Understanding Collisions of Ultracold Polar Molecules

Lead Research Organisation: Durham University
Department Name: Physics

Abstract

At temperatures about a millionth of a degree above absolute zero, atoms and molecules enter a new regime where all their motions are governed by the laws of quantum mechanics. Over the last 20 years, there has been a renaissance in atomic physics based on the new phenomena that emerge in this regime. Experiments with atomic Bose-Einstein condensates (recognised by the 2001 Nobel Prize in Physics) have explored a wide range of topics including nonlinear atom optics, quantum vortices, and phase-transitions in optical lattices. At the same time, degenerate Fermi gases have been used, for example, to improve our understanding of Fermionic superfluidity and the physics of polarons. At the heart of all these advances is a deep and detailed understanding of ultracold atomic collisions that has developed over the last two decades through the close interplay of theory and experiment.

Attention in this field is now turning to the new possibilities offered by ultracold molecules. Unlike atoms, molecules can possess an electric dipole moment, with one end positively charged and the other negatively charged. These dipoles mean that molecules can interact with one another more strongly than atoms, and crucially at longer range. Molecules also have more complicated internal structure than atoms: they have multiple spinning nuclei, and they can rotate and be oriented by external fields. Because of this, ultracold molecules offer many new possibilities for the study of novel physical phenomena and the development of new quantum technologies. Examples include the study of exotic forms of quantum magnetism and the potential to design new material properties using so-called "quantum simulators" based on arrays of molecules confined in optical lattices.

We have recently become only the third group in the world to succeed in forming a sample of ultracold polar molecules. In our case, this was done by cooling gases of rubidium and cesium atoms to ultracold temperatures, and then pairing up the atoms to form molecules. The molecules we formed were initially nonpolar and only very weakly bound, but we succeeded in transferring them to deeply bound, polar states using a two-photon optical transfer process, known as stimulated Raman adiabatic passage (STIRAP). The entire process occurs without heating, so that the temperature of the resulting molecular gas mirrors that of the atomic mixture.

Before our molecules can be used in new quantum devices, we need to understand a lot more about their interactions and collisions. A key question, which does not arise for atoms, is whether pairs of molecules "stick together" for a long time when they collide. If they do, then a third molecule may come along and destroy the first two, shortening the lifetime of the molecular sample. The objective of this project is to investigate collisions of ultracold molecules, both experimentally and theoretically, in order to understand the processes involved. We will investigate both 2-body and 3-body collisions, and distinguish between them by loading our molecules into optical lattices formed by standing waves of laser light. These can confine the molecules in stacks of flat pancakes, bundles of tubes, or even individual boxes.

Even if molecular collisions are "sticky", we expect to be able to find ways to control them and thereby preserve the molecular sample for sufficient time to perform interesting experiments. We will investigate orienting the confined molecules with applied electric fields and dressing them with microwave photons, allowing us to create forces that will hold the molecules apart and prevent collisions.

This ambitious project, combining state-of-the-art experiments with world-leading theory, will cement the UK's position at the forefront of an exciting international field.

Planned Impact

The research outlined in this proposal will have an impact on society and the economy in a number of ways, in both short and long terms:

1. Supply of highly trained personnel.
Modern high-tech industry requires personnel with strong technical backgrounds and highly developed problem-solving skills. Through this proposal two PDRAs will acquire expertise in a range of state-of-the-art experimental and theoretical techniques in quantum science. Additionally, we have an exceptionally strong track record of training postgraduates and undergraduates within the Joint Quantum Centre and we will endeavour to involve students in the project wherever possible. All personnel connected with the project will gain professional and transferable skills that are highly sought after in the current job market (e.g. project and time management, communication and presentation skills). The skills they acquire are needed in many sectors, including education, defence, R&D, technology and finance.

2. The development of high-tech equipment.
This proposal will drive the development of high-tech equipment with potential benefits to UK companies in areas such as photonics and lasers. Our research often requires us to develop new techniques or devices which can lead to commercial exploitation. For example, in the past we have developed a simple resonant electro-optic modulator which is now commercially available from Photonic Technologies, a small UK based company. Similarly, working closely with manufacturers, our research can drive the improvement of existing products and the development of new product lines.

3. Presentation of our research to the wider community.
The general public will benefit from our efforts to communicate our research in simple terms. This helps to ensure that the public is engaged with science and recognises its enormous importance in the economy and society. In addition to public lectures, laboratory tours and outreach activities, we will add videos and non-technical synopses of our research publications to our Web pages. Further societal impacts will be realised through our extensive international links.

4. Knowledge generation.
In the short term our proposal will yield a better fundamental understanding of the collisions of ultracold molecules, and we will learn how to maintain samples of molecules so that they are not destroyed by inelastic collisions. This will underpin nearly all future uses of ultracold molecules in quantum science and technology. Ultimately the realisation of a quantum simulator using polar molecules has the potential to contribute to our understanding of a range of problems in condensed matter physics (e.g. quantum magnetism and strongly correlated many-body systems). As such, our research will ultimately be relevant to two of the current Physics Grand Challenges: "Emergence and Physics Far From Equilibrium" and "Quantum Physics for New Quantum Technologies". Our efforts will contribute to the competitiveness of science research in the UK, which in turn will help attract highly skilled personnel, funding and even companies into the UK economy. It will probably take more than a decade for the knowledge generated in our research to spread beyond the academic community and on this time-scale it is hard to assess the full impact. Nevertheless we can expect potential impacts in the areas of quantum metrology, precision measurement and quantum technology. Indeed, this research will contribute to maintaining the strong base of world-leading quantum science in the UK which is vital to the development of future applications of quantum technology.
 
Description Experiments with non-reactive ultracold molecules have all observed rapid loss in an optical trap, even though it was believed that there should be no mechanism for loss if the molecules are prepared in their absolute ground state. Through this award we have identified and explained the mechanism of this loss in the case of RbCs molecules, greatly advancing the understanding of collisions between ultracold molecules. We have shown that when two molecules collide they form a long-lived collision complex (the collisions are referred to as "sticky" as a consequence). We have developed new experimental techniques to probe the collision complex. Using these techniques, we have shown that the collision complex is rapidly excited by the laser light to an electronically excited state that then decays leading to the observed loss. As part of our work, we were able to measure the lifetime of the collision complex, providing a benchmark for theoretical calculations. We have also investigated atom-molecule collisions in both the reactive and non-reactive regimes. Again, we observe loss consistent with the existence of sticky collisions.
Additionally, we have used microwave spectroscopy to understand the structure of the molecular energy levels in the presence of electric and magnetic fields. This has allowed us to engineer long-lived coherent superpositions of hyperfine states suitable for use as robust storage qubits for quantum information. Theoretically we have examined the use of microwave fields to shield molecular conditions, establishing the requirements for effective shielding in experiments, and have developed a proposal for implementing a quantum gate between molecules using microwave fields. Finally, we have predicted a magic-wavelength trap for the lowest rotational states of RbCs molecules that will allow long-rotational coherences in future experiments, opening up new possibilities for the study of quantum magnetism using ultracold molecules.
Exploitation Route Our findings are informing other experimentalists working in this field, several of whom have adopted our methodology for probing the nature of the loss. By understanding the loss, the research community is able to devise methods to suppress or eliminate the problem.
Sectors Other

 
Description The methodology we developed to study molecular collision complexes and the impact of light-induced loss has been adopted by many experimental groups around the world, leading to a more complete picture of the nature of ultracold molecular collisions. Many groups are now pursuing methods to shield lossy collisions and this has resulted in the first quantum degenerate gases of molecules.
First Year Of Impact 2022
Sector Other
Impact Types Societal

 
Title An association sequence suitable for producing ground-state RbCs molecules in optical lattices 
Description The data that support the findings of this study are uploaded here. All the data files are self-explanatory. They contain individual column names.  The experimental data for Fig. 4(a) are in Fig4a_experimental_data.csv under the folders Fig_4>Fig_4a. To convert to binding energy there is a fitting algorithm in the Python code Feshbach_Fit.py . 
Type Of Material Database/Collection of data 
Year Produced 2023 
Provided To Others? Yes  
URL https://zenodo.org/doi/10.5281/zenodo.7777261
 
Title Diatomic-py: A Python module for calculating the rotational and hyperfine structure of 1S molecules 
Description We present a computer program to calculate the quantised rotational and hyperfine energy levels of 1S diatomic molecules in the presence of dc electric, dc magnetic, and off-resonant optical fields. Our program is applicable to the bialkali molecules used in ongoing state-of-the-art experiments with ultracold molecular gases. We include functions for the calculation of space-fixed electric dipole moments, magnetic moments and transition dipole moments. 
Type Of Material Database/Collection of data 
Year Produced 2022 
Provided To Others? Yes  
URL https://data.mendeley.com/datasets/3yfxnh5bn5/1
 
Title Diatomic-py: A Python module for calculating the rotational and hyperfine structure of 1S molecules 
Description We present a computer program to calculate the quantised rotational and hyperfine energy levels of 1S diatomic molecules in the presence of dc electric, dc magnetic, and off-resonant optical fields. Our program is applicable to the bialkali molecules used in ongoing state-of-the-art experiments with ultracold molecular gases. We include functions for the calculation of space-fixed electric dipole moments, magnetic moments and transition dipole moments. 
Type Of Material Database/Collection of data 
Year Produced 2022 
Provided To Others? Yes  
URL https://data.mendeley.com/datasets/3yfxnh5bn5
 
Title MOLSCAT, BOUND and FIELD 
Description This dataset provides files for the packages MOLSCAT, BOUND and FIELD, which are referenced in the following CPC 50th Anniversary articles: MOLSCAT: A program for non-reactive quantum scattering calculations on atomic and molecular collisions - https://doi.org/10.1016/j.cpc.2019.02.014 BOUND and FIELD: Programs for calculating bound states of interacting pairs of atoms and molecules - https://doi.org/10.1016/j.cpc.2019.02.017 This dataset contains:- 1) Full documentation for the programs MOLSCAT, BOUND and FIELD in pdf form; 2) A directory source_code containing a) the Fortran source code; b) a GNUmakefile that can build the executables needed for the example calculations described in the documentation; c) a sub-directory input containing input files for the example calculations described in the documentation; d) a sub-directory output containing the corresponding output files; 4) A directory data containing auxiliary data files for some potential routines used in the example calculations; 5) A plain-text file README that gives information on changes that may be needed to adapt the GNUmakefile to a specific target computer. 
Type Of Material Database/Collection of data 
Year Produced 2019 
Provided To Others? Yes  
URL https://data.mendeley.com/datasets/rtzgf5mwpn/1
 
Title MOLSCAT, BOUND and FIELD 
Description This dataset provides files for the packages MOLSCAT, BOUND and FIELD, which are referenced in the following CPC 50th Anniversary articles: MOLSCAT: A program for non-reactive quantum scattering calculations on atomic and molecular collisions - https://doi.org/10.1016/j.cpc.2019.02.014 BOUND and FIELD: Programs for calculating bound states of interacting pairs of atoms and molecules - https://doi.org/10.1016/j.cpc.2019.02.017 This dataset contains:- 1) Full documentation for the programs MOLSCAT, BOUND and FIELD in pdf form; 2) A directory source_code containing a) the Fortran source code; b) a GNUmakefile that can build the executables needed for the example calculations described in the documentation; c) a sub-directory input containing input files for the example calculations described in the documentation; d) a sub-directory output containing the corresponding output files; 4) A directory data containing auxiliary data files for some potential routines used in the example calculations; 5) A plain-text file README that gives information on changes that may be needed to adapt the GNUmakefile to a specific target computer. 
Type Of Material Database/Collection of data 
Year Produced 2019 
Provided To Others? Yes  
URL https://data.mendeley.com/datasets/rtzgf5mwpn