Engineering quantum control with optical transitions induced by twisted light fields

We present results of experimental work in which the coherent‐control technique has been applied to study the coherent manipulation of excitonic polarization in ZnSe quantum‐well samples. We will introduce the linear control of excitonic polarization in pulse‐transmission experiments and afterwards focus on the question if and how the optical transition from the excitonic states to the bound‐biexciton state can be subject to a directed coherent control. The experimental results will be compared to simulations based on a microscopic theory and will also be explained on the base of a phenomenological few‐level model. The overall suitability of coherent control for the investigation of exciton systems in low‐dimensional wide‐gap materials will be discussed. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Atom lithography is a technique to structure layers of atoms during deposition, using interactions of near-resonant light fields with neutral atoms. The basic scheme uses a standing wave light field, aligned just above a substrate, while a beam of atoms impinges perpendicularly on the standing wave light field. The interaction of the light field and the atoms focuses the atoms towards the crests or troughs of the standing wave intensity, dependent on the tuning of the light field. The focused atoms are subsequently deposited on the substrate, resulting in an array of lines, whose periodicity is determined by the wavelength of the light field. The standing wave light field can therefore be seen as an array of lenses, focusing the atom beam into an array of lines. The first experiments on atom lithography were performed in the 1990s with sodium and chromium. In this thesis experiments with iron are described, which is a magnetic element and thus allows for the creation of magnetic nanostructures. To focus atom beams into structures using atom lithography, well-colimated atom beams are required. The most common technique to create collimated atom beams is transverse laser cooling, but iron has no closed optical transition suitable for laser cooling. Fortunately Smeets and Te Sligte found that even then atom lithography of iron is possible. If the standing wave light field is considered to be an array of lenses, the focusing of the atom beam on a single lens is determined by the local collimation of the atom beam at that position. This local collimation is determined by the geometry of the beam source and the distance of the beam source to the standing wave lens. Using a small beam source (e.g. 1 mm diameter) positioned far from the standing wave (e.g. 1 m), the geometrically collimated atom beam is suitable for atom lithography. Chapter 3 shows what the implications of geometric collimation are on the structure formation in atom lithography. The geometric effects that locally collimate the atom beam on the sample also introduce local offset angles of the atom beam with respect to the focusing light field. Structure formation has been observed with lines of up to 7 nm high on a background layer of 15 nm average height, over areas of up to 400 µm × 6 mm. This indicates that the offset angles can vary over an 8 mrad range, which is more than an order of magnitude larger than the local angle of collimation. The offset angle influence the local geometry of the deposited structures: an increasing offset angle decreases the local line height, increases the width and creates a skewness in the local line shape. The local geometry of the lines has been modelled with a Monte Carlo particle tracking model and the results were compared to experiments. It was found that the highest and narrowest lines suffer from significant broadening due to surface diffusion in experiments, limiting the achievable structure width of iron on SiOx samples to about 80 nm. We have also found that in atom lithography without laser cooling, each standing wave lens is effectively imaging the source geometry onto the substrate. We therefore propose using structured atom beam sources to image more complex patterns on sub-wavelength scales in a parallel way. The reason to use iron in atom lithography, is the option to create magnetic nanostructures. However, in previous experiments no clear magnetic signature of the atom lithographic structuring of iron was found. Therefore in Chapter 4 firstly the magnetic properties of unstructured layers of iron (Fe), nickel (Ni) and FexNi1-x are investigated. These layers are all ferromagnetic, but with a reduced magnetic moment compared to bulk values due to contaminations and crystal growth effects. As a reference for periodic atom lithography structures, periodic line structures are created with interference lithography in a polymer layer and onto these structures thin layers of FexNi1-x are shadow deposited, thereby creating a layer periodically modulated in both height and elemental composition. This periodic modulation in composition has been observed with SEM-EDX on sub-micron scales. The structures showed a clear magnetic anisotropy with an easy axis along the direction of the lines, in accordance with expectations. In Chapter 5, the magnetic properties of atom lithographic iron line structures are presented. Using MOKE microscopy, direct comparison of structured and unstructured parts of a sample is possible, which allows for the observation of clear magnetic signatures due to the atom lithographic structuring. In layers of an average thickness of about 15 nm, no anisotropy is induced by the line structures, while a magnetic easy axis along the direction of the lines is expected. The line structures introduce an isotropic increase in the coercivity of the layers, indicating that the line structures can be considered as isotropic corrugations instead of directional line structures. For layers of 30 nm average thickness and thus higher line structures, a clear magnetic anisotropy is observed for the highest line structures. This anisotropy can be seen as a magnetic easy axis along the direction of the lines, as expected for line structures. However, we also observe a sharp increase in coercivity for applied fields perpendicular to the lines. This phenomenon is intriguing and may be explained by a pinning of head-to-head domain walls along the direction of the lines. In Chapter 5, we also report on the first results of co-deposition of FexNi1-x, where the Fe is structured into lines using atom lithography, while the Ni is deposited uniformly, thereby creating an alloy of modulating composition. Magnetic analysis of these structures indicates that these structures are anisotropic, both the coercivity and the shape of domain walls is dependent on the angle of the applied field relative to the line structures. Finally in Chapter 6, we investigate the possibilities to focus a thermal beam of atoms into a single 100 nm spot using light fields, thereby creating a nanopencil suitable for deposition of nanostructures. A Monte Carlo particle tracking program was developed to model the all optical focusing or funneling of 10 µm sized atom beams to a 100 nm spot. This model included effects of initial beam divergence, magnetic substructure, laser cooling, and spontaneous as well as stimulated diffusion and it was applied to a number of promising light field configurations. The best results obtained for experimentally realistic settings are a beam focused to a full width at half maximum of FWHM = 0.55 µm in a blue detuned hollow beam where atoms are focused towards the dark center, or a FWHM = 0.31 µm in a red detuned axicon light field, where atoms are focused towards the maximum intensity at the heart line. However, in the latter case the focused beam has a flux only 25 times larger than the background flux, which is unpractical for applications. The limiting factors of all schemes are heating due to stimulated diffusion and the limited interaction time available for a thermal beam of atoms. A nanopencil could be possible if it were based on the focussing of a slow and / or monochromatic atom beam, but this would seriously complicate the practical application of such a device.

Coherent control of quantum dynamics is key to a multitude of fundamental studies and applications1. In the visible or longer-wavelength domains, near-resonant light fields have become the primary tool with which to control electron dynamics2. Recently, coherent control in the extreme-ultraviolet range was demonstrated3, with a few-attosecond temporal resolution of the phase control. At hard-X-ray energies (above 5–10 kiloelectronvolts), Mössbauer nuclei feature narrow nuclear resonances due to their recoilless absorption and emission of light, and spectroscopy of these resonances is widely used to study the magnetic, structural and dynamical properties of matter4,5. It has been shown that the power and scope of Mössbauer spectroscopy can be greatly improved using various control techniques6–16. However, coherent control of atomic nuclei using suitably shaped near-resonant X-ray fields remains an open challenge. Here we demonstrate such control, and use the tunable phase between two X-ray pulses to switch the nuclear exciton dynamics between coherent enhanced excitation and coherent enhanced emission. We present a method of shaping single pulses delivered by state-of-the-art X-ray facilities into tunable double pulses, and demonstrate a temporal stability of the phase control on the few-zeptosecond timescale. Our results unlock coherent optical control for nuclei, and pave the way for nuclear Ramsey spectroscopy17 and spin-echo-like techniques, which should not only advance nuclear quantum optics18, but also help to realize X-ray clocks and frequency standards19. In the long term, we envision time-resolved studies of nuclear out-of-equilibrium dynamics, which is a long-standing challenge in Mössbauer science20.

Coherent control of electron intersubband transitions by frequency-detuned light fields

Films of the topological insulator Bi2Se3 are grown by molecular beam epitaxy with in-situ reflection high-energy electron diffraction. The films are shown to be high-quality by X-ray reflectivity and diffraction and atomic-force microscopy. Quantum interference control of photocurrents is observed by excitation with harmonically related pulses and detected by terahertz radiation. The injection current obeys the expected excitation irradiance dependence, showing linear dependence on the fundamental pulse irradiance and square-root irradiance dependence of the frequency-doubled optical pulses. The injection current also follows a sinusoidal relative-phase dependence between the two excitation pulses. These results confirm the third-order nonlinear optical origins of the coherently controlled injection current. Experiments are compared to a tight-binding band structure to illustrate the possible optical transitions that occur in creating the injection current.

Over the past few years quantum control has proven to be very successful in steering molecular processes. By combining theory with experiment, even highly complex control aims were realized in the gas phase. In this topical review, we illustrate the past achievements on several examples in the molecular context. The next step for the quantum control of chemical processes is to translate the fruitful interplay between theory and experiment to the condensed phase and thus to the regime where chemical synthesis can be supported. On the theory side, increased efforts to include solvent effects in quantum control simulations were made recently. We discuss two major concepts, namely an implicit description of the environment via the density matrix algorithm and an explicit inclusion of solvent molecules. By application to chemical reactions, both concepts conclude that despite environmental perturbations leading to more complex control tasks, efficient quantum control in the condensed phase is still feasible.

Chapter 3 - Coherence Effects in Laser-Induced Continuum Structure

Based on weak field quantum control theory, a semiclassical approximation relates the characteristic parameters of the tailored light field to corresponding classical dynamical quantities and thus reveals the underlying physical basis of wave packet focusing. A coordinate-dependent two-level-system approximation is employed to further analyze the molecular dynamics induced by short laser pulses, thus leading to a simple interpretation of the observed correlation between the pulse chirp and vibrational focusing and defocusing. Though our study is presented in the context of quantum control, the conclusions are general, providing an intuitive picture of the quantum coherence of light–matter interaction and a guideline for the design of tailored laser fields.

We optically generated an electronic state in a single InAs/GaAs self-assembled quantum dot that is a precursor to the deterministic entanglement of the spin of the electron with an emitted photon in the proposal of W. Yao, R.-B. Liu, and L. J. Sham [Phys. Rev. Lett. 95, 030504 (2005). A superposition state is prepared by optical pumping to a pure state followed by an initial pulse. By modulating the subsequent pulse arrival times and precisely controlling them using interferometric measurement of path length differences, we are able to implement a coherent control technique to selectively drive exactly one of the two components of the superposition to the ground state. This optical transition contingent on spin was driven with the same broadband pulses that created the superposition through the use of a two pulse coherent control sequence. A final pulse affords measurement of the coherence of this "preentangled" state.

Optically active defects in solids---colour centres---are one of the most promising platforms for implementing quantum technologies. Their spin degrees of freedom serve as quantum memories that in some cases can operate at room temperature. Their control can be achieved with microwave spin control and resonant optical excitation but is hindered by the broadening of optical transitions from thermal phonons and spectral diffusion. Furthermore, spin-qubit optical transitions are often outside the telecommunications wavelength band required for long-distance fiber optic transmission. Harnessing the coupling between mechanical degrees of freedom and spins has emerged as an alternative route for controlling spin-qubits. However, connecting spin-mechanical interfaces to optical links to realize a spin-photon interface has remained a challenge. Here we demonstrate such an interface using a diamond optomechanical cavity that does not depend on optical transitions and can be applied to a wide range of spin qubits. Our device consists of a diamond microdisk resonator studied in [Optica 3, 963-970 (2016)]. The microdisk is fabricated from optical grade diamond that contains ensembles of NV centres. We use an optical mode at 1564 nm with the quality factor Qo = 150k. The mechanical mode which we use to couple to the NV spin state is a radial breathing mode with a frequency of around 2.1 GHz with the quality factor Qm = 4k. The device operates in the sideband resolved regime enabling optomechanical self-induced oscillations for sufficiently high optical input power of a blue detuned laser. These oscillations can produce the stress of a few MPa, large enough to drive the electronic spins of NV centers. We use a standard diamond NV confocal microscope to initialize and readout the NV state. The MW pulses transfer the population between |-1⟩|0⟩ and |+1⟩|0⟩ state. We wait for 0.7 us with the mechanical drive that drives the |-1⟩|+1⟩ transition. In our measurements, we observe a coinciding dip in the |+1⟩ population and a peak |-1⟩ population, that verifies that the spins are being optomechanically driven. On calibrating this signal with the MW Rabi contrast and the background signal, we estimate a driving rate of 2pix170kHz and ~45% transfer of spin population between |±1⟩ states. Feasible improvements in device geometry will increase the optomechanically-induced driving rate by a few orders of magnitude allowing for coherent control of NV spins using an optomechanical resonator.

Coherent light sources have been widely used in control schemes that exploit quantum interference effects to direct the outcome of photochemical processes. The adaptive shaping of laser pulses is a particularly powerful tool in this context: experimental output as feedback in an iterative learning loop refines the applied laser field to render it best suited to constraints set by the experimenter. This approach has been experimentally implemented to control a variety of processes, but the extent to which coherent excitation can also be used to direct the dynamics of complex molecular systems in a condensed-phase environment remains unclear. Here we report feedback-optimized coherent control over the energy-flow pathways in the light-harvesting antenna complex LH2 from Rhodopseudomonas acidophila, a photosynthetic purple bacterium. We show that phases imprinted by the light field mediate the branching ratio of energy transfer between intra- and intermolecular channels in the complex's donor acceptor system. This result illustrates that molecular complexity need not prevent coherent control, which can thus be extended to probe and affect biological functions.

Theoretical analysis leads us to the intriguing conclusion that nearly complete electronic population inversion of molecules can be achieved with intense positively chirped broadband laser pulses, as a combined result of vibrational coherence and adiabatic inversion. Strong field quantum calculations demonstrate inversion probabilities of up to 99%. The results are robust with respect to changes in light field parameters as well as to thermal and condensed phase conditions, are supported by experimental evidence, and have many potential applications in chemistry, biochemistry, biology, and physics. [S0031-9007(97)05267-8] PACS numbers: 42.50.Hz, 33.80. ‐ b Optimal inversion of the electronic population of a molecular system [1‐7] is an intriguing theoretical problem which has many potential experimental applications to a variety of fields such as (i) the suppression of ground state interference in many types of excited electronic state spectroscopy, scattering, and diffraction experiments, (ii) more effective impulsive photoinitiation of chemical and biochemical reactions as well as their quantum control, (iii) more effective pumping of molecular lasers, (iv) brighter short-pulse fluorescence microscopy of biological samples, and (v) induced transparency. In particular, for many biochemical and biophysical experiments, one would like to achieve maximal electronic excitation or initiation of chemical reactions without damaging the excited molecules or the delicate environment of living cells. In atoms [8] and in some spin systems (nuclear magnetic resonance), where two level approximations are reasonable, complete population inversion by pulses of electromagnetic radiation, where the entire population of one state is transferred to another state, is a long-established technique. The parallel solution for the electronic population of molecules, with their multiple rovibrational states, has not previously been found, although several theoretical calculations have been made [9 ‐ 12]. In this Letter, we demonstrate that such a solution does exist for molecular systems and can be understood with simple physical models. We show that this solution is robust with respect to variation of the parameters of the “pulses” as well as robust to the effects of temperature and of intermolecular interactions. Finally, we point to recent experimental evidence supporting these conclusions. For atoms and quasi-two-level systems, a resonant p pulse has a bandwidth broader than the transition line but narrow enough as to avoid overlap with neighboring absorption lines. A parallel argument for molecular systems suggests that the bandwidth of a possible molecular p pulse should be on the same order as the width of the corresponding molecular absorption spectrum, which is approximately 10 2 to 10 3 cm 21 at room temperature. Ac

In recent years, significant progress has been achieved in manipulating matter with light, and light with matter. Resonant laser fields interacting with cold, dense atom clouds provide a particularly rich system. Such light fields interact strongly with the internal electrons of the atoms, and couple directly to external atomic motion through recoil momenta imparted when photons are absorbed and emitted. Ultraslow light propagation in Bose-Einstein condensates represents an extreme example of resonant light manipulation using cold atoms. Here we demonstrate that a slow light pulse can be stopped and stored in one Bose-Einstein condensate and subsequently revived from a totally different condensate, 160 mum away; information is transferred through conversion of the optical pulse into a travelling matter wave. In the presence of an optical coupling field, a probe laser pulse is first injected into one of the condensates where it is spatially compressed to a length much shorter than the coherent extent of the condensate. The coupling field is then turned off, leaving the atoms in the first condensate in quantum superposition states that comprise a stationary component and a recoiling component in a different internal state. The amplitude and phase of the spatially localized light pulse are imprinted on the recoiling part of the wavefunction, which moves towards the second condensate. When this 'messenger' atom pulse is embedded in the second condensate, the system is re-illuminated with the coupling laser. The probe light is driven back on and the messenger pulse is coherently added to the matter field of the second condensate by way of slow-light-mediated atomic matter-wave amplification. The revived light pulse records the relative amplitude and phase between the recoiling atomic imprint and the revival condensate. Our results provide a dramatic demonstration of coherent optical information processing with matter wave dynamics. Such quantum control may find application in quantum information processing and wavefunction sculpting.

A theory of coherent control of spontaneous secondary emission of semiconductor quantum dots resonantly excited by two phase-locked laser pulse trains has been developed. We have considered quasi-elastic, optical-phonon assisted, and thermalized components of the emission with respect to a study of elementary excitation dynamics. The analysis of the time-integrated signal of the emission depending on a mutual delay between the pulses has shown that the coherent control technique is promising in the determination of dephasing rates of resonant optical transitions for both a single quantum dot and an ensemble of dots with a large inhomogeneous broadening. The role of the signal spectral selection for reliable determination of the dephasing rates has been clarified.

Summary form only given. The nonlinear optical response of semiconductor microcavities in the nonperturbative regime has been the subject of many recent experiments. Contrary to clear demonstrations of the quantized nature of the vacuum-field Rabi splitting of a single atom, most of the experiments on semi-conductor microcavities could be explained in terms of a classical light field. Only recently, quantized light field effects have been reported in a coherent control experiment (Lee et al, 1999) and theoretically investigated in secondary emission (Kira et al, 1999). Here, results are presented that display a pronounced third transmission maximum lying energetically between the two normal modes. The third peak can be observed in resonant femtosecond single-beam as well as picosecond pump-probe experiments under various excitation conditions.