Cooling molecular vibrations with shaped laser pulses: Optimal control theory exploiting the timescale separation between coherent excitation and spontaneous emission
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 applicable to the laser cooling of other degrees of freedom provided the cooling cycle consists of coherent excitation and dissipative deexcitation steps whose timescales are separated.
A theoretical model is introduced for constructing the vibrational Hamiltonian of Hydrogen-like atoms (HLA). The Hamiltonian is then used to derive the vibrational motion equations of HLA in Heisenberg picture. The Langevin equation will ultimately be formed after adding the dissipative term and fluctuating (Langevin) force according to the fluctuation-dissipation theorem (FDT). The positional noise flux is then defined as the correlation function of fluctuations that happens for the electron position during its rather fast vibrational oscillations ( ). On the other hand, the positional fluctu…
Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence
Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡大学）；Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière（里昂第一大学）
We observe experimentally the spontaneous formation of star-shaped surface patterns in driven Bose-Einstein condensates. Two-dimensional star-shaped patterns with $l$-fold symmetry, ranging from quadrupole ($l=2$) to heptagon modes ($l=7$), are parametrically excited by modulating the scattering length near the Feshbach resonance. An effective Mathieu equation and Floquet analysis are utilized, relating the instability conditions to the dispersion of the surface modes in a trapped superfluid. Identifying the resonant frequencies of the patterns, we precisely measure the dispersion relation of …
Time-resolved Raman spectroscopy techniques offer various ways to study the dynamics of molecular vibrations in liquids or gases and optical phonons in crystals. While these techniques give access to the coherence time of the vibrational modes, they are not able to reveal the fragile quantum correlations that are spontaneously created between light and vibration during the Raman interaction. Here, we present a scheme leveraging universal properties of spontaneous Raman scattering to demonstrate Bell correlations between light and a collective molecular vibration. We measure the decay of these …
The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses [Levin et al., arXiv:1411.1542]. The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective…
A new physical implementation for quantum computation is proposed. The vibrational modes of molecules are used to encode qubit systems. Global quantum logic gates are realized using shaped femtosecond laser pulses which are calculated applying optimal control theory. The scaling of the system is favourable, sources for decoherence can be eliminated. A complete set of one and two quantum gates is presented for a specific molecule. Detailed analysis regarding experimental realization shows that the structural resolution of today's pulse shapers is easiliy sufficient for pulse formation.
Decoherence is studied in an attractive proposal for an actual implementation of a quantum computer based on trapped ions. Emphasis is placed on the decoherence arising from the vibrational motion of the ions, which is compared with that due to spontaneous emission from excited states of the ions. The calculation is made tractable by exploiting the vast difference in time scales between the vibrational excitations and the intra-ionic electronic excitations. Since the latter are several orders of magnitude faster, an adiabatic approximation is used to integrate them out and find the inclusive p…
Starting from an ultracold sample of ground-state $^{23}$Na$^{87}$Rb molecules, we investigate the lowest ro-vibrational level of the $b^3Π$ state with high resolution laser spectroscopy. This electronic spin-forbidden $X^1Σ^+ \leftrightarrow b^3Π$ transition features a nearly diagonal Franck-Condon factor and has been proposed useful for probing and manipulating the ultracold molecular gas. We measure the transition strength directly by probing the ac Stark shift induced by near resonance light and determine the total excited-state spontaneous emission rate by observing the loss of molecules.…
Spontaneous Raman emission in atomic gases provides an attractive source of photon pairs with a controllable delay. We show how this technique can be implemented in solid state systems by appropriately shaping the inhomogeneous broadening. Our proposal is eminently feasible with current technology and provides a realistic solution to entangle remote rare-earth doped solids in a heralded way.
Spontaneous synchronisation is a collective phenomenon that can occur in both dynamical classical and quantum systems. Here, we analyse the spontaneous synchronisation dynamics of vibrations assisting energy transfer in a bio-inspired system. We find the emergence of a constant non-zero `synchronisation phase' between synchronised vibrational displacements as the natural frequencies of the oscillators are detuned. This phase difference arises from the asymmetric participation of local modes in the long-lived synchronised state. Furthermore, we investigate the relationships between the synchron…
We demonstrate the conversion of cold Cs_{2} molecules initially distributed over several vibrational levels of the lowest triplet state a^{3}Σ_{u}^{+} into the singlet ground state X^{1}Σ_{g}^{+}. This conversion is realized by a broadband laser exciting the molecules to a well-chosen state from which they may decay to the singlet state throug\textcolor{black}{h two sequential single-photon emission steps: Th}e first photon populates levels with mixed triplet-singlet character, making possible a second spontaneous emission down to several vibrational levels of the X^{1}Σ_{g}^{+} states. By ad…
We show the emergence of spontaneous synchronization between a pair of detuned quantum oscillators within a harmonic network. Our model does not involve any nonlinearity, driving, or external dissipation, thus providing the simplest scenario for the occurrence of local coherent dynamics in an extended harmonic system. A sufficient condition for synchronization is established by building upon the Rayleigh normal mode approach to vibrational systems. Our results show that mechanisms favoring synchronization, even between oscillators that are not directly coupled to each other, are transient ener…
In molecular photodissociation, some specific combinations of laser parameters (wavelength and intensity) lead to unexpected Zero-Width Resonances (ZWR), with in principle infinite lifetimes. Their interest in inducing basic quenching mechanisms have recently been devised in the laser control of vibrational cooling through filtration strategies [O. Atabek et al., Phys. Rev. A87, 031403(R) (2013)]. A full quantum adiabatic control theory based on the adiabatic Floquet Hamiltonian is developed to show how a laser pulse could be envelop-shaped and frequency-chirped so as to protect a given initia…
We study the dynamics of neutral cold atoms in an $L$-shaped crossed-beam optical waveguide formed by two perpendicular red-detuned lasers of different intensities and a blue-detuned laser at the corner. Complemented with a vibrational cooling process this setting works as a one-way device or "atom diode".
We demonstrate the ability to control the spontaneous emission from a superconducting qubit coupled to a cavity. The time domain profile of the emitted photon is shaped into a symmetric truncated exponential. The experiment is enabled by a qubit coupled to a cavity, with a coupling strength that can be tuned in tens of nanoseconds while maintaining a constant dressed state emission frequency. Symmetrization of the photonic wave packet will enable use of photons as flying qubits for transfering the quantum state between atoms in distant cavities.
An optical cycling center (OCC) is a recently coined term to indicate two electronic states within a complex quantum object that can repeatedly experience optical laser excitation and spontaneous decay, while being well isolated from its environment. Here we present a quantitative understanding of electronic, vibrational, and rotational excitations of the polyatomic SrOH molecule, which possesses a localized OCC near its Sr atom. In particular, we describe the vibrationally-dependent trends in the Franck-Condon factors of the bending and stretching modes of the molecular electronic states coup…
Acoustic spontaneous emission into bulk dielectrics can be a strong source of decoherence in quantum devices, especially when a qubit is in the presence of piezoelectric materials. We study the dynamics of a qubit coupled to an acoustic resonator by a piezoelectric film. By varying the surface topography of the resonator from rough to polished to shaped, we explore the crossover from fast decay of an excited qubit to quantum-coherent coupling between the qubit and an isolated phonon mode. Our experimental approach may be used for precision measurements of crystalline vibrations, the design of …
We study the quantum dynamics of an ultracold atomic gas in a deep optical lattice within an optical high-$Q$ resonator. The atoms are coherently illuminated with the cavity resonance tuned to a blue vibrational sideband, so that photon scattering to the resonator mode is accompanied by vibrational cooling of the atoms. This system exhibits a threshold above which pairwise stimulated generation of a cavity photon and an atom in the lowest vibrational band dominates spontaneous scattering and we find a combination of optical lasing with a buildup of a macroscopic population in the lowest lattic…
The equations of motion for the molecular rotation are derived for vibrationally cold dimers that are polarized by off-resonant laser light. It is shown that, by eliminating electronic and vibrational degrees of freedom, a quantum master equation for the reduced rotational density operator can be obtained. The coherent rotational dynamics is caused by stimulated Raman transitions, whereas spontaneous Raman transitions lead to decoherence in the motion of the quantized angular momentum. As an example the molecular dynamics for the optical Kerr effect is chosen, revealing decoherence and heating…
A pulse shaping algorithm for a matter wave with the purpose of controlling a binary reaction has been designed. The scheme is illustrated for an Eley-Rideal reaction where an impinging matter-wave atom recombines with an adsorbed atom on a metal surface. The wave function of the impinging atom is shaped such that the desorbing molecule leaves the surface in a specific vibrational state.
The idea about a quantum nature of Planck's blackbody radiation law is deeply rooted in minds of most physicists. Einstein's work, in which the coefficients of spontaneous and induced emission were introduced, has always been regarded as a proof that quantum energy discreteness of an atom plays a crucial role in the derivation of this law. In our paper we avoid this standpoint. It may be shown that the de Broglie wave assigned to every material particle is a result of interaction of the particle with zero-point vibrations of electromagnetic ground field. The energetic spectrum of a harmonic os…
In a semiconductor-based double quantum well (QW) coupled to a degree of freedom with an internal dynamics, we demonstrate that the electronic motion is controllable within femtoseconds by applying appropriately shaped electromagnetic pulses. In particular, we consider a pulse-driven AlxGa1-xAs based symmetric double QW coupled to uniformly distributed or localized vibrational modes and present analytical results for the lowest two levels. These predictions are assessed and generalized by full-fledged numerical simulations showing that localization and time-stabilization of the driven electron…
