We consider ultracold polar molecules trapped in a unit-filled one-dimensional chain in real space created with an optical lattice or a tweezer array and illuminated by microwaves that resonantly drive transitions within a chain of rotational states. We describe the system by a two-dimensional lattice model, with the first dimension being a lattice in real space and the second dimension being a lattice in a synthetic direction composed of rotational states. We calculate this system's ground-state phase diagram. We show that as the dipole interaction strength is increased, the molecules undergo a phase transition from a two-dimensional gas to a phase in which the molecules bind together and form a string that resembles a one-dimensional object living in the two-dimensional (i.e., one real and one synthetic dimensional) space. We demonstrate this with two complementary techniques: numerical calculations using matrix product state techniques and an analytic solution in the limit of infinitely strong dipole interaction. Our calculations reveal that the string phase at infinite interaction is effectively described by emergent particles living on the string and that this leads to a rich spectrum with excitations missed in earlier mean-field treatments.
We consider ultracold polar molecules trapped in a unit-filled one-dimensional chain in real space created with an optical lattice or a tweezer array and illuminated by microwaves that resonantly drive transitions within a chain of rotational states. We describe the system by a two-dimensional lattice model, with the first dimension being a lattice in real space and the second dimension being a lattice in a synthetic direction composed of rotational states. We calculate this system's ground-state phase diagram. We show that as the dipole interaction strength is increased, the molecules undergo a phase transition from a two-dimensional gas to a phase in which the molecules bind together and form a string that resembles a one-dimensional object living in the two-dimensional (i.e., one real and one synthetic dimensional) space. We demonstrate this with two complementary techniques: numerical calculations using matrix product state techniques and an analytic solution in the limit of infinitely strong dipole interaction. Our calculations reveal that the string phase at infinite interaction is effectively described by emergent particles living on the string and that this leads to a rich spectrum with excitations missed in earlier mean-field treatments.
Synthetic dimensions alter one of the most fundamental properties in nature, the dimension of space. They allow, for example, a real three-dimensional system to act as effectively four-dimensional. Driven by such possibilities, synthetic dimensions have been engineered in ongoing experiments with ultracold matter. We show that rotational states of ultracold molecules can be used as synthetic dimensions extending to many - potentially hundreds of - synthetic lattice sites. Microwaves coupling rotational states drive fully controllable synthetic inter-site tunnelings, enabling, for example, topological band structures. Interactions leads to even richer behavior: when molecules are frozen in a real space lattice with uniform synthetic tunnelings, dipole interactions cause the molecules to aggregate to a narrow strip in the synthetic direction beyond a critical interaction strength, resulting in a quantum string or a membrane, with an emergent condensate that lives on this string or membrane. All these phases can be detected using local measurements of rotational state populations.
Engineering synthetic dimensions, where the physics of additional spatial dimensions is simulated within the internal states of a quantum system, allows the realisation of phenomena not otherwise accessible in experiments. Ultracold ground-state polar molecules are an ideal platform to encode synthetic dimensions, offering access to large Hilbert spaces of long-lived internal states associated with the rotational and hyperfine degrees of freedom, that can be coupled together with microwave fields to simulate tunnelling. Here, to benchmark the advantages of ultracold molecules, we encode a 1D synthetic lattice in the rotational states of ultracold RbCs molecules and use it to investigate the well-known Su-Schrieffer-Heeger (SSH) model, a minimal model displaying topological properties. To probe the system, we perform spectroscopy using an auxiliary rotational state and study the time dynamics after deterministic state preparation. We demonstrate long coherence times, typically ~500 times the lattice tunnelling period, even for a synthetic lattice using 8 rotational states. Observations of dynamics at long times with full site-resolved readout of the synthetic dimension allow us to test the effects of chiral and non-chiral perturbations on the topologically protected edge states. Our work lays the foundation for further quantum simulations using the rich internal structure of molecules, including dipolar string phases in interacting samples of molecules, and adiabatic state preparation of many-body Hamiltonians.
Synthetic-dimension platforms offer unique pathways for engineering quantum matter. We compute the phase diagram of a many-body system of ultracold atoms (or polar molecules) with a set of Rydberg states (or rotational states) as a synthetic dimension, where the particles are arranged in real space in optical microtrap arrays and interact via dipole-dipole exchange interaction. Using mean-field theory, we find three ordered phases---two are localized in the synthetic dimension, predicted as zero-temperature ground states by Sundar et al. [Sci. Rep. 8, 3422 (2018); Phys. Rev. A 99, 013624 (2019)], and one is a delocalized phase. We characterize them by identifying the spontaneously broken discrete symmetries of the Hamiltonian. We also compute the phase diagram as a function of temperature and interaction strength for both signs of the interaction. For system sizes with more than six synthetic sites and attractive interactions, we find that the thermal phase transitions can be first or second order, which leads to a tricritical point on the phase boundary. By examining the dependence of the tricritical point and other special points of the phase boundary on the synthetic dimension size, we shed light on the physics for thermodynamically large synthetic dimension.
We calculate properties of dipolar interacting ultracold molecules or Rydberg atoms in a semisynthetic three-dimensional configuration---one synthetic dimension plus a two-dimensional real-space optical lattice or periodic microtrap array---using the stochastic Green's function quantum Monte Carlo method. Through a calculation of thermodynamic quantities and appropriate correlation functions, along with their finite-size scalings, we show that there is a second-order transition to a low-temperature phase in which two-dimensional ``sheets'' form in the synthetic dimension of internal rotational or electronic states of the molecules or Rydberg atoms, respectively. Simulations for different values of the interaction V, which acts between atoms or molecules that are adjacent both in real and synthetic space, allow us to compute a phase diagram. We find a finite-temperature transition at sufficiently large V as well as a quantum phase transition---a critical value Vc below which the transition temperature vanishes.
Strongly interacting ultracold dipolar molecules are a rich platform for quantum information and quantum simulation of phenomena relevant to condensed matter systems. This dissertation presents novel theoretical and computational studies of ultracold dipolar molecules relevant to these areas in three broad categories.First, the path integral ground state quantum Monte Carlo method is extended to simulations with both translational and rotational degrees of freedom, including the development of a novel estimator of the elementary excitation energies of a system with these degrees of freedom based on the well known Feynman-Bijl approximation. This is then used to study dipolar molecular ensembles confined to one-dimensional optical lattices. The ground state phase diagram is characterized with both a mean-field method and the aforementioned quantum Monte Carlo method. A quantum phase transition is found for very short optical lattice spacings or very large dipole moments. The prospects for experimentally realizing a system which exhibits this phase transition are discussed.Second, the path integral ground state quantum Monte Carlo method is utilized to study the ground state of dipole molecules confined to two-dimensional optical lattices. On square lattices a crossover from a weakly interacting disordered phase to a strongly interacting striped phase is found for short lattice spacings or large dipole moments. On triangular lattices a crossover between a disordered phase and a completely polarized phase is found, also for short lattice spacings or large dipole moments. The relevance of such simulations to self-assembled dipolar crystals in two dimensions is discussed and simulation results of these systems are presented. Simulations of polarized and harmonically confined molecular systems in two dimensions with translations and rotations are also presented and a realistic interaction potential using highly accurate ab initio quantum chemistry techniques is calculated for LiH--LiH interactions as a preliminary step toward developing a high quality trial wave function for the simulation of systems possessing both translational and rotational degrees of freedom.Finally, several novel applications for dipolar molecules confined to optical lattices are proposed. An experimental realization of a topological phase using 2Sigma ground state molecules with applied near resonant microwave fields and transverse magnetic fields is proposed. A method to create an array of dipole-coupled two-level molecules exhibiting superradiance and possessing novel spectroscopic properties using 1Sigma ground state molecules in the combination of a far off-resonant laser field and a moderate magnetic field is proposed. Additionally, a method to create entangled pairs of molecules using closed-shell dipolar molecules immersed in an intense far off-resonant laser field is reviewed and an extension in which parallel optical lattices are merged and molecules are allowed to collide in the presence of a far off-resonant laser field is proposed. Simulation results are presented indicating that a significant amount of entanglement may be generated in such a way in realistic molecular systems.
The creation of a gas of ultracold polar molecules with a high phase space density brings new possibilities beyond experiments with ultracold atomic gases. In particular, long-range, anisotropic, and tunable dipole-dipole interactions open the way for novel quantum gases, with applications including strongly correlated many-body systems, and ultracold chemistry. This thesis will present the final steps to complete control over both internal and external degrees of freedom of the molecule which allows us to control, and even completely suppress, the chemical reactions between molecules. First, the control over internal states has been achieved through coherent state transfer to the ro-vibronic ground state and coherent manipulations of the hyperfine and rotational states with microwave radiation. Second, external degrees of freedom are controlled by loading the gas into an optical lattice. With the molecules loaded into a one-dimensional lattice, the orientation of the molecular collisions is controlled by manipulating both internal (hyperfine states) and external (motional states in the direction of tight confinement) degrees of freedom. Most striking is that by preparing the molecules all in the lowest band of the lattice in the same internal state, the molecular collisions can only occur in a side-by-side" orientation, where the chemical reaction rate is suppressed by the repulsive dipole-dipole interactions. The chemical reaction can be suppressed completely by further constraining the motion in the trap in a strong 3D lattice. Here we see lifetimes longer than 20 s, limited by o-resonant light scattering. Finally, the ac polarizability of the molecules is explored and controlled. The different rotational states of the molecule have different polarizabilities and will experience a different trapping force in both the optical dipole trap or lattice. We show that there is a magic angle" between the quantization axis and the polarization of the trapping laser at which the polarizabilities of two different rotational states can be matched, eliminating dephasing and allowing for coherent manipulations between rotational states.