Tailored Light Fields Research Articles

Programmable generation of counterrotating bicircular light pulses in the multi-terahertz frequency range

The manipulation of solid states using intense infrared or terahertz light fields is a pivotal area in contemporary ultrafast photonics research. While conventional circular polarization has been well explored, the potential of counterrotating bicircular light remains widely underexplored, despite growing interest in theory. In the mid-infrared or multi-terahertz region, experimental challenges lie in difficulties in stabilizing the relative phase between two-color lights and the lack of available polarization elements. Here, we successfully generated phase-stable counterrotating bicircular light pulses in the 14–39 THz frequency range circumventing the above problems. Employing spectral broadening, polarization pulse shaping with a spatial light modulator, and intra-pulse difference frequency generation leveraging a distinctive angular-momentum selection rule within the nonlinear crystal, we achieved direct conversion from near-infrared pulses into the designed counterrotating bicircular multi-terahertz pulses. Use of the spatial light modulator enables programmable control over the shape, orientation, rotational symmetry, and helicity of the bicircular light field trajectory. This advancement provides a novel pathway for the programmable manipulation of light fields, and marks a significant step toward understanding and harnessing the impact of tailored light fields on matter, particularly in the context of topological semimetals.

Controlling the nonadiabatic dynamics of the charge-transfer process with chirped pulses: Insights from a double-pump time-resolved fluorescence spectroscopy scheme.

The manipulation of the ultrafast quantum dynamics of a molecular system can be achieved through the application of tailored light fields. This has been done in many ways in the past. In our present investigation, we show that it is possible to exert specific control over the nonadiabatic dynamics of a generic model system describing ultrafast charge-transfer within a condensed dissipative environment by using frequency-chirped pulses. By adjusting the external photoexcitation conditions, such as the chirp parameter, we show that the final population of the excitonic and charge-transfer states can be significantly altered, thereby influencing the elementary steps controlling the transfer process. In addition, we introduce an excitation scheme based on double-pump time-resolved fluorescence spectroscopy using chirped-pulse excitations. Here, our findings reveal that chirped excitations enhance the vibrational system dynamics as evidenced by the simulated spectra, where a substantial signal intensity dependence on the chirp is observed. Our simulations show that chirped pulses are a promising tool for steering the dynamics of the charge-transfer process toward a desired target outcome.

Coherent control of the photoinduced transition in a strongly correlated material

The use of intense tailored light fields is the perfect tool to achieve ultrafast control of electronic properties in quantum materials. Among them, Mott insulators are materials in which strong electron-electron interactions drive the material into an insulating phase. When shining a Mott insulator with a strong laser pulse, the electric field may induce the creation of doublon-hole pairs, triggering a photoinduced transition into a metallic state. In this paper, we take advantage of the threshold character of this photoinduced transition and we propose a setup that consists of a midinfrared laser pulse and a train of short pulses separated by a half period of the midinfrared with alternating phases. By varying the time delay between the two pulses and the internal carrier envelope phase of the short pulses, we achieve control of the phase transition, which leaves its fingerprint at its high harmonic spectrum.

Imprinting Chirality on Atoms Using Synthetic Chiral Light Fields.

Atoms are usually thought of as achiral objects. However, one can construct superpositions of atomic states that are chiral [1]. Here, we show how to excite such superpositions with tailored light fields both in the weak-field and strong-field regimes, using realistic laser parameters. First, we use time-dependent Schrödinger equation simulations to demonstrate the creation of a time-dependent bound chiral wave packet in sodium atoms. Second, we show how the time-dependent handedness of this wave packet can be probed by photoelectron circular dichroism, in spite of the central symmetry of the core potential. Third, we use time-dependent Schrödinger equation simulations to show how chirality can be directly imprinted on a photoelectron wave packet created by strong-field ionization and introduce an unambiguous chiral measure that allows us to characterize its handedness.

Fiber-based 3D nano-printed holography with individually phase-engineered remote points

The generation of tailored light fields with spatially controlled intensity and phase distribution is essential in many areas of science and application, while creating such patterns remotely has recently defined a key challenge. Here, we present a fiber-compatible concept for the remote generation of complex multi-foci three-dimensional intensity patterns with adjusted relative phases between individual foci. By extending the well-known Huygens principle, we demonstrate, in simulations and experiments, that our interference-based approach enables controlling of both intensity and phase of individual focal points in an array of spots distributed in all three spatial directions. Holograms were implemented using 3D nano-printing on planar substrates and optical fibers, showing excellent agreement between design and implemented structures. In addition to planar substrates, holograms were also generated on modified single-mode fibers, creating intensity distributions consisting of about 200 individual foci distributed over multiple image planes. The presented scheme yields an innovative pathway for phase-controlled 3D digital holography over remote distances, yielding an enormous potential application in fields such as quantum technology, life sciences, bioanalytics and telecommunications. Overall, all fields requiring precise excitation of higher-order optical resonances, including nanophotonics, fiber optics and waveguide technology, will benefit from the concept.

All-Optical Scheme for Generation of Isolated Attosecond Electron Pulses.

We theoretically propose an all-optical scheme for generation of isolated electron pulses with subfemtosecond durations for ultrafast electron microscopy and diffraction. The scheme is based on simultaneous longitudinal and transverse momentum modulation of freely propagating electrons at two distinct frequencies via ponderomotive interaction with tailored light fields of three phase-controlled laser pulses in vacuum. After a drift distance, an attosecond electron pulse train is formed with the individual pulses displaced in the transverse direction. Spatial filtering of the electron beam by an aperture leads to isolation of an individual attosecond pulse with a duration of <100 as. Subfemtosecond isolated electron pulses will enable direct space-time imaging of attosecond electronic dynamics in atoms, molecules, and solids with atomic spatial resolution, allowing us to directly observe phenomena such as electron tunneling or electron-electron interaction in strong laser fields of few-cycle laser pulses.

Polarization nano-tomography of tightly focused light landscapes by self-assembled monolayers

Recently, four-dimensional (4D) functional nano-materials have attracted considerable attention due to their impact in cutting-edge fields such as nano-(opto)electronics, -biotechnology or -biomedicine. Prominent optical functionalizations, representing the fourth dimension, require precisely tailored light fields for its optimal implementation. These fields need to be like-wise 4D, i.e., nano-structured in three-dimensional (3D) space while polarization embeds additional longitudinal components. Though a couple of approaches to realize 4D fields have been suggested, their breakthrough is impeded by a lack of appropriate analysis techniques. Combining molecular self-assembly, i.e., nano-chemistry, and nano-optics, we propose a polarization nano-tomography of respective fields using the functional material itself as a sensor. Our method allows a single-shot identification of non-paraxial light fields at nano-scale resolution without any data post-processing. We prove its functionality numerically and experimentally, elucidating its amplitude, phase and 3D polarization sensitivity. We analyze non-paraxial field properties, demonstrating our method’s capability and potential for next generation 4D materials.

Light-emitting metasurfaces

Abstract Photonic metasurfaces, that is, two-dimensional arrangements of designed plasmonic or dielectric resonant scatterers, have been established as a successful concept for controlling light fields at the nanoscale. While the majority of research so far has concentrated on passive metasurfaces, the direct integration of nanoscale emitters into the metasurface architecture offers unique opportunities ranging from fundamental investigations of complex light-matter interactions to the creation of flat sources of tailored light fields. While the integration of emitters in metasurfaces as well as many fundamental effects occurring in such structures were initially studied in the realm of nanoplasmonics, the field has recently gained significant momentum following the development of Mie-resonant dielectric metasurfaces. Because of their low absorption losses, additional possibilities for emitter integration, and compatibility with semiconductor-based light-emitting devices, all-dielectric systems are promising for highly efficient metasurface light sources. Furthermore, a flurry of new emission phenomena are expected based on their multipolar resonant response. This review reports on the state of the art of light-emitting metasurfaces, covering both plasmonic and all-dielectric systems.

Polarization Singularity Explosions in Tailored Light Fields (Laser Photonics Rev. 12(6)/2018)

Singular Optics Optical singularities belong to the most fundamental properties of light. In article number 1700200, Eileen Otte and co-workers tailor and investigate singularity “explosions” by combining perturbed higher-order phase and polarization singularities. These complex spatio-temporal propagation dynamics include singularity unfolding, type conversion, annihilation and creation, revealing fascinating properties of structured light fields.

Polarization Singularity Explosions in Tailored Light Fields

AbstractComplex propagation dynamics of higher‐order polarization singularities are investigated within tailored Poincaré beams. Spatial polarization modulation and additional phase vortices of higher strength are combined, evoking polarization singularity splitting, type conversion, creation and annihilation. These phenomena form singularity “explosions” along their longitudinal evolution. These dynamics of propagating customized light fields and embedded singularities are analyzed experimentally and numerically. Furthermore, similarities of polarization singularity explosion and phase vortex unfolding are discussed, exploring fundamental propagation and spatio‐temporal interaction properties of optical singularities.

Ultrahigh-definition dynamic 3D holographic display by active control of volume speckle fields

Holographic displays generate realistic 3D images that can be viewed without the need for any visual aids. They operate by generating carefully tailored light fields that replicate how humans see an actual environment. However, the realization of high-performance, dynamic 3D holographic displays has been hindered by the capabilities of present wavefront modulator technology. In particular, spatial light modulators have a small diffraction angle range and limited pixel number limiting the viewing angle and image size of a holographic 3D display. Here, we present an alternative method to generate dynamic 3D images by controlling volume speckle fields significantly enhancing image definition. We use this approach to demonstrate a dynamic display of micrometre-sized optical foci in a volume of 8 mm × 8 mm × 20 mm. Control of speckle fields yields high-definition 3D holographic images.

Waveform-Controlled Relativistic High-Order-Harmonic Generation.

We consider the efficiency limit of relativistic high-order-harmonic emission from solid targets achievable with tailored light fields. Using one-dimensional particle-in-cell simulations, the maximum energy conversion efficiency is shown to reach as high as 10% for the harmonics in the range of 80-200eV and is largely independent of laser intensity and plasma density. The waveforms most effective at driving harmonics have a broad spectrum with a lower-frequency limit set by the width of the incident pulse envelope and an upper limit set by the relativistic plasma frequency.

Theory for optical assembling of anisotropic nanoparticles by tailored light fields under thermal fluctuations

In order to evaluate the assembling processes of arbitrary-shaped nanoparticles (NPs) by the irradiation of a tailored laser beam under thermal fluctuations, we have developed a “Light-induced-force Nano Metropolis Method (LNMM)” as a new theoretical method based on the stochastic algorithm in the energy region and the general formula of light-induced force. By using LNMM, we have investigated the change of configurations of silver NPs with anisotropic shapes under the irradiation of laser beams with various polarizations and intensity distributions (Gaussian beam and axially-symmetric vector beams) in an aqueous solution at room temperature. As a result, it has been clarified that silver NPs can be selectively arranged into a characteristic spatial configuration reflecting the properties of an irradiated laser beam (wavelength, intensity distribution, and polarization distribution), and that the assembled structures possess broadband spectra and exhibit a strong optical response to the irradiated laser beam through the optimization with the help of fluctuations.

Three‐Dimensional Exploration and Mechano‐Biophysical Analysis of the Inner Structure of Living Cells

A novel mechanobiological method is presented to explore qualitatively and quantitatively the inside of living biological cells in three dimensions, paving the way to sense intracellular changes during dynamic cellular processes. For this purpose, holographic optical tweezers, which allow the versatile manipulation of nanoscopic and microscopic particles by means of tailored light fields, are combined with self-interference digital holographic microscopy. This biophotonic holographic workstation enables non-contact, minimally invasive, flexible, high-precision optical manipulation and accurate 3D tracking of probe particles that are incorporated by phagocytosis in cells, while simultaneously quantitatively phase imaging the cell morphology. In a first model experiment, internalized polystyrene microspheres with 1 μm diameter are three-dimensionally moved and tracked in order to quantify distances within the intracellular volume with submicrometer accuracy. Results from investigations on cell swelling provoked by osmotic stimulation demonstrate the homogeneous stretching of the cytoskeleton network, and thus that the proposed method provides a new way for the quantitative 3D analysis of the dynamic intracellular morphology.

Tailored Light Fields: A Novel Approach for Creating Complex Optical Traps

Get PDF Email Share Share with Facebook Tweet This Post on reddit Share with LinkedIn Add to CiteULike Add to Mendeley Add to BibSonomy Get Citation Copy Citation Text C. Alpmann , M. Woerdemann, and C. Denz, "Tailored Light Fields: A Novel Approach for Creating Complex Optical Traps," Optics & Photonics News 22(12), 28-28 (2011) Export Citation BibTex Endnote (RIS) HTML Plain Text Citation alert Save article

Ultrafast laser control of electron dynamics in atoms, molecules and solids

Exploiting coherence properties of laser light together with quantum mechanical matter interferences in order to steer a chemical reaction into a pre-defined target channel is the basis of coherent control. The increasing availability of laser sources operating on the time scale of molecular dynamics, i.e. the femtosecond regime, and the increasing capabilities of shaping light in terms of amplitude, phase and polarization also on the time scale of molecular dynamics brought the temporal aspect of this field to the fore. Since the last Faraday Discussion (Faraday Discussion 113, Stereochemistry and control in molecular reaction dynamics) devoted to this topic more than a decade ago a tremendous cross-fertilization to neighbouring "quantum technology disciplines" in terms of experimental techniques and theoretical developments has occurred. Examples are NMR, quantum information, ultracold molecules, nonlinear spectroscopy and microscopy and extreme nonlinear optics including attosecond-science. As pointed out by the organizers, this meeting brings us back to chemistry and aims to assess recent progress in our general understanding of coherence and control in chemistry and to define new avenues for the future. To that end we will in the Introductory lecture first shortly review some aspects of coherent control. This will not be fully comprehensive and is mainly meant to give some background to current experimental efforts of our research group in controlling (coherent) electronic excitations with tailored light fields. Examples and perspectives for the latter will be given.

Riemannζfunction from wave-packet dynamics

We show that the time evolution of a thermal phase state of an anharmonic oscillator with logarithmic energy spectrum is intimately connected to the generalized Riemann $\ensuremath{\zeta}$ function $\ensuremath{\zeta}(s,a)$. Indeed, the autocorrelation function at a time $t$ is determined by $\ensuremath{\zeta}(\ensuremath{\sigma}+i\ensuremath{\tau},a)$, where $\ensuremath{\sigma}$ is governed by the temperature of the thermal phase state and $\ensuremath{\tau}$ is proportional to $t$. We use the JWKB method to solve the inverse spectral problem for a general logarithmic energy spectrum; that is, we determine a family of potentials giving rise to such a spectrum. For large distances, all potentials display a universal behavior; they take the shape of a logarithm. However, their form close to the origin depends on the value of the Hurwitz parameter $a$ in $\ensuremath{\zeta}(s,a)$. In particular, we establish a connection between the value of the potential energy at its minimum, the Hurwitz parameter and the Maslov index of JWKB. We compare and contrast exact and approximate eigenvalues of purely logarithmic potentials. Moreover, we use a numerical method to find a potential which leads to exact logarithmic eigenvalues. We discuss possible realizations of Riemann $\ensuremath{\zeta}$ wave-packet dynamics using cold atoms in appropriately tailored light fields.

Control of Molecular Fragmentation Using Shaped Femtosecond Pulses

The possibility that chemical reactions may be controlled by tailored femtosecond laser pulses has inspired recent studies that take advantage of their short pulse duration, comparable to intramolecular dynamics, and high peak intensity to fragment and ionize molecules. In this article, we present an experimental quest to control the chemical reactions that take place when isolated molecules interact with shaped near-infrared laser pulses with peak intensities ranging from 1013 to 1016 W/cm2. Through the exhaustive evaluation of hundreds of thousands of experiments, we methodically evaluated the molecular response of 16 compounds, including isomers, to the tailored light fields, as monitored by time-of-flight mass spectrometry. Analysis of the experimental data, taking into account its statistical significance, leads us to uncover important trends regarding the interaction of isolated molecules with an intense laser field. Despite the energetics involved in fragmentation and ionization, the integrated second-harmonic generation of a given laser pulse (ISHG), which was recorded as an independent diagnostic parameter, was found to be linearly proportional to the total ion yield (IMS) generated by that pulse in all of our pulse shaping measurements. Order of magnitude laser control over the relative yields of different fragment ions was observed for most of the molecules studied; the fragmentation yields were found to vary monotonically with IMS and/or ISHG. When the extensive changes in fragmentation yields as a function of IMS were compared for different phase functions, we found essentially identical results. This observation implies that fragmentation depends on a parameter that is responsible for IMS and independent from the particular time-frequency structure of the shaped laser pulse. With additional experiments, we found that individual ion yields depend only on the average pulse duration, implying that coherence does not play a role in the observed changes in yield as a function of pulse shaping. These findings were consistently observed for all molecules studied (p-, m-, o-nitrotoluene, 2,4-dinitrotoluene, benzene, toluene, naphthalene, azulene, acetone, acetyl chloride, acetophenone, p-chrolobenzonitrile, N,N-dimethylformamide, dimethyl phosphate, 2-chloroethyl ethyl sulfide, and tricarbonyl-[eta5-1-methyl-2,4-cyclopentadien-1-yl]-manganese). The exception to our conclusion is that the yield of small singly-charged fragments resulting from a multiple ionization process in a subset of molecules, were found to be highly sensitive to the phase structure of the intense pulses. This coherent process plays a minimal role in photofragmentation; therefore, we consider it an exception rather than a rule. Changes in the fragmentation process are dependent on molecular structure, as evidenced in a number of isomers, therefore femtosecond laser fragmentation could provide a practical dimension to analytical chemistry techniques.

Quantum control of dissipative systems: Exact solutions

Optimal quantum control theory, which predicts the tailored light fields that best drive a system to a desired target, is applied to the quantum dissipative dynamics of systems linearly coupled to a Gaussian bath. To calculate the material response function required for optimizing the light field, the analytical solution is derived for the two-level Brownian harmonic oscillator model and the recently developed method for directly simulating the Gaussian force is implemented for anharmonic Brownian oscillators. This study confirms the feasibility of quantum control in favorable condensed phase environments and explores new quantum control features in the presence of dissipation, including memory effects and temperature dependence.

Mode-locking matter with light

Theory and experiments are currently being developed in our laboratory to use tailored light fields to control the dynamics of molecular reactions. We have recently shown theoretically that a properly chirped light pulse can be used to overcome the natural tendency of wave packets to spread on anharmonic molecular potential energy surfaces. The optimal chirp rate can be readily obtained by solving a linear optimal control equation. In this paper we analyze a number of aspects crucial to the success of the experiments. We test the robustness of the optimal electric field with respect to variations in the field parameters (chirp rates, pulse duration, and carrier frequency). We also study the effects of finite temperature by using a thermal vibrational distribution as the initial in the dynamics