Strong molecule-light interaction enables the control of molecular structures and dynamical processes. A model with strong laser drive is proposed to greatly enhance the intermolecular distance of resonant energy transfer, where the molecules are strongly driven by an optical cavity. The optimal Rabi frequency and quantum yield of energy transfer are observed, resulting from the trade off between dipole-dipole interaction and molecule-cavity coupling. When the strong drive at certain Rabi frequency is applied, a larger spatial range of effective energy transfer and a slower decay rate with the distance compared to the Förster mechanism of resonant energy transfer are observed in our model. Our work sheds light on spectroscopic study of the cooperative energy transfer in molecular polaritons.
We investigate the effect of a laser shining perpendicularly to a waveguide channeling two-level atoms. For weak transversal coupling the excitation of transverse atomic levels occurs at avoided crossings associated with "Rabi resonances" in which the Rabi frequency coincides with the transition frequency between the transverse levels.
Non Born-Oppenheimer quantum dynamics of H$_{2}^{+}$ excited by shaped one-cycle laser pulses linearly polarized along the molecular axis have been studied by the numerical solution of the time-dependent Schrödinger equation within a %three-body three-dimensional model, including the internuclear separation, $R$, and the electron coordinates $z$ and $ρ$. Laser carrier frequencies corresponding to the wavelengths $λ_{l}=25$~nm through $λ_{l}=400$~nm were used and the amplitudes of the pulses were chosen such that the energy of H$_{2}^{+}$ was close to its dissociation threshold at the end of an…
The amplitude and probability of quantum transitions are represented as a path integrals in energy state space of the investigated multi-level quantum system. Using this approach we consider rotational dynamics of nitrogen molecules $^{14}N_{2}$ and $^{15}N_{2}$ which interact with a sequence of ultrashort laser pulses. Our computer simulations indicate the complex dependency of the high rotation states excitation probability upon ultrashort laser pulses sequence periods. We observe pronounced resonances, which correspond to the results of some experiments.
Laser cooling of molecules employing broadband optical pumping involves a timescale separation between laser excitation and spontaneous emission. Here, we optimize the optical pumping step using shaped laser pulses. We derive two optimization functionals to drive population into those excited state levels that have the largest spontaneous emission rates to the target state. We show that, when using optimal control, laser cooling of molecules works even if the Franck-Condon map governing the transitions is preferential to heating rather than cooling. Our optimization functional is also applicab…
We study theoretically fast transfer of excitons between pairs of coupled quantum dots driven by the optical Stark effect that is produced by a short nonresonant laser pulse. The Schrödinger equation, in which the relative position of energy levels of quantum dot subsystems is time-dependent, is solved numerically. Computer simulation shows a way to achieve efficient excitation transfer by the action of a picosecond laser pulse with a rectangular envelope function.
A zeptosecond multi--MeV laser pulse may either excite a "plasma" of strongly interacting nucleons or a collective mode. We derive the conditions on laser energy and photon number such that either of these scenarios is realized. We use the nuclear Giant Dipole Resonance as a representative example, and a random--matrix description of the fine--structure states and perturbation theory as tools.
Nonlinear dynamics of establishment of electron-hole coherent superpositions states in graphene by multiphoton resonant excitation of interband transitions in laser fields is considered. The single-particle time dependent density matrix for such a quantized system is calculated in the multiphoton resonant approximation. The dependence of Rabi oscillations of Fermi-Dirac sea in graphene on the time, momentum, and photon number at multiphoton laser-excitation is analyzed.
The excitation dynamics of a laser-driven Rydberg gas exhibits a cooperative effect due to the interatomic Rydberg-Rydberg interaction, but the large many-body system with inhomogeneous Rydberg coupling is hard to exactly solved or numerically study by density matrix equations. In this paper, we find that the laser-driven Rydberg gas with most of the atoms being in the ground state can be described by a simplified interaction model resembling the optical Kerr effect if the distance-dependent Rydberg-Rydberg interaction is replaced by an infinite-range coupling. We can then quantitatively study…
We demonstrate a three step laser stabilisation scheme for excitation to nP and nF Rydberg states in 85Rb, with all three lasers stabilised using active feedback to independent Rb vapour cells. The setup allows stabilisation to the Rydberg states 36P3/2 to 70P3/2 and 33F7/2 to 90F7/2, with the only limiting factor being the available third step laser power. We study the scheme by monitoring the three laser frequencies simultaneously against a self-referenced optical frequency comb. The third step laser, locked to the Rydberg transition, displays an Allan deviation of 30 kHz over 1 second and <…
Antihydrogen production by charge exchange reaction between Positronium (Ps) atoms and antiprotons requires an efficient excitation of Ps atoms up to high-n levels (Rydberg levels). In this study it is assumed that a Ps cloud is produced within a relatively strong uniform magnetic field (1 Tesla) and with a relatively high temperature (100 K). Consequently, the structure of energy levels are deeply modified by Zeeman and motional Stark effects. A two-step laser light excitation, the first one from ground to n=3 and the second from this level to a Rydberg level, is proposed and the physics of t…
We explore a method for laser cooling and optical detection of excitations in a LC electrical circuit. Our approach uses a nanomechanical oscillator as a transducer between optical and electronic excitations. An experimentally feasible system with the oscillator capacitively coupled to the LC and at the same time interacting with light via an optomechanical force is shown to provide strong electro-mechanical coupling. Conditions for improved sensitivity and quantum limited readout of electrical signals with such an "optical loud speaker" are outlined.
Three-photon laser excitation of Rydberg states by three different laser beams can be arranged in a star-like geometry that simultaneously eliminates the recoil effect and Doppler broadening. Our analytical and numerical calculations for a particular laser excitation scheme 5S_{1/2}->5P_{3/2}->6S_{1/2}->nP in Rb atoms have shown that compared to the one- and two-photon laser excitation this approach provides much narrower line width and longer coherence time for both cold atom samples and hot vapors, if the intermediate one-photon resonances of the three-photon transition are detuned by more t…
Experimental realizations of two qubit entangling gates with trapped ions typically rely on addressing spectroscopically resolved motional sidebands, limiting gate speed to the secular frequency. Fast entangling gates using ultrafast pulsed lasers overcome this speed limit. This approach is based on state-dependent photon recoil kicks from a sequence of counter-propagating, resonant, ultrafast pulse pairs, which can allow sub-microsecond gate speeds. Here we demonstrate a key component of the ultrafast gate protocol, the coherent excitation of a 171Yb+ ion across the 2S1/2-2P1/2 transition wit…
The coherent radiation spectrum of two-level polar molecules with UV transition is studied at the multiphoton resonant excitation by a moderately strong laser field. The spectrum corresponding to harmonic generation and low-frequency radiation is investigated both analytically and numerically. Specifically, a mechanism for generation of intense smoothly tunable terahertz radiation by two-level molecular configurations (with dynamic Stark shifts) possessing permanent dipole moments, is considered.
We present a versatile laser system which provides more than 1.5W of narrowband light, tunable in the range from 455-463 nm. It consists of a commercial Titanium-Sapphire laser which is frequency doubled using resonant cavity second harmonic generation and stabilized to an external reference cavity. We demonstrate a wide wavelength tuning range combined with a narrow linewidth and low intensity noise. This laser system is ideally suited for atomic physics experiments such as two-photon excitation of Rydberg states of potassium atoms with principal quantum numbers n > 18. To demonstrate this we…
We propose a mechanism to produce a superposition of atomic and molecular states by a train of ultrashort laser pulses combined with weak control fields. By adjusting the repetition rate of the pump pulses and the intensity of the coupling laser, one can suppress a transition while simultaneously enhancing the desired transitions. As an example, various superpositions of vibrational states of the $K_2$ molecule are shown.
We derive the Heisenberg representation of the ultrafast inverse Faraday effect that provides the time evolution of magnetic vectors of a magnetic system during its interaction with a laser pulse. We obtain a time-dependent effective magnetic operator acting in the Hilbert space of the total angular momentum that describes a process of nonthermal excitation of magnetic precessions in an electronic system by a circularly polarized laser pulse. The magnetic operator separates the effect of the laser pulse on the magnetic system from other magnetic interactions. The effective magnetic operator pr…
We demonstrate a single-photon Rydberg excitation spectroscopy of cesium (Cs) atoms in a room-temperature vapor cell. Cs atoms are excited directly from 6S1/2 ground state to nP3/2 (n = 70 - 100) Rydberg states with a 318.6 nm ultraviolet (UV) laser,and Rydberg excitation spectra are obtained by transmission enhancement of a probe beam resonant to Cs 6S1/2, F = 4 - 6P3/2, F' = 5 transition as partial population on F = 4 ground state are transferred to Rydberg state .Analysis reveals that the observed spectra are velocity-selective spectroscopy of Rydberg state, from which the amplitude and lin…
We investigate experimentally the effect of quantum resonance in the rotational excitation of the simplest quantum rotor - a diatomic molecule. By using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detection, we measure directly the amount of energy absorbed by molecules interacting with a periodic train of laser pulses, and study its dependence on the train period. We show that the energy transfer is significantly enhanced at quantum resonance, and use this effect for demonstrating selective rotational excitation of two nitrogen isotopologues, $ ^{…
We investigate the dynamics of chiral edge states in topological polariton systems under laser driving. Using a model system comprised of topolgically trivial excitons and photons with a chiral coupling proposed by Karzig et al. [Phys. Rev. X 5, 031001 (2015)], we investigate the real-time dynamics of a lattice version of this model driven by a laser pulse. By analyzing the time- and momentum-resolved spectral function, measured by time- and angle-resolved photoluminescence in analogy with time- and angle-resolved photoemission spectroscopy in electronic systems, we find that polaritonic state…
We investigate the generation of higher-order harmonics from a quantum optics perspective via the interaction of a semiconductor with a coherent pump field focusing on the regime where strong-field intraband excitations dominate. The related Schrödinger equation for the system is solved approximately and the classical and quantum characteristics of the fundamental light mode as well as the higher frequency modes are analyzed. We find intricate but sufficiently mild modifications of the fundamental mode and coherent displacements depending on the position quadrature component of the driving las…
We examine the adiabatic preparation of crystalline phases of Rydberg excitations in a one-dimensional lattice gas by frequency sweep of the excitation laser, as proposed by Pohl et al. [Phys. Rev. Lett. 104, 043002 (2010)] and recently realized experimentally by Schauß et al. [Science 347, 1455 (2015)]. We find that the preparation of crystals of a few Rydberg excitations in a unitary system of several tens of atoms requires exceedingly long times for the adiabatic following of the ground state of the system Hamiltonian. Using quantum stochastic (Monte-Carlo) wavefunction simulations, we show…
The efficient excitation of quantum sources such as quantum dots or single molecules requires high NA optics which is often a challenge in cryogenics, or in ultrafast optics. Here we propose a 3.2 um wide parabolic mirror, with a 0.8 um focal length, fabricated by direct laser writing on CdSe/CdS colloidal quantum dots, capable of focusing the excitation light to a sub-wavelength spot and to extract the generated emission by collimating it into a narrow beam. This mirror is fabricated via in-situ volumetric optical lithography, which can be aligned to individual emitters, and it can be easily …
The interaction of a trapped ion with a laser beam in the strong excitation regime is analyzed. In this regime, a variety of non--classical states of motion can be prepared either by using laser pulses of well defined area, or by an adiabatic passage scheme based on the variation of the laser frequency. We show how these states can be used to investigate fundamental properties of quantum mechanics. We also study possible applications of this system to build an ion interferometer.
Combining topologically-protected chiral light transport and laser amplification gives rise to topological lasers, whose operation is immune to fabrication imperfections and defects, uncovering the role of topology in a novel nonlinear non-Hermitian regime. We study a topological laser based on the photonic Haldane model with selective pumping of chiral edge modes described by saturable gain. We investigate elementary excitations around the mean-field steady state and their consequences for the coherence properties. In particular, we show that the hybridization of chiral edge modes gives rise …
Following excitation by a strong ultra-short laser pulse, molecules develop coordinated rotational motion, exhibiting transient alignment along the direction of the laser electric field, followed by periodic full and fractional revivals that depend on the molecular rotational constants. In mixtures, the different species undergo similar rotational dynamics, all starting together but evolving differently with each demonstrating its own periodic revival cycles. For a bimolecular mixture of linear molecules, at predetermined times, one species may attain a maximally aligned state while the other …
We present experimental and theoretical study of single semiconductor quantum dots excited by two non-degenerate, resonantly tuned variably polarized lasers. The first laser is tuned to excitonic resonances. Depending on its polarization it photogenerates a coherent single exciton state. The second laser is tuned to biexciton resonances. By scanning the energy of the second laser for various polarizations of the two lasers, while monitoring the emission from the biexciton and exciton spectral lines, we map the biexciton photoluminescence excitation spectra. The resonances rich spectra of the s…
We propose a method to reconstruct the vibrational quantum state of molecules excited by a general excitation laser pulse. Unlike existing methods, we do not require the molecules before excitation to be in a pure state, allowing us to treat the important case of initially thermally excited molecules. Even if only a single initial level is appreciably populated, initial levels with small populations can still give major contributions to the unknown vibrational state, making it essential to take them into account. In addition to the excitation pulse, the method uses two incident, short laser pu…
A collapse and revival shape of Rabi oscillations of a single Nitrogen-Vacancy (NV) center electron spin has been observed in diamond at room temperature. Because of hyperfine interaction between the host 14N nuclear spin and NV center electron spin, different orientation of the 14N nuclear spin leads to a triplet splitting of the transition between the ground ms=0 and excited states ms=1. Microwave can excite the three transitions equally to induce three independent nutations and the shape of Rabi oscillations is a combination of the three nutations. This result provides an innovative view of…
We discuss the use of electromagnetically modified absorption to achieve selective excitation in atoms: that is, the laser excitation of one transition while avoiding simultaneously exciting another transition whose frequency is the same as or close to that of the first. The selectivity which can be achieved in the presence of electromagnetically induced transparency (EIT) is limited by the decoherence rate of the dark state. We present exact analytical expressions for this effect, and also physical models and approximate expressions which give useful insights into the phenomena. When the lase…
In an atomic ensemble, quantum information is typically carried as single collective excitations. It is very advantageous if the creation of single excitations is efficient and robust. Rydberg blockade enables deterministic creation of single excitations via collective Rabi oscillation by precisely controlling the pulse area, being sensitive to many experimental parameters. In this paper, we implement the adiabatic rapid passage technique to the Rydberg excitation process in a mesoscopic atomic ensemble. We make use of a two-photon excitation scheme with an intermediate state off-resonant and …
For molecules and materials responding to femtosecond-scale optical laser pulses, we predict maximum relative excitation of a Raman-active vibrational mode with period T when the pulse has an FWHM duration of 0.42 T. This result follows from a general analytical model, and is precisely confirmed by detailed density-functional-based dynamical simulations for C60 and a carbon nanotube, which include anharmonicity, nonlinearity, no assumptions about the polarizability tensor, and no averaging over rapid oscillations within the pulse. The mode specificity is, of course, best at low temperature and…
Superfluidity is an emergent quantum phenomenon which arises due to strong interactions between elementary excitations in liquid helium. These excitations have been probed with great success using techniques such as neutron and light scattering. However measurements to-date have been limited, quite generally, to average properties of bulk superfluid or the driven response far out of thermal equilibrium. Here, we use cavity optomechanics to probe the thermodynamics of superfluid excitations in real-time. Furthermore, strong light-matter interactions allow both laser cooling and amplification of…
We combine multi-channel electronic structure theory with quantum optimal control to derive Raman pulse sequences that coherently populate a valence excited state. For a neon atom, Raman target populations of up to 13% are obtained. Superpositions of the ground and valence Raman states with a controllable relative phase are found to be reachable with up to 4.5% population and phase control facilitated by the pump pulse carrier envelope phase. Our results open a route to creating core-hole excitations in molecules and aggregates that locally address specific atoms and represent the first step t…
The response of conduction band electrons to a local, pulse-like external excitation is investigated. The charge density wave packets that emerge as a consequence of the excitation leave the interaction region with a speed close to the initial state's band velocity, but there are also oscillations with essentially the same frequency as that of the laser field. As a good estimation, the excitation can also be considered as a localized, time-dependent ponderomotive potential, leading to slowly varying current oscillations. The role of all these effects are investigated for different electron ene…
We propose a method for the determination of the interaction potential of Rydberg atoms. Specifically, we consider a laser-driven Rydberg gas confined in a one-dimensional lattice and demonstrate that the Rydberg atom number after a laser excitation cycle as a function of the laser detuning provides a measure for the Rydberg interaction coefficient. With the lattice spacing precisely known, the proposed scheme only relies on the measurement of the number of Rydberg atoms and thus circumvents the necessity to map the interaction potential by varying the interparticle separation.
Two-photon excitation (TPE) proceeds via a "virtual" pathway, which depends on the accessibility of one or more intermediate states, and, in the case of non-centrosymmetric molecules, an additional "dipole" pathway involving the off-resonance dipole-allowed one-photon transitions and the change in the permanent dipole moment between the initial and final states. Here, we control the quantum interference between these two optical excitation pathways by using phase-shaped femtosecond laser pulses. We find enhancements by a factor of up to 1.75 in the two-photon-excited fluorescence of the photob…
