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Register a new userControlling the quantum stereodynamics of ultracold bimolecular reactions
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Chemical reaction rates often depend strongly on stereodynamics, namely the orientation and movement of molecules in three-dimensional space. An ultracold molecular gas, with a temperature below 1 uK, provides a highly unusual regime for chemistry, where polar molecules can easily be oriented using an external electric field and where, moreover, the motion of two colliding molecules is strictly quantized. Recently, atom-exchange reactions were observed in a trapped ultracold gas of KRb molecules. In an external electric field, these exothermic and barrierless bimolecular reactions, KRb+KRb -> K2+Rb2, occur at a rate that rises steeply with increasing dipole moment. Here we show that the quantum stereodynamics of the ultracold collisions can be exploited to suppress the bimolecular chemical reaction rate by nearly two orders of magnitude. We use an optical lattice trap to confine the fermionic polar molecules in a quasi-two-dimensional, pancake-like geometry, with the dipoles oriented along the tight confinement direction. With the combination of sufficiently tight confinement and Fermi statistics of the molecules, two polar molecules can approach each other only in a side-by-side collision, where the chemical reaction rate is suppressed by the repulsive dipole-dipole interaction. We show that the suppression of the bimolecular reaction rate requires quantum-state control of both the internal and external degrees of freedom of the molecules. The suppression of chemical reactions for polar molecules in a quasi-two-dimensional trap opens the way for investigation of a dipolar molecular quantum gas. Because of the strong, long-range character of the dipole-dipole interactions, such a gas brings fundamentally new abilities to quantum-gas-based studies of strongly correlated many-body physics, where quantum phase transitions and new states of matter can emerge.
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Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. Here we take the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest ro-vibronic quantum state at ultralow temperatures, thereby drastically reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium molecules at a temperature of 500~nK, we directly observe reactants, intermediates, and products of the reaction $^{40}$K$^{87}$Rb + $^{40}$K$^{87}$Rb $rightarrow$ K$_2$Rb$^*_2$ $rightarrow$ K$_2$ + Rb$_2$. Beyond observation of a long-lived energy-rich intermediate complex, this technique opens the door to further studies of quantum-state resolved reaction dynamics in the ultracold regime.
We investigate theoretically the suppression of two-body losses when the on-site loss rate is larger than all other energy scales in a lattice. This work quantitatively explains the recently observed suppression of chemical reactions between two rotational states of fermionic KRb molecules confined in one-dimensional tubes with a weak lattice along the tubes [Yan et al., Nature 501, 521-525 (2013)]. New loss rate measurements performed for different lattice parameters but under controlled initial conditions allow us to show that the loss suppression is a consequence of the combined effects of lattice confinement and the continuous quantum Zeno effect. A key finding, relevant for generic strongly reactive systems, is that while a single-band theory can qualitatively describe the data, a quantitative analysis must include multiband effects. Accounting for these effects reduces the inferred molecule filling fraction by a factor of five. A rate equation can describe much of the data, but to properly reproduce the loss dynamics with a fixed filling fraction for all lattice parameters we develop a mean-field model and benchmark it with numerically exact time-dependent density matrix renormalization group calculations.
Controlling non-equilibrium quantum dynamics in many-body systems is an outstanding challenge as interactions typically lead to thermalization and a chaotic spreading throughout Hilbert space. We experimentally investigate non-equilibrium dynamics following rapid quenches in a many-body system composed of 3 to 200 strongly interacting qubits in one and two spatial dimensions. Using a programmable quantum simulator based on Rydberg atom arrays, we probe coherent revivals corresponding to quantum many-body scars. Remarkably, we discover that scar revivals can be stabilized by periodic driving, which generates a robust subharmonic response akin to discrete time-crystalline order. We map Hilbert space dynamics, geometry dependence, phase diagrams, and system-size dependence of this emergent phenomenon, demonstrating novel ways to steer entanglement dynamics in many-body systems and enabling potential applications in quantum information science.
How does a chemical reaction proceed at ultralow temperatures? Can simple quantum mechanical rules such as quantum statistics, single scattering partial waves, and quantum threshold laws provide a clear understanding for the molecular reactivity under a vanishing collision energy? Starting with an optically trapped near quantum degenerate gas of polar $^{40}$K$^{87}$Rb molecules prepared in their absolute ground state, we report experimental evidence for exothermic atom-exchange chemical reactions. When these fermionic molecules are prepared in a single quantum state at a temperature of a few hundreds of nanoKelvins, we observe p-wave-dominated quantum threshold collisions arising from tunneling through an angular momentum barrier followed by a near-unity probability short-range chemical reaction. When these molecules are prepared in two different internal states or when molecules and atoms are brought together, the reaction rates are enhanced by a factor of 10 to 100 due to s-wave scattering, which does not have a centrifugal barrier. The measured rates agree with predicted universal loss rates related to the two-body van der Waals length.
We introduce a model to study the collisions of two ultracold diatomic molecules in one dimension interacting via pairwise potentials. We present results for this system, and argue that it offers lessons for real molecular collisions in three dimensions. We analyze the distribution of the adiabatic potentials in the hyperspherical coordinate representation as well as the distribution of the four-body bound states in the adiabatic approximation (i.e. no coupling between adiabatic channels). It is found that while the adiabatic potential distribution transitions from chaotic to non-chaotic as the two molecules are separated, the four-body bound states show no visible chaos in the distribution of nearest-neighbor energy level spacing. We also study the effects of molecular properties, such as interaction strength, interaction range, and atomic mass, on the resonance density and degree of chaos in the adiabatic potentials. We numerically find that the dependence of the four-body bound state density on these parameters is captured by simple scaling laws, in agreement with previous analytic arguments, even though these arguments relied on uncontrolled approximations. This agreement suggests that similar scaling laws may also govern real molecular collisions in three dimensions.
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