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1.
Opt Express ; 30(9): 15546-15555, 2022 Apr 25.
Artículo en Inglés | MEDLINE | ID: mdl-35473271

RESUMEN

Recent studies in high-order harmonic generation (HHG) in solid targets reveal new scenarios of extraordinary rich electronic dynamics, in comparison to the atomic and molecular cases. For the later, the main aspects of the process can be described semiclassically in terms of electrons that recombine when the trajectories revisit the parent ion. HHG in solids has been described by an analogous mechanism, in this case involving electron-hole pair recombinations. However, it has been recently reported that a substantial part of the HHG emission corresponds to situations where the electron and hole trajectories do not overlap in space. According to the present knowledge, HHG from this imperfect recollisions reflects the quantum nature of the process, arising in systems with large Berry curvatures or for elliptically polarized driving fields. In this work, we demonstrate that imperfect recollisions are also relevant in the more general case. We show the signature of such recollisions in the HHG spectrum from monolayer graphene -a system with null Berry curvature- irradiated by linearly polarized driving fields. Our calculations also reveal that imperfect multiple-order recollisions contribute to the harmonic emission when electron-hole excursion times exceed one cycle of the driving field. We believe that our work adds a substantial contribution to the full understanding of the sub-femtosecond dynamics of HHG in solid systems.

2.
Opt Express ; 29(2): 2488-2500, 2021 Jan 18.
Artículo en Inglés | MEDLINE | ID: mdl-33726443

RESUMEN

The efficiency of high-harmonic generation (HHG) from a macroscopic sample is strongly linked to the proper phase matching of the contributions from the microscopic emitters. We develop a combined micro+macroscopic theoretical model that allows us to distinguish the relevance of high-order harmonic phase matching in single-layer graphene. For a Gaussian driving beam, our simulations show that the relevant HHG emission is spatially constrained to a phase-matched ring around the beam axis. This remarkable finding is a direct consequence of the non-perturbative behavior of HHG in graphene-whose harmonic efficiency scaling is similar to that already observed in gases- and bridges the gap between the microscopic and macroscopic HHG in single-layer graphene.

3.
Opt Express ; 29(23): 38119-38128, 2021 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-34808871

RESUMEN

High-harmonic generation (HHG) is a unique tabletop light source with femtosecond-to-attosecond pulse duration and tailorable polarization and beam shape. Here, we use counter-rotating femtosecond laser pulses of 0.8 µm and 2.0 µm to extend the photon energy range of circularly polarized high-harmonics and also generate single-helicity HHG spectra. By driving HHG in helium, we produce circularly polarized soft x-ray harmonics beyond 170 eV-the highest photon energy of circularly polarized HHG achieved to date. In an Ar medium, dense spectra at photon energies well beyond the Cooper minimum are generated, with regions composed of a single helicity-consistent with the generation of a train of circularly polarized attosecond pulses. Finally, we show theoretically that circularly polarized HHG photon energies can extend beyond the carbon K edge, extending the range of molecular and materials systems that can be accessed using dynamic HHG chiral spectro-microscopies.

4.
Opt Express ; 28(13): 19760-19771, 2020 Jun 22.
Artículo en Inglés | MEDLINE | ID: mdl-32672246

RESUMEN

We study high-order harmonic generation (HHG) in armchair-type single-wall carbon nanotubes (SWNTs) driven by ultrashort, mid-infrared laser pulses. For a SWNT with chiral indices (n, n), we demonstrate that HHG is dominated by bands |m| = n - 1 and that the cut-off frequency saturates with intensity, as it occurs in the case of single layer graphene. As a consequence, HHG in SWNTs can be described effectively as a one-dimensional periodic system, whose high-frequency emission can be modified through the proper control of the structural parameters. Additionally, we show that the HHG mechanism in nanotubes has some similarities to that previously reported in single layer graphene. However, as a main difference, the electron-hole pair excitation in SWNTs is connected to the non-adiabatic crossing through the first van Hove singularity of the |m| = n - 1 bands, instead of the crossing through the Dirac point that takes place in graphene.

5.
Opt Lett ; 45(20): 5636-5639, 2020 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-33057245

RESUMEN

Ultrafast laser pulses generated at the attosecond timescale represent a unique tool to explore the fastest dynamics in matter. An accurate control of their properties, such as polarization, is fundamental to shape three-dimensional laser-driven dynamics. We introduce a technique to generate attosecond pulse trains whose polarization state varies from pulse to pulse. This is accomplished by driving high-harmonic generation with two time-delayed bichromatic counter-rotating fields with proper orbital angular momentum (OAM) content. Our simulations show that the evolution of the polarization state along the train can be controlled via OAM, pulse duration, and time delay of the driving fields. We, thus, introduce an additional control into structured attosecond pulses that provides an alternative route to explore ultrafast dynamics with potential applications in chiral and magnetic materials.

6.
Opt Express ; 27(5): 7776-7786, 2019 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-30876335

RESUMEN

High harmonic generation in atomic or molecular targets stands as a robust mechanism to produce coherent ultrashort pulses with controllable polarization in the extreme-ultraviolet. However, the production of elliptically or circularly-polarized harmonics is not straightforward, demanding complex combinations of elliptically or circularly-polarized drivers, or the use of molecular alignment techniques. Nevertheless, recent studies show the feasibility of high-harmonic generation in solids. In contrast with atoms and molecules, solids are high-density targets and therefore more efficient radiation sources. Among solid targets, 2D materials are of special interest due to their particular electronic structure, which conveys special optical properties. In this paper, we present theoretical calculations that demonstrate an extraordinary complex light-spin conversion in single-layer graphene irradiated at non perturbative intensities. Linearly-polarized drivings result in the emission of elliptically-polarized harmonics, and elliptically-polarized drivings may result in linearly-polarized or ellipticity-reversed harmonics. In addition, we demonstrate the ultrafast temporal modulation of the harmonic ellipticity.

7.
Phys Rev Lett ; 122(20): 203201, 2019 May 24.
Artículo en Inglés | MEDLINE | ID: mdl-31172784

RESUMEN

High-order harmonic generation stands as a unique nonlinear optical up-conversion process, mediated by a laser-driven electron recollision mechanism, which has been shown to conserve energy, linear momentum, and spin and orbital angular momentum. Here, we present theoretical simulations that demonstrate that this process also conserves a mixture of the latter, the torus-knot angular momentum J_{γ}, by producing high-order harmonics with driving pulses that are invariant under coordinated rotations. We demonstrate that the charge J_{γ} of the emitted harmonics scales linearly with the harmonic order, and that this conservation law is imprinted onto the polarization distribution of the emitted spiral of attosecond pulses. We also demonstrate how the nonperturbative physics of high-order harmonic generation affect the torus-knot angular momentum of the harmonics, and we show that this configuration harnesses the spin selection rules to channel the full yield of each harmonic into a single mode of controllable orbital angular momentum.

8.
Proc Natl Acad Sci U S A ; 112(46): 14206-11, 2015 Nov 17.
Artículo en Inglés | MEDLINE | ID: mdl-26534992

RESUMEN

We demonstrate, to our knowledge, the first bright circularly polarized high-harmonic beams in the soft X-ray region of the electromagnetic spectrum, and use them to implement X-ray magnetic circular dichroism measurements in a tabletop-scale setup. Using counterrotating circularly polarized laser fields at 1.3 and 0.79 µm, we generate circularly polarized harmonics with photon energies exceeding 160 eV. The harmonic spectra emerge as a sequence of closely spaced pairs of left and right circularly polarized peaks, with energies determined by conservation of energy and spin angular momentum. We explain the single-atom and macroscopic physics by identifying the dominant electron quantum trajectories and optimal phase-matching conditions. The first advanced phase-matched propagation simulations for circularly polarized harmonics reveal the influence of the finite phase-matching temporal window on the spectrum, as well as the unique polarization-shaped attosecond pulse train. Finally, we use, to our knowledge, the first tabletop X-ray magnetic circular dichroism measurements at the N4,5 absorption edges of Gd to validate the high degree of circularity, brightness, and stability of this light source. These results demonstrate the feasibility of manipulating the polarization, spectrum, and temporal shape of high harmonics in the soft X-ray region by manipulating the driving laser waveform.

9.
Opt Express ; 25(9): 10126-10144, 2017 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-28468388

RESUMEN

We investigate the macroscopic physics of noncollinear high harmonic generation (HHG) at high pressures. We make the first experimental demonstration of phase matching of noncollinear high-order-difference-frequency generation at ionization fractions above the critical ionization level, which normally sets an upper limit on the achievable cutoff photon energies. Additionally, we show that noncollinear high-order-sum-frequency generation requires much higher pressures for phase matching than single-beam HHG does, which mitigates the short interaction region in this geometry. We also dramatically increase the experimentally realized cutoff energy of noncollinear circularly polarized HHG, reaching photon energies of 90 eV. Finally, we achieve complete angular separation of high harmonic orders without the use of a spectrometer.

10.
Phys Rev Lett ; 119(6): 063201, 2017 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-28949633

RESUMEN

High harmonics driven by two-color counterrotating circularly polarized laser fields are a unique source of bright, circularly polarized, extreme ultraviolet, and soft x-ray beams, where the individual harmonics themselves are completely circularly polarized. Here, we demonstrate the ability to preferentially select either the right or left circularly polarized harmonics simply by adjusting the relative intensity ratio of the bichromatic circularly polarized driving laser field. In the frequency domain, this significantly enhances the harmonic orders that rotate in the same direction as the higher-intensity driving laser. In the time domain, this helicity-dependent enhancement corresponds to control over the polarization of the resulting attosecond waveforms. This helicity control enables the generation of circularly polarized high harmonics with a user-defined polarization of the underlying attosecond bursts. In the future, this technique should allow for the production of bright highly elliptical harmonic supercontinua as well as the generation of isolated elliptically polarized attosecond pulses.

11.
Proc Natl Acad Sci U S A ; 111(23): E2361-7, 2014 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-24850866

RESUMEN

High harmonic generation driven by femtosecond lasers makes it possible to capture the fastest dynamics in molecules and materials. However, to date the shortest subfemtosecond (attosecond, 10(-18) s) pulses have been produced only in the extreme UV region of the spectrum below 100 eV, which limits the range of materials and molecular systems that can be explored. Here we experimentally demonstrate a remarkable convergence of physics: when midinfrared lasers are used to drive high harmonic generation, the conditions for optimal bright, soft X-ray generation naturally coincide with the generation of isolated attosecond pulses. The temporal window over which phase matching occurs shrinks rapidly with increasing driving laser wavelength, to the extent that bright isolated attosecond pulses are the norm for 2-µm driving lasers. Harnessing this realization, we experimentally demonstrate the generation of isolated soft X-ray attosecond pulses at photon energies up to 180 eV for the first time, to our knowledge, with a transform limit of 35 attoseconds (as), and a predicted linear chirp of 300 as. Most surprisingly, advanced theory shows that in contrast with as pulse generation in the extreme UV, long-duration, 10-cycle, driving laser pulses are required to generate isolated soft X-ray bursts efficiently, to mitigate group velocity walk-off between the laser and the X-ray fields that otherwise limit the conversion efficiency. Our work demonstrates a clear and straightforward approach for robustly generating bright isolated attosecond pulses of electromagnetic radiation throughout the soft X-ray region of the spectrum.


Asunto(s)
Algoritmos , Rayos Láser , Modelos Teóricos , Rayos X , Química Física/instrumentación , Química Física/métodos , Fotones , Espectroscopía Infrarroja por Transformada de Fourier , Factores de Tiempo
12.
Phys Rev Lett ; 117(16): 163202, 2016 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-27792355

RESUMEN

High-order harmonic generation (HHG) has been recently proven to produce extreme-ultraviolet (XUV) vortices from the nonlinear conversion of infrared twisted beams. Previous works have demonstrated a linear scaling law of the vortex charge with the harmonic order. We demonstrate that this simple law hides an unexpectedly rich scenario for the buildup of orbital angular momentum (OAM) due to the nonperturbative behavior of HHG. The complexity of these twisted XUV beams appears only when HHG is driven by nonpure vortex modes, where the XUV OAM content is dramatically increased. We explore the underlying mechanisms for this diversity and derive a general conservation rule for the nonperturbative OAM buildup. The simple scaling found in previous works corresponds to the collapse of this scenario for the particular case of pure (single-mode) OAM driving fields.

13.
Plant Cell Rep ; 35(2): 303-16, 2016 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-26518427

RESUMEN

KEY MESSAGE: Using in silico and functional analyses, we cloned and validated the expression profile of an inducible soybean promoter (GmERF3) along with its novel wound-induced and delayed expression (WIDE) element. Promoters and their contributing promoter elements are the main regulators of gene expression at the transcriptional level. Although the Ethylene Response Factor (ERF) gene family is one of the most well-studied stress-responsive gene families in plants, their promoter regions have received little attention. In this study, we investigated the expression patterns driven by the soybean (Glycine max) GmERF3 promoter and its cis-acting elements in soybean and tobacco. Transcriptomic data revealed that the native GmERF3 gene was differentially expressed in organs and tissues of plants. In transgenic soybeans containing a 1.3 kb GmERF3 promoter fused to the green fluorescent protein (gfp) gene, organ- and tissue-specificity was observed in untreated plants while mechanical wounding led to induction of GFP expression. Further in silico and in planta analyses of the GmERF3 promoter sequence in soybean revealed different cis-acting elements, including a novel cis-acting element, which contributed to increased expression, 1-2 days after mechanical wounding. We have named this DNA motif the wound-induced and delayed expression element (GGATTCAAGTTTAACC). A synthetic promoter containing a tetrameric repeat of this element showed high but late wound-induced GFP expression in leaves of transgenic tobacco. Our study expands the toolbox of inducible promoters and promoter elements for potential use in basic and applied research.


Asunto(s)
Regulación de la Expresión Génica de las Plantas/genética , Glycine max/genética , Nicotiana/genética , Proteínas de Plantas/genética , Regiones Promotoras Genéticas/genética , Proteínas de Plantas/metabolismo , Plantas Modificadas Genéticamente/genética , Plantas Modificadas Genéticamente/fisiología , Glycine max/fisiología , Nicotiana/fisiología
14.
ACS Photonics ; 11(4): 1673-1683, 2024 Apr 17.
Artículo en Inglés | MEDLINE | ID: mdl-38645995

RESUMEN

High-order harmonic generation (HHG) arising from the nonperturbative interaction of intense light fields with matter constitutes a well-established tabletop source of coherent extreme-ultraviolet and soft X-ray radiation, which is typically emitted as attosecond pulse trains. However, ultrafast applications increasingly demand isolated attosecond pulses (IAPs), which offer great promise for advancing precision control of electron dynamics. Yet, the direct generation of IAPs typically requires the synthesis of near-single-cycle intense driving fields, which is technologically challenging. In this work, we theoretically demonstrate a novel scheme for the straightforward and compact generation of IAPs from multicycle infrared drivers using hollow capillary fibers (HCFs). Starting from a standard, intense multicycle infrared pulse, a light transient is generated by extreme soliton self-compression in a HCF with decreasing pressure and is subsequently used to drive HHG in a gas target. Owing to the subcycle confinement of the HHG process, high-contrast IAPs are continuously emitted almost independently of the carrier-envelope phase (CEP) of the optimally self-compressed drivers. This results in a CEP-robust scheme which is also stable under macroscopic propagation of the high harmonics in a gas target. Our results open the way to a new generation of integrated all-fiber IAP sources, overcoming the efficiency limitations of usual gating techniques for multicycle drivers.

15.
Phys Rev Lett ; 111(8): 083602, 2013 Aug 23.
Artículo en Inglés | MEDLINE | ID: mdl-24010438

RESUMEN

We present a theoretical study of high-order harmonic generation (HHG) and propagation driven by an infrared field carrying orbital angular momentum (OAM). Our calculations unveil the following relevant phenomena: extreme-ultraviolet harmonic vortices are generated and survive to the propagation effects, vortices transport high-OAM multiples of the corresponding OAM of the driving field and, finally, the different harmonic vortices are emitted with similar divergence. We also show the possibility of combining OAM and HHG phase locking to produce attosecond pulses with helical pulse structure.

16.
J Phys Chem Lett ; 14(49): 11160-11167, 2023 Dec 14.
Artículo en Inglés | MEDLINE | ID: mdl-38054653

RESUMEN

Coherent control over electron dynamics in atoms and molecules using high-intensity circularly polarized laser pulses gives rise to current loops, resulting in the emission of magnetic fields. We propose, and demonstrate with ab initio calculations, "current-gating" schemes to generate direct or alternating-current magnetic pulses in the infrared spectral region, with highly tunable waveform and frequency, and showing femtosecond-to-attosecond pulse duration. In optimal conditions, the magnetic pulse can be highly isolated from the driving laser and exhibits a high flux density (∼1 T at a few hundred nanometers from the source, with a pulse duration of 787 attoseconds) for application in forefront experiments of ultrafast spectroscopy. Our work paves the way toward the generation of attosecond magnetic fields to probe ultrafast magnetization, chiral responses, and spin dynamics.

17.
Sci Adv ; 9(12): eadf3486, 2023 Mar 24.
Artículo en Inglés | MEDLINE | ID: mdl-36961899

RESUMEN

Symmetries and conservation laws of energy, linear momentum, and angular momentum play a central role in nonlinear optics. Recently, paraxial light fields with nontrivial topology have been attracting a keen interest. Despite not being eigenstates of the orbital and spin angular momenta (OAM and SAM), they are eigenstates of the generalized angular momentum (GAM) operator-a mixture of the OAM and SAM operators with fractional eigenvalues. By driving high harmonic generation with a polarization Möbius strip carrying a half-integer GAM charge and implementing angular momentum characterization methods in the extreme ultraviolet range, we demonstrate the linear scaling of the GAM with the harmonic order, each harmonic carrying a precise half-integer GAM charge. Our work shows that beyond SAM and OAM, the GAM is, in some situations, an appropriate quantum number. It paves the way for finer manipulations and applications of light beams containing fractional-order polarization singularities.

18.
Sci Adv ; 8(5): eabj7380, 2022 Feb 04.
Artículo en Inglés | MEDLINE | ID: mdl-35119926

RESUMEN

The extreme nonlinear optical process of high-harmonic generation (HHG) makes it possible to map the properties of a laser beam onto a radiating electron wave function and, in turn, onto the emitted x-ray light. Bright HHG beams typically emerge from a longitudinal phased distribution of atomic-scale quantum antennae. Here, we form a transverse necklace-shaped phased array of linearly polarized HHG emitters, where orbital angular momentum conservation allows us to tune the line spacing and divergence properties of extreme ultraviolet and soft x-ray high-harmonic combs. The on-axis HHG emission has extremely low divergence, well below that obtained when using Gaussian driving beams, which further decreases with harmonic order. This work provides a new degree of freedom for the design of harmonic combs-particularly in the soft x-ray regime, where very limited options are available. Such harmonic beams can enable more sensitive probes of the fastest correlated charge and spin dynamics in molecules, nanoparticles, and materials.

19.
Sci Adv ; 8(51): eadd7482, 2022 Dec 23.
Artículo en Inglés | MEDLINE | ID: mdl-36563146

RESUMEN

The concept of critical ionization fraction has been essential for high-harmonic generation, because it dictates the maximum driving laser intensity while preserving the phase matching of harmonics. In this work, we reveal a second, nonadiabatic critical ionization fraction, which substantially extends the phase-matched harmonic energy, arising because of the strong reshaping of the intense laser field in a gas plasma. We validate this understanding through a systematic comparison between experiment and theory for a wide range of laser conditions. In particular, the properties of the high-harmonic spectrum versus the laser intensity undergoes three distinctive scenarios: (i) coincidence with the single-atom cutoff, (ii) strong spectral extension, and (iii) spectral energy saturation. We present an analytical model that predicts the spectral extension and reveals the increasing importance of the nonadiabatic effects for mid-infrared lasers. These findings are important for the development of high-brightness soft x-ray sources for applications in spectroscopy and imaging.

20.
BMC Plant Biol ; 10: 237, 2010 Nov 04.
Artículo en Inglés | MEDLINE | ID: mdl-21050446

RESUMEN

BACKGROUND: Although numerous factors can influence gene expression, promoters are perhaps the most important component of the regulatory control process. Promoter regions are often defined as a region upstream of the transcriptional start. They contain regulatory elements that interact with regulatory proteins to modulate gene expression. Most genes possess their own unique promoter and large numbers of promoters are therefore available for study. Unfortunately, relatively few promoters have been isolated and characterized; particularly from soybean (Glycine max). RESULTS: In this research, a bioinformatics approach was first performed to identify members of the Gmubi (G.max ubiquitin) and the GmERF (G. max Ethylene Response Factor) gene families of soybean. Ten Gmubi and ten GmERF promoters from selected genes were cloned upstream of the gfp gene and successfully characterized using rapid validation tools developed for both transient and stable expression. Quantification of promoter strength using transient expression in lima bean (Phaseolus lunatus) cotyledonary tissue and stable expression in soybean hairy roots showed that the intensity of gfp gene expression was mostly conserved across the two expression systems. Seven of the ten Gmubi promoters yielded from 2- to 7-fold higher expression than a standard CaMV35S promoter while four of the ten GmERF promoters showed from 1.5- to 2.2-times higher GFP levels compared to the CaMV35S promoter. Quantification of GFP expression in stably-transformed hairy roots of soybean was variable among roots derived from different transformation events but consistent among secondary roots, derived from the same primary transformation events. Molecular analysis of hairy root events revealed a direct relationship between copy number and expression intensity; higher copy number events displayed higher GFP expression. CONCLUSION: In this study, we present expression intensity data on 20 novel soybean promoters from two different gene families, ubiquitin and ERF. We also demonstrate the utility of lima bean cotyledons and soybean hairy roots for rapid promoter analyses and provide novel insights towards the utilization of these expression systems. The soybean promoters characterized here will be useful for production of transgenic soybean plants for both basic research and commercial plant improvement.


Asunto(s)
Regulación de la Expresión Génica de las Plantas , Glycine max/genética , Proteínas de Plantas/genética , Regiones Promotoras Genéticas/genética , Proteínas de Soja/genética , Factores de Transcripción/genética , Ubiquitina/genética , Secuencia de Aminoácidos , Cotiledón/genética , Cotiledón/metabolismo , Proteínas Fluorescentes Verdes/genética , Proteínas Fluorescentes Verdes/metabolismo , Datos de Secuencia Molecular , Phaseolus/genética , Phaseolus/metabolismo , Filogenia , Proteínas de Plantas/clasificación , Raíces de Plantas/genética , Raíces de Plantas/metabolismo , Plantas Modificadas Genéticamente , Isoformas de Proteínas/genética , Glycine max/metabolismo , Ubiquitina/clasificación
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