Coherent Excitation Research Articles

High-harmonic spectroscopy of coherent lattice dynamics in graphene

High-harmonic spectroscopy of solids is a powerful tool, which provides access to both electronic structure and ultrafast electronic response of solids, from their band structure and density of states to phase transitions, including the emergence of the topological edge states, to the PetaHertz electronic response. However, in spite of these successes, high-harmonic spectroscopy has hardly been applied to analyze the role of coherent femtosecond lattice vibrations in the attosecond electronic response. Here we study coherent phonon excitations in monolayer graphene to show how high-harmonic spectroscopy can be used to detect the influence of coherent lattice dynamics, particularly longitudinal and transverse optical phonon modes, on the electronic response. Coherent excitation of the in-plane phonon modes results in the appearance of sidebands in the spectrum of the emitted harmonic radiation. We show that the spectral positions and the polarization of the sideband emission offer a sensitive probe of the dynamical symmetries associated with the excited phonon modes. Our work brings the key advantage of high-harmonic spectroscopy---the combination of subfemtosecond to tens of femtoseconds temporal resolution---to the problem of probing phonon-driven electronic response and its dependence on the dynamical symmetries in solids.

Valley control by linearly polarized laser pulses: example of WSe2

Electrons at the band edges of materials are endowed with a valley index, a quantum number locating the band edge within the Brillouin zone. An important question is then how this index may be controlled by laser pulses, with current understanding that it couples exclusively via circularly polarized light. Employing both tight-binding and state-of-the-art time dependent density function theory, we show that on femtosecond time scales valley coupling is a much more general effect. We find that two time separated linearly polarized pulses allow almost complete control over valley excitation, with the pulse time difference and polarization vectors emerging as key parameters for valley control. Our findings highlight the possibility of controlling coherent electronic excitation by successive femtosecond laser pulses, and offer a route towards valleytronics in two-dimensional materials.

Coherent full polarization control based on bound states in the continuum

Bound states in the continuum (BICs) are resonant modes of open structures that do not suffer damping, despite being compatible with radiation in terms of their momentum. They have been raising significant attention for their intriguing topological features, and their opportunities in photonics to enhance light-matter interactions. In parallel, the coherent excitation of optical devices through the tailored interference of multiple beams has been explored as a way to enhance the degree of real-time control over their response. Here, we leverage the combination of these phenomena, and exploit the topological features of BICs in the presence of multiple input beams to enable full polarization control on the entire Poincaré sphere in a photonic crystal slab only supporting a symmetry-protected BIC, experimentally demonstrating highly efficient polarization conversion controlled in real time through the superposition of coherent excitations. Our findings open exciting opportunities for a variety of photonic and quantum optics applications, benefitting from extreme wave interactions and topological features around BICs combined with optical control through coherent interference of multiple excitations.

Laser-induced THz piezomagnetism and lattice dynamics of antiferromagnets [formula omitted] and [formula omitted

The piezomagnetic effect manifests itself in emergence of a net magnetic moment in a mechanically-stressed magnetically ordered material. Up to now, this effect was theoretically analyzed and experimentally studied for the case of static or low frequency deformations of antiferromagnets, and in our brief overview we present the recent progress in exploring the piezomagnetic effect at the THz frequencies. We discuss particular lattice distortions in the model piezomagnetic antiferromagnets MnF2 and CoF2 that are associated with the Raman-active phonons. We show that the phonons of the Eg and B2g symmetry should support emergence of a dynamic magnetic moment oscillating at the corresponding THz phonon frequencies. We further analyze conditions for coherent excitations of these modes by using ultrashort laser pulses via the mechanism of impulsive stimulated Raman scattering. We show that observation of transverse piezomagnetic effect is, in principle, feasible for the Eg phonon. We also discuss experimental results demonstrating laser-induced excitation of coherent Eg phonon in MnF2 and CoF2, as well as speculate about possibilities to detect piezomagnetic effect at the THz frequencies.

Long-Time Bit Storage and Retrieval without Cold Atom Technology

We report computer studies showing how the duration of memory for storage and retrieval of a classical bit can be increased to 100 times the decay time of an isolated atom, with no use of high-tech cold-atom preparations recently developed in the light-matter field. We suggest that our low-tech procedure can greatly enlarge the number of experimenters able to enter this field. The role of symmetry in this procedure arises in a careful interplay of incoherent and coherent excitations of a large collection of “two-level” atoms, the level separation being matched by the dominant frequency of the electromagnetic fields (short pulses and continuing field) applied to the system.

SUPER Scheme in Action: Experimental Demonstration of Red-Detuned Excitation of a Quantum Emitter.

The quest for the perfect single-photon source includes finding the optimal protocol for exciting the quantum emitter. Coherent optical excitation was, up until now, achieved by tuning the laser pulses to the transition frequency of the emitter, either directly or in average. Recently, it was theoretically discovered that an excitation with two red-detuned pulses is also possible where neither of which would yield a significant upper-level population individually. We show that the so-called swing-up of quantum emitter population (SUPER) scheme can be implemented experimentally with similar properties to existing schemes by precise amplitude shaping of a broadband pulse. Because of its truly off-resonant nature, this scheme has the prospect of powering high-purity photon sources with superior photon count rate.

Few-cycle excitation of atomic coherence: an analytical solution beyond the rotating-wave approximation

Developing an analytical theory for atomic coherence driven by ultrashort laser pulses has proved to be challenging due to the breakdown of the rotating wave approximation (RWA). In this paper, we present an approximate analytical solution that describes a two-level atom under the excitation of a far-off-resonance, few-cycle pulse of arbitrary shape without invoking the RWA. As an example of its applicability, a closed-form solution for Gaussian pulses is explicitly given, and the result is used to analyse the impact of carrier envelope phase on atomic population ratios. Comparisons with numerical solutions validate the accuracy our solution within the scope of the approximation. Finally, we outline an alternative approach that can lead to a more accurate solution by capturing the nonlinear behaviors of the system. The work lays out feasible theoretical paths toward analytically describing two-level atoms driven by ultrashort pulses.

Mode-selective ballistic pathway to a metastable electronic phase.

Exploiting vibrational excitation for the dynamic control of material properties is an attractive goal with wide-ranging technological potential. Most metal-to-insulator transitions are mediated by few structural modes and are, thus, ideal candidates for selective driving toward a desired electronic phase. Such targeted navigation within a generally multi-dimensional potential energy landscape requires microscopic insight into the non-equilibrium pathway. However, the exact role of coherent inertial motion across the transition state has remained elusive. Here, we demonstrate mode-selective control over the metal-to-insulator phase transition of atomic indium wires on the Si(111) surface, monitored by ultrafast low-energy electron diffraction. We use tailored pulse sequences to individually enhance or suppress key phonon modes and thereby steer the collective atomic motion within the potential energy surface underlying the structural transformation. Ab initio molecular dynamics simulations demonstrate the ballistic character of the structural transition along the deformation vectors of the Peierls amplitude modes. Our work illustrates that coherent excitation of collective modes via exciton-phonon interactions evades entropic barriers and enables the dynamic control of materials functionality.

Phonon modes involved in triggering threshold phenomenon characterising sliding-velocity dependence of wearless nanofriction

ABSTRACT Wearless nanofriction between nonmetallic solids is investigated in terms of molecular dynamics (MD). The results of this study concern wearless-nanofrictional characteristics of the MD models in which the thermal-buffer zone is located far enough from the sliding interface so as not to disturb the heat generation mechanism. An enormous number of simulation runs and frequent validation of their results were carried out so that the pressure and the interfacial temperature, which directly affect the heat generation processes, were made common at different sliding velocities even under the above constraint. Sliding-velocity dependence of the ensemble-averaged frictional force density under the steady sliding condition is characterised by the threshold phenomenon. The dramatic increase in rate of the frictional-heat generation at sliding speeds above the threshold is triggered by resonant coherent excitation of certain phonon modes. Spatiotemporal patterns of such elastic waves hidden in random thermal motion of atoms near the sliding interface were clarified by the sampling and averaging. Features of these patterns are discussed in relation to the threshold characteristics of wearless nanofriction.

Spin-Mapping Methods for Simulating Ultrafast Nonadiabatic Dynamics

Many chemical reactions exhibit nonadiabatic effects as a consequence of coupling between electronic states and/or interaction with light. While a fully quantum description of nonadiabatic reactions is unfeasible for most realistic molecules, a more computationally tractable approach is to combine a classical description of the nuclei with a quantum description of the electronic states. Combining the formalisms of quantum and classical dynamics is however a difficult problem for which standard methods (such as Ehrenfest dynamics and surface hopping) may be insufficient. In this article, we review a new trajectory-based approach developed in our group that is able to describe nonadiabatic dynamics with a higher accuracy than previous approaches but for a similar level of computational effort. This method treats the electronic states with a phase-space representation for discrete-level systems, which in the two-level case is analogous to a spin-½. We point out the key features of the method and demonstrate its use in a variety of applications, including ultrafast transfer through conical intersections, damped coherent excitation under coupling to a strong light field, and nonlinear spectroscopy of light-harvesting complexes.

Coherent atomic orbital polarization probes the geometric phase in photodissociation of polyatomic molecules

AbstractQuantum interference between multiple pathways in molecular photodissociation often results in angular momentum polarization of atomic products and this can give deep insight into fundamental physical processes. For dissociation of diatomic molecules, the resulting orbital polarization is fully understood and consistent with quantum mechanical theory. For polyatomic molecules, however, coherent photofragment orbital polarization is frequently observed but so far has eluded theoretical explanation, and physical insight is lacking. Here, we present a model of these effects for ozone photodissociation that reveals the importance of a novel manifestation of the geometric phase. We show this geometric phase effect permits the existence of coherent polarization in cases where it would otherwise vanish, and cancels it in some cases where it might otherwise exist. The model accounts for measurements in ozone that have hitherto defied explanation, and represents a step toward a deeper understanding of coherent electronic excitation in polyatomic molecules and a new role of the geometric phase.Key Points Coherent photofragment atomic orbital polarization reveals matter wave interference in dissociation along multiple paths. In diatomic molecules, this is well‐understood, but in polyatomic molecules, large effects are seen but these have defied a rigorous explanation. A model is developed describing these phenomena in the UV dissociation of ozone that accounts for a number of conflicting observations and reveals a new manifestation of the geometric phase in molecular physics.

Spectral and generation properties of new coumarins – benzopyrylium derivatives

The spectral and generation parameters of coumarins, benzopyrylium derivatives, in ethanol and acetonitrile under coherent excitation were studied. It was found that the absorption spectra of the investigated compounds contain several maxima and the structuredness of the spectra is associated with their bichromophoric structure. It is shown that these organic dyes are bichromophoric compounds. It is noted that the nature of the substituents in positions 6 and 7 of the coumarin base and positions 6′ and 7′ of the benzopyrylium core determines their spectral-luminescent and lasing properties. It is demonstrated that the presence of substituents in certain positions of the coumarin base and the benzopyrylium core changes the conformation of the molecule and, accordingly, the dipole moments and oscillator strengths of the transition. The generation ability of coumarins of this class manifests itself only in the presence of the strongest donor substituents (for example, Et2N and OH) in position 7, and sufficiently strong acceptors in positions 6′ and 7′. Lasing was obtained in the spectral region of 730 –740 nm on dyes – benzopyrylium derivatives.

Enhanced optical mode coherence in exchange coupled soft magnetic multilayers

We report on an all-optical investigation of coupled spin excitation modes in a series of magnetic trilayer structures. Using time-resolved magneto-optic Kerr effect (tr-MOKE) magnetometry, we observe multi-mode coherent spin excitations in Ni81Fe19/Ru/Co49Fe49V2 multilayers even though the tr-MOKE optical detection is sensitive only to the Co49Fe49V2 magnetization dynamics. Frequency shifts of the different modes indicate that the coupling between the Ni81Fe19 and Co49Fe49V2 layers varies from anti-ferromagnetic to ferromagnetic to uncoupled as the Ru spacer layer thickness is increased from 8 Å to 200 Å. The lifetime of the high frequency coherent oscillations in the Co49Fe49V2 layer increases by over 200%–300% even in the case of uncoupled Ni81Fe19 and Co49Fe49V2 layers with a 200 Å thick Ru spacer. The results suggest an additional method to decrease the damping of high-moment alloys in layered magnetic nanostructures.

Enhanced Chemical Sensing with Multiorder Coherent Raman Scattering Spectroscopic Dephasing.

Molecular vibrational spectroscopy is widely used in various sensing and imaging applications, providing intrinsic information at the molecular level. Nonlinear optical interactions using ultrashort laser pulses facilitate the selective coherent excitation of molecular vibrational modes by focusing energy into specific molecular bonds, boosting the signal level for multiple orders of magnitude. The dephasing of such coherence, which is susceptible to the local molecular environment, however, is often neglected. The unique capability of vibrational dephasing dynamics to serve as a unique probe for complex molecular interactions and the effect of local nano- and microenvironments are beyond the reach of conventional, intensity-based spectroscopy. Here, we developed a novel multiorder coherent Raman spectroscopy platform with a special focus on the temporal evolution of molecular vibrational dephasing, termed as time-resolved coherent Raman scattering (T-CRS) spectroscopy. By utilizing a high dynamic range detection, molecular vibrational dynamics and the environmental effects are demonstrated with multidimensional spectroscopic sensing, which promises a new range of applications in biology, materials, and chemical sciences.

Spatiotemporal Analysis of Electromagnetic Field Coherence in Complex Media

We study the coherence in time and space of electromagnetic fields propagated through complex media. Whether for localization, imaging, or telecommunication, the development of dedicated numerical techniques is generally based on the exploitation of simplified models considering either coherent or diffuse fields. The optimization of such applications in conditions of partial coherence can therefore be particularly challenging, requiring the development of hybrid algorithms adaptable to prior knowledge on the processed fields. The objective of this work is to provide numerical techniques for decomposing an electromagnetic field into subspaces that can then be filtered according to their level of spatial and temporal coherence. In contrast to the studies carried out on space-space transfer matrices notably used for the calculation of Wigner-Smith operators, these decompositions are carried out on space-time matrices in order to facilitate the study of temporal dispersion. The theory is developed for illustrative purposes using experimental results from a leaky resonant system, but seem to be applicable to any scattering and reverberating media capable of transforming localized and coherent excitations into complex and diffuse distributions. To conclude this work, the proposed technique is exploited to improve image reconstruction in a millimeter-wave computational imaging demonstration. In the studied context and from a more general perspective, we propose a technique to select the most suitable subspaces for each application operating under conditions of partial coherence, whether these correspond in the most extreme cases to ballistic paths or to diffuse fields.

Direct convolution integration method for random vibration analysis of structures subjected to nonuniformly modulated nonstationary excitations

A comprehensive direct convolution integration method is presented in this study for the random vibration analysis of linear structures subjected to multiple nonuniformly modulated nonstationary excitations. The structural unit impulse responses with respect to each independent excitation are first identified and stored by a few time-history analyses. Then the structural response statistics are calculated by the direct convolution integration of unit impulse responses and excitation statistics. Further, two fast Fourier transform algorithms are presented to speed up the convolution integration. Because the convolution expressions are explicit, the presented method can be used to only calculate the responses at some specific degrees of freedom of interest in engineering. Furthermore, it can only calculate the responses at a small number of sparse moments in consideration of the time slow-varying property of nonstationary processes. Finally, the random vibration analysis of a frame structure excited by the fully coherent and incoherent nonstationary excitations is utilized to demonstrate its high accuracy and efficiency. Some suggestions of application are given.

SU(2) hyper-clocks: Quantum engineering of spinor interferences for time and frequency metrology

In 1949, Ramsey's method of separated oscillating fields was elaborated boosting over many decades metrological performances of atomic clocks and becoming the standard technique for very high precision spectroscopic measurements. A generalization of this interferometric method is presented replacing the two single coherent excitations by arbitrary composite laser pulses. The rotation of the state vector of a two-level system under the effect of a single pulse is described using the Pauli matrices basis of the SU(2) group. It is then generalized to multiple excitation pulses by a recursive Euler-Rodrigues-Gibbs algorithm describing a composition of rotations with different rotation axes. A general analytical formula for the phase-shift associated with the clock's interferometric signal is derived. As illustrations, hyper-clocks based on three-pulse and five-pulse interrogation protocols are studied and shown to exhibit nonlinear cubic and quintic sensitivities to residual probe-induced light-shifts. The presented formalism is well suited to optimize composite phase-shifts produced by tailored quantum algorithms in order to design a new generation of optical frequency standards and robust engineering control of atomic interferences in AMO physics with cold matter and anti-matter.

Avalanche structural rearrangements in cold dusty plasma liquids through cascaded coherent excitations of heterogeneous multiscale thermal acoustic waves

Microscopically, the cold liquid around freezing consists of crystalline ordered domains supporting thermally excited acoustic wave turbulence. Whether and how the above uncertain multiscale waves can lead to uncertain avalanche microstructure rearrangements in the form of multiscale clusters, and identifying their precursors, are elusive fundamental issues. Here, using a cold quasi-two-dimensional dusty plasma liquid as a platform, we experimentally address the above issues, especially the extreme avalanche activities, by correlating avalanche dynamics with the spatiotemporal evolutions of local structural order, defects, and the local amplitudes and phases of various wave modes. It is found that the preceding larger skeleton of poor structural order around more and widely spread defects can facilitate the later sequential multiscale wave excitations from slow to fast modes and their cascaded intermittent phase synchronizations for bond-breaking/reconnection and structural rearrangements. It is the key for the onset, spreading with defect propagation, and termination of the large avalanche cluster.

Stochastic Buffeting Analysis of Uncertain Long-Span Bridge Deck with an Optimized Method

The buffeting analysis of an uncertain long-span bridge deck was carried out in this paper. Due to the effect of strong spatial correlation of wind excitation, it should be assumed as partially coherent multiple excitations. The following includes a theoretical formula for the buffeting analysis of a long-span bridge deck with uncertain parameters, which was achieved mainly by a combination of the stochastic pseudo excitation method (SPEM) and response surface method (RSM). The SPEM-RSM was firstly applied to deal with the complicated spectral density function matrix of wind excitation. The buffeting response of the bridge deck was then calculated and verified by the results from the Monte Carlo simulation (MCS). The efficiency and applicability of the hybrid method for strong spatial correlation was proved. After the comparison, the effect of uncertain structural parameters and wind speed on the buffeting performance of the bridge deck were computed. The results showed that the whole uncertainties essentially affected the buffeting response of the deck. The uncertain wind speed played the most significant role in the vertical and lateral motion of the deck. The joint influences between structural uncertainties and uncertain wind speed further affect the random characteristics of the responses. Finally, the effects of different wind speed and wind angle of attack on the aerodynamic performance of the bridge are examined. The variance of the responses increased with the development of wind speed. The effect of different attack angles on the buffeting responses was significant.

Coherent two-beam steering of delocalized nonlinear photoluminescence in a plasmon cavity.

We aim at controlling the spatial distribution of nonlinear photoluminescence in a shaped micrometer-size crystalline gold flake. Interestingly, the underlying surface plasmon modal landscape sustained by this mesoscopic structure can be advantageously used to generate nonlinear photoluminescence (nPL) in remote locations away from the excitation spot. By controlling the modal pattern, we show that the delocalized nonlinear photoluminescence intensity can be redistributed spatially. This is first accomplished by changing the polarization orientation of the pulsed laser excitation in order to select a subset of available surface plasmon modes within a continuum. We then propose a second approach to redistribute the nPL within the structure by implementing a phase control of the plasmon interference pattern arising from a coherent two-beam excitation. Control and engineering of the nonlinear photoluminescence spatial extension is a prerequisite for deploying the next generation of plasmonic-enabled integrated devices relying on hot carriers.