Necklace-structured high-harmonic generation for low-divergence, soft x-ray harmonic combs with tunable line spacing

Rego, Laura; Brooks, Nathan J.; Nguyen, Quynh L.; Román, Julio San; Binnie, Iona; Plaja, Luis; Kapteyn, Henry C.; Murnane, Margaret M.; Hernández-García, Carlos

doi:10.1126/sciadv.abj7380

Cited by 26 publications

(17 citation statements)

References 61 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Further studies of tight focusing of such beams are required. Fortunately, the versatility of the HHG process offers different lensless focusing approaches ,, that could be used to achieve low divergence beams without the need for focusing optics. In this regard, we also note that the EUV wavefront sensing allows for the determination of the HHG beam waist position from the measured wavefront curvature radius, therefore, offering the possibility to investigate the optics-less focusing aspect of high-OAM EUV vortex beams.…”

Section: Discussionmentioning

confidence: 99%

“…On the one hand, HHG driven by a combination of two vortex beams of different topological charges in a noncollinear geometry leads to an array of spatially separated beams, each carrying a different OAM, and hence, it has provided an additional knob to control the topological charge of EUV vortex beams. , On the other hand, in a collinear HHG configuration involving two distinct topological charge drivers, theoretical investigations predict a more involved OAM distribution . Indeed, by properly selecting the OAM of the two driving beams, several properties, such as polarization, , self-torque, and spectral line spacing of high-order harmonic beams, can be tailored. Moreover, the effect of the nonperturbative harmonic intrinsic phase has been studied numerically in ref and can further increase the OAM content.…”

mentioning

confidence: 99%

“…24,25 On the other hand, in a collinear HHG configuration involving two distinct topological charge drivers, theoretical investigations predict a more involved OAM distribution. 34 Indeed, by properly selecting the OAM of the two driving beams, several properties, such as polarization, 27,28 self-torque, 29 and spectral line spacing of high-order harmonic beams, 35 can be tailored. Moreover, the effect of the nonperturbative harmonic intrinsic phase has been studied numerically in ref 34 and can further increase the OAM content.…”

mentioning

confidence: 99%

See 2 more Smart Citations

Characterization of Extreme Ultraviolet Vortex Beams with a Very High Topological Charge

et al. 2022

Self Cite

View full text Add to dashboard Cite

Recent developments of high harmonic generation (HHG) have enabled the production of structured extreme-ultraviolet (EUV) ultrafast laser beams with orbital angular momentum (OAM). Precise manipulation and characterization of their spatial structure are paramount for their application in state-of-the-art ultrafast studies. In this work, we report the generation and characterization of EUV vortex beams bearing a topological charge as high as 100. Thanks to OAM conservation, HHG in noble gases offers a unique opportunity to generate ultrafast harmonic beams with a high topological charge from low charge infrared vortex beams. A high-resolution Hartmann wavefront sensor allows us to perform a complete spatial characterization of the amplitude and phase of the 25th harmonic beam (32.6 nm), revealing very high-topological charges in the EUV spectral regime. Our experimental results, supported by numerical HHG simulations, demonstrate the linear upscaling of the OAM of the high-order harmonics with that of low-charge driving vortex beams, showing the sensitiveness of the OAM content to the purity of the driving beam. The generation of structured EUV beams carrying large topological charges brings in the promising scenario of OAM transfer from light to matter at both macroscopic and microscopic scales.

show abstract

Section: Discussionmentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

See 1 more Smart Citation

Characterization of Extreme Ultraviolet Vortex Beams with a Very High Topological Charge

et al. 2022

Self Cite

View full text Add to dashboard Cite

show abstract

“…In the last decade, structured vortex light has been successfully applied to drive highly non-linear interactions in matter, such as structured high-order harmonic generation (HHG), leading to the creation of ultrashort structured pulses in the extremeultraviolet domain [25][26][27][28][29][30][31][32][33][34][35] . An interesting aspect of this capacity to structure the HHG radiation is that it allows us to spatially separate harmonics radiation with different properties, enabling control over the polarization of ultrashort pulses 35,36 or their spectral content 37 .…”

Section: Introductionmentioning

confidence: 99%

Structuring the local handedness of synthetic chiral light: global chirality versus polarization of chirality

Rego

Ayuso

2022

Preprint

Self Cite

View full text Add to dashboard Cite

Synthetic chiral light enables ultrafast and highly efficient imaging of molecular chirality. Unlike standard circularly polarized light, the handedness of synthetic chiral light does not rely on the spatial structure of the light field: it is encoded locally, in the chiral trajectory that the tip of the electric-field vector draws in time, at each point in space. Being locally chiral, already within the electric-dipole approximation, synthetic chiral light is a highly efficient chiral photonic reagent. Synthetic chiral light that is locally and globally chiral allows us to selectively quench the nonlinear response of a selected molecular enantiomer while maximizing it in its mirror twin at the level of total signal intensities. Synthetic chiral light that exhibits polarization of chirality allows us to realize a chiral version of Young’s double-slit experiment that leads to enantio-sensitive light bending. Here we connect these two new concepts and show how one can structure the local and global handedness of synthetic chiral light in space, and how these local and global properties are imprinted in the enantio-sensitive response of the chiral molecules, creating new opportunities for ultrafast, all-optical and highly efficient imaging of molecular chirality.

show abstract

“…1. Our proposal exploits the potential of structuring light's polarization [58][59][60][61][62][63][64] to realize an enantio-sensitive interferometer for efficient chiral recognition that separates the nonlinear response of opposite molecular enantiomers in space. We consider an ultrashort and tightly focused Gaussian beam with elliptical polarization, where the pulse duration is only a few cycles, and the size of the beam waist is only a few times larger than its wavelength.…”

mentioning

confidence: 99%

Tilting light's polarization plane to spatially separate the nonlinear optical response of chiral molecules on ultrafast timescales

Rego¹,

Ayuso²

2022

Preprint

Self Cite

View full text Add to dashboard Cite

Distinguishing between the left-and right-handed versions of a chiral molecule (enantiomers) is vital, but also inherently difficult. Traditional optical methods using elliptically or circularly polarized light rely on weak linear effects which arise beyond the electric-dipole approximation, posing major limitations for time resolving ultrafast chiral molecular dynamics. Here we show how, by tilting the plane of polarization of an ultrashort burst of intense elliptically polarized light, towards its propagation direction, we can turn the light field into a highly efficient chiro-optical tool. This "forward tilting" can be achieved by focusing the beam tightly, creating structured light which exhibits a nontrivial polarization pattern in space. We demonstrate that our structured field allows us to realize an interferometer for efficient chiral recognition that separates the nonlinear optical response of left-and right-handed molecules in space. Our work provides a simple, yet highly efficient, way of spatially structuring the polarization of light to image molecular chirality, with extreme enantio-sensitivity and on ultrafast time scales.Chirality plays key roles in nature, from dictating the behaviour of subatomic particles 1 to selecting the mating partners of snails 2 . In general, an object is chiral when it cannot be superimposed to its mirror image, with our hands being the typical example. In chemistry, the left-and right-handed versions of a chiral molecule are called enantiomers. Their handedness is essential in molecular recognition, and thus distinguishing between opposite enantiomers is vital in many different fields, including bio-medicine, organic chemistry or materials science. However, chiral distinction is challenging, as opposite molecular enantiomers behave identically unless they interact with another chiral object, such as another chiral molecule or chiral light.Cutting-edge laser technology creates exciting opportunities for studying molecular chirality, allowing us to access the natural temporal and spatial scales of molecules with unprecedented sub-femtosecond and sub-Angstrom resolution 3 . Important breakthroughs include the real-time observation of electronic currents in atoms 4-6 , molecules [7][8][9] , and solids [10][11][12] . Yet, despite these groundbreaking achievements, imaging the three-dimensional chiral currents governing enantio-sensitive chemical reactions is still very challenging, as natural chiral light is ill-suited for this purpose.Circularly polarized light is a standard tool for chiral recognition. In photo-absorption circular dichroism, one measures the differential absorption of left-and right-handed circularly polarized photons, ∆I = I L − I R , in a chiral medium 13 . While ∆I has opposite sign in opposite in opposite molecular enantiomers, it is only a small fraction of the total intensity of the optical response (I L I R ), making chiral recognition challenging, especially on ultrafast time scales. The reason behind this weak enantio-sensitivity is that circularl...

show abstract

Necklace-structured high-harmonic generation for low-divergence, soft x-ray harmonic combs with tunable line spacing

Cited by 26 publications

References 61 publications

Characterization of Extreme Ultraviolet Vortex Beams with a Very High Topological Charge

Characterization of Extreme Ultraviolet Vortex Beams with a Very High Topological Charge

Structuring the local handedness of synthetic chiral light: global chirality versus polarization of chirality

Tilting light's polarization plane to spatially separate the nonlinear optical response of chiral molecules on ultrafast timescales

Contact Info

Product

Resources

About