The optical scattering force, behind Doppler cooling and magneto-optical trapping, may be amplified without incurring additional spontaneous emission by the state-dependent coherent deflection produced by a pulsed or chirped laser field. At some cost in experimental complexity, amplified forces allow efficient cooling on narrow transitions and permit the compact deceleration of beams with reduced transverse heating, and will be of interest for molecules and atoms with open level schemes where losses following spontaneous emission would otherwise prevail. We present a general analysis of the amplification scheme, and propose an optimized, dynamic cooling scheme that allows the temperature of a sample to be reduced by around a factor of two per excited state lifetime.
The optical scattering force, behind Doppler cooling and magneto-optical trapping, may be amplified without incurring additional spontaneous emission by the state-dependent coherent deflection produced by a pulsed or chirped laser field. At some cost in experimental complexity, amplified forces allow efficient cooling on narrow transitions and permit the compact deceleration of beams with reduced transverse heating, and will be of interest for molecules and atoms with open level schemes where losses following spontaneous emission would otherwise prevail. We present a general analysis of the amplification scheme, and propose an optimized, dynamic cooling scheme that allows the temperature of a sample to be reduced by around a factor of two per excited state lifetime.
Laser cooling and trapping are central to modern atomic physics. It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields and a number of Nobel prizes. Prior to the work presented in this thesis, laser cooling had not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. The first direct laser cooling of a molecule and further results we present here provide a new route to ultracold temperatures for molecules. In particular, these methods bridge the gap between ultracold temperatures and the approximately 1 kelvin temperatures attainable with directly cooled molecules (e.g. with cryogenic buffer gas cooling or decelerated supersonic beams). Using the carefully chosen molecule strontium monofluoride (SrF), decays to unwanted vibrational states are suppressed. Driving a transition with rotational quantum number R=1 to an excited state with R'=0 eliminates decays to unwanted rotational states. The dark ground-state Zeeman sublevels present in this specific scheme are remixed via a static magnetic field. Using three lasers for this scheme, a given molecule should undergo an average of approximately 100,000 photon absorption/emission cycles before being lost via unwanted decays. This number of cycles should be sufficient to load a magneto-optical trap (MOT) of molecules. In this thesis, we demonstrate transverse cooling of an SrF beam, in both Doppler and a Sisyphus-type cooling regimes. We also realize longitudinal slowing of an SrF beam. Finally, we detail current progress towards trapping SrF in a MOT. Ultimately, this technique should enable the production of large samples of molecules at ultracold temperatures for molecules chemically distinct from competing methods.
This Letter reports the demonstration of laser cooling without spontaneous emission, and thereby addresses a significant controversy. It works by restricting the atom-light interaction to a time short compared to a cycle of absorption followed by natural decay. It is achieved by using the bichromatic force on an atomic transition with a relatively long excited state lifetime and a relatively short cooling time so that spontaneous emission effects are minimized. The observed width of the one-dimensional velocity distribution is reduced by ×2 thereby reducing the "temperature" by ×4. Moreover, our results comprise a compression in phase space because the spatial expansion of the atomic sample is limited. This accomplishment is of interest to direct laser cooling of molecules or in experiments where working space or time is limited.
From studies of fundamental physics to quantum technologies the production of ultracold molecules will have a huge impact across a range of applications. For many years laser cooling, which became an invaluable tool in cold atomic physics, was deemed to be too impractical for application to molecules. Nevertheless, laser cooling has now been demonstrated for a few molecular species. Using a frequency-chirped laser slowing technique, the velocity distribution of a pulse of CaF molecules is compressed and slowed from 180 m/s to about 10 m/s. These slow molecules are then captured in a magneto-optical trap. I present measurements that show how the number of molecules, the photon scattering rate, the oscillation frequency, damping constant, temperature, cloud size and lifetime depend on the key parameters of the magneto-optical trap, especially the intensity and detuning of the main cooling laser. The trap contains up to 2*10^4 molecules, the maximum photon scattering rate is 2.5*10^6 s-1 per molecule, the maximum oscillation frequency is 100 Hz, the maximum damping constant is 500 s^-1, and the minimum rms radius of the trapped cloud is 1.5 mm. A minimum temperature of 730 microkelvin is obtained by ramping down the laser intensity to lower values. To reach lower temperatures, the cloud is loaded into a blue-detuned optical molasses, which cools the molecules to 55 microkelvin, well below the Doppler-limiting temperature. I characterise the cooling process and suggest the sub-Doppler mechanisms responsible. These ultracold molecules are the optically pumped into a single quantum state, and coherently transferred between selected hyperfine components of the ground and first-excited rotational states. Finally, the ultracold, state-selected molecules are loaded into a magnetic trap that has a lifetime of about 1 s.
The bichromatic force allows laser cooling using stimulated processes only. We provide details of our simulations of the bichromatic force when the effects of spontaneous emission are suppressed by restricting the atom-light interaction time to be short enough that there cannot be a significant number of spontaneous emission events. This short interaction time requires that the simulation include dynamics of the atomic motion through the light field that is coupled to the internal state dynamics that determine the force on the atom. The simulation is first tested with several standard optical field configurations to confirm its accuracy. Then the results, using conditions that match our experiment, are presented and compared with our measurements. The simulation shows that the resolution of the experiment greatly obscures the degree of cooling. Our simulation predicts an observed velocity distribution reduced by up to a factor of 4 in width over a time comparable to the excited state lifetime. This technique can allow the direct laser cooling of atoms and molecules without closed cycling transitions.
The dipole force, which avoids the closed cycle of pumping and spontaneous emission that renders laser cooling unsuitable for molecules, is conservative: without dissipation, particles entering a trap retain the energy to escape. Fortunately, dissipation need not involve spontaneous emission if it instead results from the decoherence or decay of the optical trapping field that is coupled to the particle. To enhance the weak attraction of an atom to its reflection, cavity-mediated cooling recycles light through multiple reflections, amplifying the force and the retardation - a process related to the mechanical amplification in a near confocal cavity [5]. Resonant cavities and structures can increase the retardation, but not the intensity, even when the atoms or particles lie outside them - e.g. when the cavity is the narrow-band coating of a single mirror. Plasmon resonances of a structured metal can enhance both the delay and the optical intensity. Such processes, possible with arrays of micromirrors, resemble speckle field cooling [6], except that spontaneous emission is again replaced by decay of the optical field, and offer a new class of cooling mechanisms in which weak cooling is extended over a broad array, rather than concentrated at the centre of a single external cavity.
In the last several years we have discovered a variety of remarkable pulse strategies for manipulating molecular motion by employing a design strategy we call “local optimization.'' Here we review the concept of local optimization and contrast it with optimal control theory. By way of background, we give highlights from two recent examples of the method: (1) a strategy for eliminating population transfer to one or many excited electronic states during strong field excitation, an effect we call ‘optical paralysis’; (2) a generalization of the counterintuitive STIRAP (stimulated Raman adiabatic passage) pulse sequence from three levels to N levels, a strategy we call ‘straddling STIRAP.' We then turn to a third example, which is the main subject of this paper: laser cooling of molecular internal degrees of freedom. We study a model that includes both coherent interaction with the radiation field and spontaneous emission; the latter is necessary to carry away the entropy from the molecule. An optimal control calculation was performed first and succeeded in producing vibrational cooling, but the resulting pulse sequence was difficult to interpret. Local optimization subsequently revealed the cooling mechanism: the instantaneous phase of the laser is locked to the phase of the transition dipole moment between the excited state amplitude and v=0 of the ground state. Thus, the molecules that reach v=0 by spontaneous emission become decoupled from the field, and no longer absorb, while molecules in all other states are continually repumped. The mechanism could be called “vibrationally selective coherent population trapping,'' in analogy to the corresponding mechanism of velocity selective coherent population trapping in atoms for sub-Doppler cooling of translations.