Publications
2021
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(2021) Scientific Reports. 11, 495. Abstract
The Coulomb interaction between a photoelectron and its parent ion plays an important role in a large range of light-matter interactions. In this paper we obtain a direct insight into the Coulomb interaction and resolve, for the first time, the phase accumulated by the laser-driven electron as it interacts with the Coulomb potential. Applying extreme-ultraviolet interferometry enables us to resolve this phase with attosecond precision over a large energy range. Our findings identify a strong laser-Coulomb coupling, going beyond the standard recollision picture within the strong-field framework. Transformation of the results to the time domain reveals Coulomb-induced delays of the electrons along their trajectories, which vary by tens of attoseconds with the laser field intensity.
2020
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(2020) Optics Express. 28, 3, p. 3803-3810 Abstract
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.
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(2020) Nature Photonics. 14, 3, p. 188-194 Abstract[All authors]
A single-molecule attosecond interferometry that can retrieve the spectral phase information associated with the structure of molecular orbitals, as well as the phase accumulated by an electron as it tunnels out, is demonstrated.Interferometry is a basic tool to resolve coherent properties in a wide range of light or matter wave phenomena. In the strong-field regime, interferometry serves as a fundamental building block in revealing ultrafast electron dynamics. In this work we manipulate strong-field-driven electron trajectories and probe the coherence of a molecular wavefunction by inducing an interferometer on a microscopic level. The two arms of the interferometer are controlled by a two-colour field, while the interference pattern is read via advanced, three-dimensional high-harmonic spectroscopy. This scheme recovers the spectral phase information associated with the structure of molecular orbitals, as well as the spatial properties of the interaction itself. Zooming into one of the most fundamental strong-field phenomena-field-induced tunnel ionization-we reconstruct the angle at which the electronic wavefunction tunnels through the barrier and follow its evolution with attosecond precision.
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(2020) Nature Photonics. 14, 3, p. 183-+ Abstract[All authors]
Strong-field-driven electric currents in condensed-matter systems are opening new frontiers in petahertz electronics. In this regime, new challenges are arising as the roles of band structure and coherent electron-hole dynamics have yet to be resolved. Here, by using high-harmonic generation spectroscopy, we reveal the underlying attosecond dynamics that dictates the temporal evolution of carriers in multi-band solid-state systems. We demonstrate that when the electron-hole relative velocity approaches zero, enhanced constructive interference leads to the appearance of spectral caustics in the high-harmonic generation spectrum. We introduce the role of the dynamical joint density of states and identify its mapping into the spectrum, which exhibits singularities at the spectral caustics. By studying these singularities, we probe the structure of multiple unpopulated high conduction bands.
2019
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(2019) Optics Express. 27, 26, p. 37835-37845 Abstract
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.
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(2019) Physical Review X. 9, 3, 031004. Abstract
Controlling the polarization state of electromagnetic radiation enables the investigation of fundamental symmetry properties of matter through chiroptical processes. Over the past decades, many strategies have been developed to reveal structural or dynamical information about chiral molecules with high sensitivity, from the microwave to the extreme ultraviolet range. Most schemes employ circularly or elliptically polarized radiation, and more sophisticated configurations involve, for instance, light pulses with time-varying polarization states. All these schemes share a common property-the polarization state of light is always considered as constant over one optical cycle. In this study, we focus on the optical cycle in order to resolve and control a subcyle chiroptical process. We engineer an electric field whose instantaneous chirality can be controlled within the optical cycle, by combining two phase-locked orthogonally polarized fundamental and second harmonic fields. While the composite field has zero net ellipticity, it shows an instantaneous optical chirality which can be controlled via the two-color delay. We theoretically and experimentally investigate the photoionization of chiral molecules with this controlled chiral field. We find that electrons are preferentially ejected forward or backward relative to the laser propagation direction depending on the molecular handedness, similarly to the well-established photoelectron circular dichroism process. However, since the instantaneous chirality switches sign from one half-cycle to the next, electrons ionized from two consecutive half-cycles of the laser show opposite forward-backward asymmetries. This chiral signal, the enantiosensitive subcycle antisymmetric response gated by electric-field rotation, provides a unique insight into the influence of instantaneous chirality in the dynamical photoionization process. More generally, our results demonstrate the important role of subcycle polarization shaping of electric fields as a new route to study and manipulate chiroptical processes.
[All authors] -
(2019) Nature Photonics. 13, 3, p. 198–204 Abstract
Probing the vectorial properties of light-matter interactions inherently requires control over the polarization state of light. The generation of extreme-ultraviolet attosecond pulses has opened new perspectives in measurements of chiral phenomena. However, limited polarization control in this regime prevents the development of advanced vectorial measurement schemes. Here, we establish an extreme-ultraviolet lock-in detection scheme, allowing the isolation and amplification of extremely weak chiral signals, by achieving dynamical polarization control. We demonstrate a time-domain approach to control and modulate the polarization state, and perform its characterization via an in situ measurement. Our approach is based on the collinear superposition of two independent, phase-locked, orthogonally polarized extreme-ultraviolet sources and the control of their relative delay with sub-cycle accuracy. We achieve lock-in detection of magnetic circular dichroism, transferring weak amplitude variations into a phase modulation. This approach holds the potential to significantly extend the scope of vectorial measurements to the attosecond and nanometre frontiers.
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(2019) Nature Photonics. 13, 2, p. 91-95 Abstract
A key challenge in attosecond science is the temporal characterization of attosecond pulses that are essential for understanding the evolution of electronic wavefunctions in atoms, molecules and solids(1-7). Current characterization methods, based on nonlinear light-matter interactions, are limited in terms of stability and waveform complexity. Here, we experimentally demonstrate a conceptually new linear and all-optical pulse characterization method, inspired by double-blind holography. Holography is realized by measuring the extreme ultraviolet (XUV) spectra of two unknown attosecond signals and their interference. Assuming a finite pulse duration constraint, we reconstruct the missing spectral phases and characterize the unknown signals in both isolated pulse and double pulse scenarios. This method can be implemented in a wide range of experimental realizations, enabling the study of complex electron dynamics via a single-shot and linear measurement.
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(2019) Applied Sciences (Switzerland). 9, 3, 378. Abstract
High-harmonic generation spectroscopy is a powerful tool for ultrafast spectroscopy with intrinsic attosecond time resolution. Its major limitation-the fact that a strong infrared driving pulse is governing the entire generation process-is lifted by extreme ultraviolet (XUV)-initiated high-harmonic generation (HHG). Tunneling ionization is replaced by XUV photoionization, which decouples ionization from recollision. Here we probe the intensity dependence of XUV-initiated HHG and observe strong spectral frequency shifts of the high harmonics. We are able to tune the shift by controlling the instantaneous intensity of the infrared field. We directly access the reciprocal intensity parameter associated with the electron trajectories and identify short and long trajectories. Our findings are supported and analyzed by ab initio calculations and a semiclassical trajectory model. The ability to isolate and control long trajectories in XUV-initiated HHG increases the range of the intrinsic attosecond clock for spectroscopic applications.
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(2019) Nature Reviews Physics. 1, 2, p. 107-111 Abstract
Seven scientists share their views on some of the latest developments in attosecond science and X-ray free electron lasers (XFELs) and highlight exciting new directions.
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(2019) Nature Photonics. 13, 1, p. 54-59 Abstract
In photoelectron spectroscopy, the ionized electron wavefunction carries information about the structure of the bound orbital and the ionic potential as well as about the photoionization dynamics. However, retrieving the quantum phase information has been a long-standing challenge. Here, we transfer the electron phase retrieval problem into an optical one by measuring the time-reversed process of photoionization-photo-recombination-in attosecond pulse generation. We demonstrate all-optical interferometry of two independent phase-locked attosecond light sources. This measurement enables us to directly determine the phase shift associated with electron scattering in simple quantum systems such as helium and neon, over a large energy range. Moreover, the strong-field nature of attosecond pulse generation resolves the dipole phase around the Cooper minimum in argon through a single scattering angle. This method may enable the probing of complex orbital phases in molecular systems as well as electron correlations through resonances subject to strong laser fields.
[All authors] -
Attosecond Singularities in Solid State High Harmonic Generation(2019) accepted at Nature Photonics.
2018
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(2018) JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS. 51, 13, 134002. Abstract
Spectral focusing of the recolliding electron in high-order harmonic generation driven by two-color fields is shown to be a powerful tool for isolating and enhancing hidden spectral features of the target under study. In previous works we used this technique for probing multi-electron effects in xenon and we compared our experimental results with time-dependent configuration-interaction singles calculations. We demonstrate here that this technique can be exploited for reconstructing the enhancement factor of the xenon giant dipole resonance and we discuss the sensitivity of this method to macroscopic effects. We then extend the technique to argon in order to test the applicability of this procedure to other targets.
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(2018) Nature Communications. 9, 2805. Abstract
Ultrafast strong-field physics provides insight into quantum phenomena that evolve on an attosecond time scale, the most fundamental of which is quantum tunneling. The tunneling process initiates a range of strong field phenomena such as high harmonic generation (HHG), laser-induced electron diffraction, double ionization and photoelectron holography-all evolving during a fraction of the optical cycle. Here we apply attosecond photoelectron holography as a method to resolve the temporal properties of the tunneling process. Adding a weak second harmonic (SH) field to a strong fundamental laser field enables us to reconstruct the ionization times of photoelectrons that play a role in the formation of a photoelectron hologram with attosecond precision. We decouple the contributions of the two arms of the hologram and resolve the subtle differences in their ionization times, separated by only a few tens of attoseconds.
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(2018) Optics Express. 26, 7, p. 9310-9322 Abstract
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. (c) 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
2017
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(2017) Science. 358, 6368, p. 1288-1293 Abstract
Chiral light-matter interactions have been investigated for two centuries, leading to the discovery of many chiroptical processes used for discrimination of enantiomers. Whereas most chiroptical effects result from a response of bound electrons, photoionization can produce much stronger chiral signals that manifest as asymmetries in the angular distribution of the photoelectrons along the light-propagation axis. We implemented self-referenced attosecond photoelectron interferometry to measure the temporal profile of the forward and backward electron wave packets emitted upon photoionization of camphor by circularly polarized laser pulses. We measured a delay between electrons ejected forward and backward, which depends on the ejection angle and reaches 24 attoseconds. The asymmetric temporal shape of electron wave packets emitted through an autoionizing state further reveals the chiral character of strongly correlated electronic dynamics.
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(2017) Nature Communications. 8, Abstract
Single-photon ionization is one of the most fundamental light matter interactions in nature, serving as a universal probe of the quantum state of matter. By probing the emitted electron, one can decode the full dynamics of the interaction. When photo-ionization is evolving in the presence of a strong laser field, the fundamental properties of the mechanism can be signicantly altered. Here we demonstrate how the liberated electron can perform a self-probing measurement of such interaction with attosecond precision. Extreme ultraviolet attosecond pulses initiate an electron wavepacket by photo-ionization, a strong infrared field controls its motion, and finally electron-ion collision maps it into re-emission of attosecond radiation bursts. Our measurements resolve the internal clock provided by the self-probing mechanism, obtaining a direct insight into the build-up of photo-ionization in the presence of the strong laser field.
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(2017) Physical Review A. 95, 5, 51401. Abstract
Strong-field ionization followed by recollision provides a unique pump-probe measurement which reveals a range of electronic processes, combining sub-Angstrom spatial and attosecond temporal resolution. A major limitation of this approach is imposed by the coupling between the spatial and temporal degrees of freedom. In this paper we focus on the study of high harmonic generation and demonstrate the ability to isolate the internal dynamics-decoupling the temporal information from the spatial one. By applying an in situ approach we reveal the universality of the intrinsic pump-probe measurement and establish its validity in molecular systems. When several orbitals are involved we identify the fingerprint of the transition from the single-channel case into the multiple-channel dynamics, where complex multielectron phenomena are expected to be observed.
2016
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(2016) Physical Review Letters. 117, 9, Abstract
We investigated the giant resonance in xenon by high-order harmonic generation spectroscopy driven by a two-color field. The addition of a nonperturbative second harmonic component parallel to the driving field breaks the symmetry between neighboring subcycles resulting in the appearance of spectral caustics at two distinct cutoff energies. By controlling the phase delay between the two color components it is possible to tailor the harmonic emission in order to amplify and isolate the spectral feature of interest. In this Letter we demonstrate how this control scheme can be used to investigate the role of electron correlations that give birth to the giant resonance in xenon. The collective excitations of the giant dipole resonance in xenon combined with the spectral manipulation associated with the two-color driving field allow us to see features that are normally not accessible and to obtain a good agreement between the experimental results and the theoretical predictions.
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(2016) Physical Review Letters. 116, 5, p. 053002 (5 pp.) 053002 (5 . Abstract
Probing electronic wave functions of polyatomic molecules is one of the major challenges in high-harmonic spectroscopy. The extremely nonlinear nature of the laser-molecule interaction couples the multiple degrees of freedom of the probed system. We combine two-dimensional control of the electron trajectories and vibrational control of the molecules to disentangle the two main steps in high-harmonic generation-ionization and recombination. We introduce a new measurement scheme, frequency-resolved optomolecular gating, which resolves the temporal amplitude and phase of the harmonic emission from excited molecules. Focusing on the study of vibrational motion in N 2O 4, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.
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(2016) Nature Communications. 7, 10820. Abstract
The non-crystallographic phase problem arises in numerous scientific and technological fields. An important application is coherent diffractive imaging. Recent advances in X-ray free-electron lasers allow capturing of the diffraction pattern from a single nanoparticle before it disintegrates, in so-called 'diffraction before destruction' experiments. Presently, the phase is reconstructed by iterative algorithms, imposing a non-convex computational challenge, or by Fourier holography, requiring a well-characterized reference field. Here we present a convex scheme for single-shot phase retrieval for two (or more) sufficiently separated objects, demonstrated in two dimensions. In our approach, the objects serve as unknown references to one another, reducing the phase problem to a solvable set of linear equations. We establish our method numerically and experimentally in the optical domain and demonstrate a proof-of-principle single-shot coherent diffractive imaging using X-ray free-electron lasers pulses. Our scheme alleviates several limitations of current methods, offering a new pathway towards direct reconstruction of complex objects.
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(2016) Quantitative Phase Imaging II. 9718, UNSP 97182. Abstract
The phase retrieval problem arises in various fields ranging from physics and astronomy to biology and microscopy. Computational reconstruction of the Fourier phase from a single diffraction pattern is typically achieved using iterative alternating projections algorithms imposing a non-convex computational challenge. A different approach is holography, relying on a known reference field. Here we present a conceptually new approach for the reconstruction of two (or more) sufficiently separated objects. In our approach we combine the constraint the objects are finite as well as the information in the interference between them to construct an overdetermined set of linear equations. We show that this set of equations is guaranteed to yield the correct solution almost always and that it can be solved efficiently by standard numerical algebra tools. Essentially, our method combine commonly used constraint (that the object is finite) with a holographic approach (interference information). It differs from holographic methods in the fact that a known reference field is not required, instead the unknown objects serve as reference to one another (hence blind holography). Our method can be applied in a single-shot for two (or more) separated objects or with several measurements with a single object. It can benefit phase imaging techniques such as Fourier phytography microscopy, as well as coherent diffractive X-ray imaging in which the generation of a well-characterized, high resolution reference beam imposes a major challenge. We demonstrate our method experimentally both in the optical domain and in the X-ray domain using XFEL pulses.
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(2016) Faraday Discussions. 194, p. 369-405 Abstract
High harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multidimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
[All authors]
2015
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(2015) Nature Physics. 11, 10, p. 815-U184 Abstract
Attosecond physics offers new insights into ultrafast quantum phenomena involving electron dynamics on the fastest measurable timescales. The rapid progress in this field enables us to re-visit one of the most fundamental strong-field phenomena: field-induced tunnel ionization(1-3). In this work, we employ high-harmonic generation to probe the electron wavefunction during field-induced tunnelling through a potential barrier. By using a combination of strong and weak driving laser fields, we modulate the atomic potential barrier on optical subcycle timescales. This induces a temporal interferometer between attosecond bursts originating from consecutive laser half-cycles. Our study provides direct insight into the basic properties of field-induced tunnelling, following the evolution of the electronic wavefunction within a temporal window of approximately 200 attoseconds.
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(2015) 2015 CONFERENCE ON LASERS AND ELECTRO-OPTICS (CLEO). (Conference on Lasers and Electro-Optics). Abstract
We present a single-pulse two-dimensional Raman spectroscopy scheme. Our scheme offers not only a major simplification of the conventional setup but also an inherent favoring of the direct fifth-order signal over the cascaded signal, the latter being a signal that carries no coupling information.
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(2015) Nature Photonics. 9, 5, p. 339-343 Abstract
Vibrational modes are often localized in certain regions of a molecule, and so the coupling between these modes is sensitive to the molecular structure. Two-dimensional vibrational spectroscopy can probe the strength of this coupling in a manner analogous to two-dimensional NMR spectroscopy, but on ultrafast timescales. Here, we demonstrate how two-dimensional Raman spectroscopy, based on fifth-order optical nonlinearity, can be performed with a single beam of shaped femtosecond optical pulses. Our spectroscopy scheme offers not only a major simplification of the conventional set-up, but also an inherent elimination of a competing nonlinear signal, which overwhelms the desired signal in other schemes and carries no coupling information.
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(2015) Nature Communications. 6, Abstract
High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20-26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.
[All authors]
2014
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(2014) JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS. 47, 20, Abstract
High-harmonic generation spectroscopy is a promising tool for resolving electron dynamics and structure in atomic and molecular systems. This scheme, commonly described by the strong field approximation, requires a deep insight into the basic mechanism that leads to the harmonic generation. Recently, we have demonstrated the ability to resolve the first stage of the process-field induced tunnel ionization-by adding a weak perturbation to the strong fundamental field. Here we generalize this approach and show that the assumptions behind the strong field approximation are valid over a wide range of tunnel ionization conditions. Performing a systematic study-modifying the fundamental wavelength, intensity and atomic system-we observed a good agreement with quantum path analysis over a range of Keldysh parameters. The generality of this scheme opens new perspectives in high harmonics spectroscopy, holding the potential of probing large, complex molecular systems.
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(2014) Optics Express. 22, 21, p. 24935-24950 Abstract
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. (C) 2014 Optical Society of America
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(2014) JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS. 47, 12, 124023. Abstract
Strong field transient grating spectroscopy has shown to be a very versatile tool in time-resolved molecular spectroscopy. Here we use this technique to investigate the high-order harmonic generation from SF6 molecules vibrationally excited by impulsive stimulated Raman scattering. Transient grating spectroscopy enables us to reveal clear modulations of the harmonic emission. This heterodyne detection shows that the harmonic emission generated between 14 and 26 eV is mainly sensitive to two among the three active Raman modes in SF6, i.e. the strongest and fully symmetric upsilon 1-A(1g) mode (774 cm(-1), 43 fs) and the slowest mode upsilon 5-T-2g (524 cm(-1), 63 fs). A time-frequency analysis of the harmonic emission reveals additional dynamics: the strength and central frequency of upsilon 1 mode oscillate with a frequency of 52 cm(-1) (640 fs). This could be a signature of the vibration of dimers in the generating medium. Harmonic 11 shows a remarkable behaviour, oscillating in the opposite phase, both on the fast (774 cm(-1)) and slow (52 cm(-1)) timescales, which indicates a strong modulation of the recombination matrix element as a function of the nuclear geometry. These results demonstrate that the high sensitivity of high-order harmonic generation to molecular vibrations, associated to the high sensitivity of transient grating spectroscopy, make their combination a unique tool to probe vibrational dynamics.
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(2014) Physics. 7, 53, Abstract
The frequency and intensity of attosecond light pulses can be increased by optimizing the optical pulses that drive a high-harmonic generation process.
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2013
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(2013) Physical Review Letters. 111, 2, 023005. Abstract
In strong-field light-matter interactions, the strong laser field dominates the dynamics. However, recent experiments indicate that the Coulomb force can play an important role as well. In this Letter, we have studied the photoelectron momentum distributions produced from noble gases in elliptically polarized, 800 nm laser light. By performing a complete mapping of the three-dimensional electron momentum, we find that Coulomb focusing significantly narrows the lateral momentum spread. We find a surprisingly sensitive dependence of Coulomb focusing on the initial transverse momentum distribution, i.e., the momentum at the moment of birth of the photoelectron. We also observe a strong signature of the low-energy structure in the above threshold ionization spectrum.
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(2013) IEEE Transactions on Signal Processing. 61, 7, p. 1632-1643 Abstract
Reconstruction of signals from measurements of their spectral intensities, also known as the phase retrieval problem, is of fundamental importance in many scientific fields. In this paper we present a novel framework, denoted as vectorial phase retrieval, for reconstruction of pairs of signals from spectral intensity measurements of the two signals and of their interference. We show that this new framework can alleviate some of the theoretical and computational challenges associated with classical phase retrieval from a single signal. First, we prove that for compactly supported signals, in the absence of measurement noise, this new setup admits a unique solution. Next, we present a statistical analysis of vectorial phase retrieval and derive a computationally efficient algorithm to solve it. Finally, we illustrate via simulations, that our algorithm can accurately reconstruct signals even at considerable noise levels.
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(2013) Chemical Physics. 414, p. 176-183 Abstract
Recollision experiments have been very successful in resolving attosecond scale dynamics. However, such schemes rely on the single atom response, neglecting the macroscopic properties of the interaction and the effects of using multi-cycle laser fields. In this paper we perform a complete spatio-spectral analysis of the high harmonic generation process and resolve the distribution of the subcycle dynamics of the recolliding electron. Specifically, we focus on the measurement of ionization times. Recently, we have demonstrated that the addition of a weak, crossed polarized second harmonic field allows us to resolve the moment of ionization (Shafir, 2012) [1]. In this paper we extend this measurement and perform a complete spatio-spectral analysis. We apply this analysis to reconstruct the ionization times of both short and long trajectories showing good agreement with the quantum path analysis. (c) 2012 Elsevier B.V. All rights reserved.
2012
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(2012) Physical Review Letters. 108, 20, Abstract
Recollision processes provide direct insight into the structure and dynamics of electronic wave functions. However, the strength of the process sets its basic limitations-the interaction couples numerous degrees of freedom. In this Letter we decouple the basic steps of the process and resolve the role of the ionic potential which is at the heart of a broad range of strong field phenomena. Specifically, we measure high harmonic generation from argon atoms. By manipulating the polarization of the laser field we resolve the vectorial properties of the interaction. Our study shows that the ionic core plays a significant role in all steps of the interaction. In particular, Coulomb focusing induces an angular deflection of the electrons before recombination. A complete spatiospectral analysis reveals the influence of the potential on the spatiotemporal properties of the emitted light.
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(2012) Nature. 485, 7398, p. 343-346 Abstract
The tunnelling of a particle through a barrier is one of the most fundamental and ubiquitous quantum processes. When induced by an intense laser field, electron tunnelling from atoms and molecules initiates a broad range of phenomena such as the generation of attosecond pulses(1), laser-induced electron diffraction(2,3) and holography(2,4). These processes evolve on the attosecond timescale (1 attosecond equivalent to 1 as = 10(-18) seconds) and are well suited to the investigation of a general issue much debated since the early days of quantum mechanics(5-7)-the link between the tunnelling of an electron through a barrier and its dynamics outside the barrier. Previous experiments have measured tunnelling rates with attosecond time resolution(8) and tunnelling delay times(9). Here we study laser-induced tunnelling by using a weak probe field to steer the tunnelled electron in the lateral direction and then monitor the effect on the attosecond light bursts emitted when the liberated electron re-encounters the parent ion(10). We show that this approach allows us to measure the time at which the electron exits from the tunnelling barrier. We demonstrate the high sensitivity of the measurement by detecting subtle delays in ionization times from two orbitals of a carbon dioxide molecule. Measurement of the tunnelling process is essential for all attosecond experiments where strong-field ionization initiates ultrafast dynamics(10). Our approach provides a general tool for time-resolving multi-electron rearrangements in atoms and molecules(11-13)-one of the key challenges in ultrafast science.
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(2012) Nature Photonics. 6, 3, p. 170-173 Abstract
Many intriguing phenomena in nature-from phase transitions to black holes-occur at singularities. A unique type of singularity common in wave phenomena, known as caustics(1,2), links processes observed in many different branches of physics(3,4). Here, we investigate the role of caustics in attosecond science and in particular the physical process behind high harmonic generation(5). We experimentally demonstrate spectral focusing in high harmonic generation, showing a robust intensity enhancement of an order of magnitude over a spectral width of several harmonics. This new level of control holds promises in both scientific and technological aspects of attosecond science(6,7). Moreover, our study provides a deeper insight into the basic mechanism underlying the high harmonic generation process, revealing its quantum nature(8) and universal properties.
2011
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(2011) Physical Review Letters. 107, 13, 133902. Abstract
The waveforms of attosecond pulses produced by high-harmonic generation carry information on the electronic structure and dynamics in atomic and molecular systems. Current methods for the temporal characterization of such pulses have limited sensitivity and impose significant experimental complexity. We propose a new linear and all-optical method inspired by widely used multidimensional phase retrieval algorithms. Our new scheme is based on the spectral measurement of two attosecond sources and their interference. As an example, we focus on the case of spectral polarization measurements of attosecond pulses, relying on their most fundamental property-being well confined in time. We demonstrate this method numerically by reconstructing the temporal profiles of attosecond pulses generated from aligned CO(2) molecules.
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(2011) Optics Express. 19, 2, p. 679-686 Abstract
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 similar to 1 photon per pulse, a regime in which nonlinear techniques are impractical, at a temporal resolution of similar to 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. (C) 2011 Optical Society of America
2010
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(2010) Physical Review Letters. 105, 14, 143904. Abstract
We study high-order harmonic generation in aligned molecules close to the ionization threshold. Two distinct contributions to the harmonic signal are observed, which show very different responses to molecular alignment and ellipticity of the driving field. We perform a classical electron trajectory analysis, taking into account the significant influence of the Coulomb potential on the strong-field-driven electron dynamics. The two contributions are related to primary ionization and excitation processes, offering a deeper understanding of the origin of high harmonics near the ionization threshold. This Letter shows that high-harmonic spectroscopy can be extended to the near-threshold spectral range, which is in general spectroscopically rich.
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Probing the symmetry of atomic wavefunctions from the point of view of strong field-driven electrons(2010) New Journal of Physics. 12, 73032. Abstract
In this paper, we analyze a new approach that was first presented by Shafir et al (2009 Nat. Phys. 5 412-6) to probe the symmetry of atomic wavefunctions via the high harmonic generation process. In this scheme, we control the two-dimensional (2D) motion of a free electron using a two-color field to probe the atoms from different angles. We present a new theoretical analysis that focuses on the spherical symmetry of atomic potentials. We analyze previously presented experimental results (Shafir et al 2009 Nat. Phys. 5 412-6) and demonstrate the ability to distinguish between spherically symmetric (s state) and non-spherically symmetric (p state) orbitals. Finally, we discuss the limitations of our approach and compare it with alternative methods.
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(2010) Physical Review Letters. 105, 5, 53003. Abstract
We have measured high-order harmonic generation spectra of D-2, N-2, and CO2 by mixing orthogonally polarized 800 and 400 nm laser fields. The intensity of the high-harmonic spectrum is modulated as we change the relative phase of the two pulses. For randomly orientated molecules, the phase of the intensity modulation depends on the symmetry of the molecular orbitals from which the high harmonics are emitted. This allows us to identify the symmetry of any orbital that contributes to high-harmonic generation, even without aligning the molecule. Our approach can be a route to imaging dynamical changes in three-dimensional molecular orbitals on a time scale as short as a few hundred attoseconds.
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(2010) Physical Review Letters. 104, 21, Abstract
We perform high harmonic generation spectroscopy of aligned nitrogen molecules to characterize the attosecond dynamics of multielectron rearrangement during strong-field ionization. We use the spectrum and ellipticity of the harmonic light to reconstruct the relative phase between different ionization continua participating in the ionization, and thus determine the shape and location of the hole left in the molecule by strong-field ionization. Our interferometric technique uses transitions between the ionic states, induced by the laser field on the subcycle time scale.
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(2010) JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS. 43, 6, Abstract
We study the spatial profile of high order harmonics generated by a transient grating of rotational excitation. We show that the phase modulation of the harmonic emission as a function of molecular alignment is encoded in the diffraction pattern. In molecular nitrogen, the phase difference between aligned and isotropic molecules decreases from 1.6 rad for harmonic 19 to less than 0.3 rad for harmonic 27. In CO(2) we observe a strong phase jump for the highest harmonics. The position of this phase jump in the harmonic spectrum depends on the laser intensity, reflecting the contribution from multiple molecular orbitals to the harmonic emission.
2009
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(2009) Proceedings of the National Academy of Sciences of the United States of America. 106, 39, p. 16556-16561 Abstract
Molecular structures, dynamics and chemical properties are determined by shared electrons in valence shells. We show how one can selectively remove a valence electron from either Pi vs. Sigma or bonding vs. nonbonding orbital by applying an intense infrared laser field to an ensemble of aligned molecules. In molecules, such ionization often induces multielectron dynamics on the attosecond time scale. Ionizing laser field also allows one to record and reconstruct these dynamics with attosecond temporal and sub-Angstrom spatial resolution. Reconstruction relies on monitoring and controlling high-frequency emission produced when the liberated electron recombines with the valence shell hole created by ionization.
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(2009) Nature. 460, 7258, p. 972-977 Abstract
High harmonic emission occurs when an electron, liberated from a molecule by an incident intense laser field, gains energy from the field and recombines with the parent molecular ion. The emission provides a snapshot of the structure and dynamics of the recombining system, encoded in the amplitudes, phases and polarization of the harmonic light. Here we show with CO2 molecules that high harmonic interferometry can retrieve this structural and dynamic information: by measuring the phases and amplitudes of the harmonic emission, we reveal 'fingerprints' of multiple molecular orbitals participating in the process and decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. These findings establish high harmonic interferometry as an effective approach to resolving multi-electron dynamics with sub-Angstrom spatial resolution arising from the de Broglie wavelength of the recombining electron, and attosecond temporal resolution arising from the timescale of the recombination event.
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(2009) Physical Review A. 80, 1, Abstract
We present a method for controlling the spatial properties of a high-order harmonic beam on a subcycle time scale. By adding a second-harmonic field to the driving laser field, we modify the spatiotemporal structure of the harmonic beam and manipulate it with attosecond resolution. Such a manipulation maps the subcycle dynamics of a recolliding electron to the spatial domain.
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(2009) Nature Physics. 5, 6, p. 412-416 Abstract
Strong-field light-matter interactions can encode the spatial properties of the electronic wavefunctions that contribute to the process(1-4). In particular, the broadband harmonic spectra, measured for a series of molecular alignments, can be used to create a tomographic reconstruction of molecular orbitals(5). Here, we present an extension of the tomography approach to systems that cannot be naturally aligned. We demonstrate this ability by probing the two-dimensional properties of atomic wavefunctions. By manipulating an electron-ion recollision process(6), we are able to resolve the symmetry of the atomic wavefunction with high contrast.
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(2009) Physical Review Letters. 102, 6, Abstract
We describe the roles of multiple electronic continua in high-harmonic generation from aligned molecules. First, we show how the circularity of emitted harmonics tracks the interplay of different electronic continua participating in the nonlinear response. Second, we show that the interplay of different continua can lead to large variations of harmonic phases. Finally, we show how multiple electronic continua allow one to shape the polarization of high harmonics and attosecond pulses.
2008
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(2008) Physical Review Letters. 100, 14, Abstract
We study high-order harmonic generation in excited media using a four-wave-mixing-like configuration. We analyze the spatial profile of high harmonics emitted by a grating of rotationally excited molecules as a function of the pump-probe delay. We demonstrate a dramatic improvement in the contrast of the diffracted signal relative to the total high harmonic signal. This allows us to observe subtle effects in the rotational wave packet excitation such as the pump-intensity dependence of the wave packet dynamics. High harmonic transient grating spectroscopy can be extended to all forms of molecular excitation and to weak resonant excitation.
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(2008) New Journal of Physics. 10, Abstract
We study experimentally and theoretically the high harmonic emission from aligned samples of nitrogen and carbon dioxide, in an elliptically polarized laser field. The ellipticity induces a lateral shift of the recombining electron wavepacket in the generation process. We show that this effect, which is well known from high harmonic generation (HHG) in atoms, can be useful to maintain the plane wave approximation in the case of HHG from molecules whose orbitals contain nodal planes. The study of the harmonic signal as a function of molecular alignment also reveals the role of the ellipticity on the recollision angle of the electron wavepacket, which can be used to accurately track the position of resonances in harmonic spectra.
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(2008) Journal of Modern Optics. 55, 16, p. 2591-2602 Abstract
While high harmonic generation from atoms is relatively well understood, the ability to align gas-phase molecules opens an opportunity to more deeply understand the underlying physics. Many assumptions, such as the single active electron approximation, neglect of the Coulomb potential, the strong field approximation, and the assumption of plane waves, are being challenged by new experimental observations. We study high harmonic emission from aligned molecules such as N(2), O(2) and CO(2). We present experimental measurements of the amplitude of the emission as a function of molecular angle, as well as the polarization state.
2007
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(2007) Physical Review Letters. 99, 24, 243001. Abstract
High harmonic emission in isotropic gases is polarized in the same direction as the incident laser polarization. Laser-induced molecular alignment allows us to break the symmetry of the gas medium. By using aligned molecules in high harmonic generation experiments, we show that the polarization of the extreme ultraviolet emission depends strongly on the molecular alignment and the orbital structure. Polarization measurements give insight into the molecular orbital symmetry. Furthermore, molecular alignment will allow us to produce attosecond pulses with time-dependent polarization.
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(2007) Optics Letters. 32, 4, p. 436-438 Abstract
We present a method for controlling the spatial properties of high-harmonic beams with high efficiency. The high nonlinearity of harmonic generation allows weak control beams to induce a phase mask for the extreme UV light as it is formed. We fabricate a phase grating and demonstrate efficient diffraction in the far field. Diffractive elements formed in this way are transient. Since they are induced by the subcycle interaction of the medium with the fundamental and control fields, they can be extended to the attosecond time scale.
2006
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(2006) Physical Review Letters. 97, 25, 253903. Abstract
Temporal gating allows high accuracy time-resolved measurements of a broad range of ultrafast processes. By manipulating the interaction between an atom and an intense laser field, we extend gating into the nonlinear medium in which attosecond optical and electron pulses are generated. Our gate is an amplitude gate induced by ellipticity of the fundamental pulse. The gate modulates the spectrum of the high harmonic emission and we use the measured modulation to characterize the sub-laser-cycle dynamics of the recollision electron wave packet.
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(2006) Nature Physics. 2, 11, p. 781-786 Abstract
Generating attosecond pulses has required a radically different approach from previous ultrafast optical methods. The technology of attosecond measurement, however, is built on established methods of characterizing femtosecond pulses: the pulse is measured after it has left the region where it was produced. We offer a completely different approach: in situ measurement. That is, we integrate attosecond-pulse production and measurement in a manner that can be applied to many high-order nonlinear interactions. To demonstrate this approach, we combine a low-intensity (
2005
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(2005) Physical Review A. 72, 6, Abstract
Polarization gating of high-order harmonic generation takes advantage of the significant reduction of harmonic generation efficiency for elliptically polarized excitation fields, in order to generate short bursts of harmonic radiation from relatively long pulses. We show that the currently used method for generation of polarization gated pulses using wave-plate combinations is inefficient, and propose an alternative method based on polarization pulse shaping techniques. This method is shown to be significantly more efficient and to enable significant shortening of the gate duration. Using this scheme, isolated attosecond pulses should be achievable with excitation pulses of a duration as long as 20 fs.
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(2005) Physical Review Letters. 94, 8, Abstract
Coherent-control schemes to manipulate weak-field interactions are generally invalid at stronger fields, since strong-field interactions are accompanied by level power broadenings and level shifts that usually elude simple analytical treatments. Here we show that a broad subgroup of weak-field solutions (those with real fields, i.e., fields with only one quadrature in the complex plane) can be extended to the strong-field regime while retaining their properties. The salient feature of these fields is a symmetry that cancels out power broadening effects. Such fields can be generated from ultrashort coherent pulses or from incoherent broadband down-converted light. Weak-field coherent-control approaches based on these solutions can therefore be extended to the strong-field regime as we demonstrate in a two-photon absorption experiment in atomic cesium.
2004
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(2004) Physical Review A. 70, 2, Abstract
In spectroscopy, the fingerprint of a substance is usually comprised of a sequence of spectral lines with characteristic frequencies and strengths. Identification of substances often involves postprocessing, where the measured spectrum is compared with tabulated fingerprint spectra. Here we suggest a scheme for nonlinear spectroscopy, where, through coherent control of the nonlinear process, the information from the entire spectrum can be practically collected into a single coherent entity. We apply this for all-optical analysis of coherent Raman spectra and demonstrate enhanced detection and effective background suppression using coherent processing.
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(2004) Physical Review Letters. 92, 10, Abstract
The newly developed technique of polarization pulse shaping is applied to the control of two-photon absorption in atomic rubidium. This technique enables the manipulation of the transient vector properties of a light matter interaction. We establish that control can be exerted on the angular distribution of the final state, and demonstrate the ability to control the final state population of a nearly degenerate system, as well as to perform M-state resolved spectroscopy.
2003
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(2003) Journal of Chemical Physics. 118, 20, p. 9208-9215 Abstract
Quantum coherent control techniques are applied to achieve high spectral resolution nonlinear vibrational spectroscopy using a single ultrashort laser source. By controlling the spectral phase of similar to10 fs pulses, we are able to obtain detailed coherent anti-Stokes Raman (CARS) spectra in the important fingerprint spectral region, which reflects the structural chemical information. A full theoretical analysis and an experimental demonstration of two alternative schemes leading to spectral resolution two orders of magnitude better than the pulse bandwidth are presented. The first involves selective excitation of vibrational levels within the pulse bandwidth by periodic modulation of the spectral phase of the pulse. In the second scheme an effective narrow probing of the vibrational level has been achieved by phase shifting of a narrow spectral band. Single-pulse CARS offers an attractive alternative to conventional multibeam nonlinear vibrational spectroscopy techniques. (C) 2003 American Institute of Physics.
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(2003) Physical Review Letters. 90, 21, Abstract
Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.
2002
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(2002) Physical Review Letters. 89, 27, Abstract
High spectral resolution nonlinear vibrational spectroscopy with a single ultrashort pulse is demonstrated on a variety of samples. The spectral data are obtained by shaping the excitation pulse in order to control the relative phase between the weak resonant signal and the strong nonresonant background, in analogy with phase-contrast microscopy techniques. This is unlike the more conventional approach to nonlinear spectroscopy, in which the nonresonant background is reduced to a minimum. By measuring the spectrum of the coherent anti-Stokes Raman signal, it is possible to infer the vibrational energy levels in a band spanning almost an entire octave.
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(2002) Nature. 418, 6897, p. 512-514 Abstract
Molecular vibrations have oscillation periods that reflect the molecular structure, and are hence being used as a spectroscopic fingerprint for detection and identification. At present, all nonlinear spectroscopy schemes use two or more laser beams to measure such vibrations(1). The availability of ultrashort (femtosecond) optical pulses with durations shorter than typical molecular vibration periods has enabled the coherent excitation of molecular vibrations using a single pulse(2). Here we perform single-pulse vibrational spectroscopy on several molecules in the liquid phase, where both the excitation and the readout processes are performed by the same pulse. The main difficulty with single-pulse spectroscopy is that all vibrational levels with energies within the pulse bandwidth are excited. We achieve high spectral resolution, nearly two orders of magnitude better than the pulse bandwidth, by using quantum coherent control techniques. By appropriately modulating the spectral phase of the pulse we are able to exploit the quantum interference between multiple paths to selectively populate a given vibrational level, and to probe this population using the same pulse. This scheme, using a single broadband laser source, is particularly attractive for nonlinear microscopy applications, as we demonstrate by constructing a coherent anti-Stokes Raman (CARS) microscope operating with a single laser beam.
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(2002) Physical Review A. 65, 4, Abstract
Using femtosecond pulse-shaping techniques, we are able to control several useful parameters of coherent anti-Stokes Raman spectroscopy (CARS). By shaping both the pump and the Stokes pulses with an appropriate spectral phase function, we eliminated the nonresonant CARS background. In addition, we designed pulses which selectively excite one of two neighboring Raman levels, even when both are well within the excitation spectrum. High-resolution CARS spectra were recorded in spite of the broad femtosecond pulse spectrum.
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(2002) Physical Review Letters. 88, 12, Abstract
By applying pulse shaping techniques to a broadband 100 fs pulse in resonance with a two-level atomic transition, we are able to enhance the peak transient excited level population relative to that achievable with transform limited pulses. We also demonstrate how the dispersion induced by the absorption line itself leads to similar rapidly oscillating transients in the excited population. These transient population effects are applicable in any multiphoton resonant transition.
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(2002) Physical Review Letters. 88, 6, Abstract
By tailoring the phase of a 100 femtosecond probe pulse we are able to obtain a narrow-band coherent anti-Stokes Raman spectroscopy (CARS) resonant signal with a width of less than 15 cm(-1), which is an order of magnitude narrower than the CARS signal from a transform limited pulse. Thus, by measuring the spectrum of the CARS signal we are able to obtain a high-resolution energy level diagram of the probed sample in spite of the broad femtosecond pulse spectrum.
2001
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(2001) IEEE Journal of Quantum Electronics. 37, 8, p. 1030-1039 Abstract
Under certain conditions, a high-finesse resonance phenomenon can occur in a grating waveguide structure (GWS). By varying these conditions, a shift in the resonance wavelength can be achieved. Specifically, utilizing the high finesse property of the GWS, small changes in the refractive index can result in a tuning range larger than the resonance bandwidth. Here, we consider different electric-field and charge carrier mechanisms that can affect the refractive index in semiconductor materials, and exploit them in order to control the refractive index change and, therefore, the resonance wavelength in the GWS. The predicted results are verified experimentally with an active GWS formed with semiconductor materials and operated in a reverse voltage configuration.
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(2001) Physical Review Letters. 86, 1, p. 47-50 Abstract
Maximizing nonlinear light-matter interactions is a primary motive for compressing laser pulses to achieve ultrashort transform limited pulses. Here we show how, by appropriately shaping the pulses, resonant multiphoton transitions can be enhanced significantly beyond the level achieved by maximizing the pulse's peak intensity. We demonstrate the counterintuitive nature of this effect with an experiment in a resonant two-photon absorption, in which, by selectively removing certain spectral hands, the peak intensity of the pulse is reduced by a factor of 40, yet the absorption rate is doubled. Furthermore, by suitably designing the spectral phase of the pulse, we increase the absorption rate by a factor of 7.