize chiral molecules using a strong laser field and detect the three-dimensional photoelectron momentum distribution. The non-dichroic, enantiosensitive asymmetry is encoded in octupolar and higher multipolar terms in the photoelectron angular distribution, which appear in multiphoton ionization with elliptically polarized fields or cross polarized two-color fields. The robustness of the enantiosensitivity with respect to the relative phase between the vectorial components of the ionizing field represents an example of symmetry protection, and opens unexplored opportunities for imaging ultrafast dynamics in chiral molecules, such as enantiosensitive photoelectron spectroscopy with bright squeezed vacuum states.

physics.chem-ph

Ultrafast Polarization-Tunable Monochromatic Extreme Ultraviolet Source at High-Repetition-Rate

We report on the development of a high-order harmonic generation (HHG)-based ultrafast high-repetition-rate (250 kHz) monochromatic extreme ultraviolet (21.6 eV) source with polarization tunability, specifically designed for multi-modal dichroism in time- and angle-resolved photoemission spectroscopy. Driving HHG using an annular beam allows us to spatially separate the high-power 515 nm driving laser from the XUV beamlet while preserving the linear polarization axis angle tunability. This enables controlling the polarization state of the XUV radiation with a fixed all-reflective phase-shifter. This scheme leads to a source brightness of 5.7$\times$10$^{12}$ photons/s at 21.6 eV (up to 4$\times$10$^{11}$ photons/s on target) with ellipticities as high as 90$\%$.

physics.optics

Laser structured micro-targets generate MeV electron temperature at $4 \times 10^{16}$ W/cm$^2$

Relativistic temperature electrons higher than 0.5 MeV are generated typically with laser intensities of about 10$^{18}$ W/cm$^{2}$. Their generation with high repetition rate lasers that operate at non-relativistic intensities ($\simeq$10$^{16}$ W/cm$^{2}$) is cardinal for the realization of compact, ultra-short, bench-top electron sources. New strategies, capable of exploiting different aspects of laser-plasma interaction, are necessary for reducing the required intensity. We report here, a novel technique of dynamic target structuring of microdroplets, capable of generating 200 keV and 1 MeV electron temperatures at 1/100th of the intensity required by ponderomotive scaling($10^{18}$ W/cm$^2$) to generate relativistic electron temperature. Combining the concepts of pre-plasma tailoring, optimized scale length and micro-optics, this method achieves two-plasmon decay boosted electron acceleration with "non-ideal" ultrashort (25 fs) pulses at $4\times10^{16}$ W/cm$^2$, only. With shot repeatability at kHz, this precise in-situ targetry produces directed, imaging quality beam-like electron emission up to 6 MeV with milli-joule class lasers, that can be transformational for time-resolved, microscopic studies in all fields of science.

physics.plasm-ph

Bright, polarization-tunable high repetition rate extreme ultraviolet beamline for coincidence electron-ion imaging

After decades of supremacy of the Titanium:Sapphire technology, Ytterbium-based high-order harmonic sources are emerging as an interesting alternative for experiments requiring high flux of ultrashort extreme ultraviolet (XUV) radiation. In this article we describe a versatile experimental setup delivering XUV photons in the 10-50 eV range. The use of cascaded high-harmonic generation enables us to reach 1.8 mW of average power at 18 eV. Several spectral focusing schemes are presented, to select either a single harmonic or group of high-harmonics and thus an attosecond pulse train. In the perspective of circular dichroism experiments, we produce highly elliptical XUV radiation using resonant elliptical high-harmonic generation, and circularly polarized XUV by bichromatic bicircular high-harmonic generation. As a proof of principle experiment, we focus the XUV beam in a coincidence electron-ion imaging spectrometer, where we measure the photoelectron momentum angular distributions of xenon monomers and dimers.

physics.optics