arXiv subjects

Martin Zeppenfeld

Publications and source records attributed to Martin Zeppenfeld.

18 recordsLinked to original sources

arXiv2024

Coherence of Symmetry-Protected Rotational Qubits in Cold Polyatomic Molecules

Polar polyatomic molecules provide an ideal but largely unexplored platform to encode qubits in rotational states. Here, we trap cold (100-600 mK) formaldehyde (H$_2$CO) inside an electric box and perform a Ramsey-type experiment to observe long-lived (~100 $\mu$s) coherences between symmetry-protected molecular states with opposite rotation but identical orientation, representing a quasi-hidden molecular degree of freedom. As a result, the observed qubit is insensitive to the magnitude of an external electric field, and depends only weakly on magnetic fields. Our findings provide a basis for future quantum and precision experiments with trapped cold molecules.

physics.atom-ph↗

arXiv2023

A robust framework for quantum computation using quasi-hidden molecular degrees of freedom

We discuss a novel approach to quantum information processing with molecules based on molecular degrees of freedom which are isolated from the environment as well as from the rest of the molecule. Such a degree of freedom can provide long-term quantum storage even in a noisy environment, and provides an independent protected quantum memory while quantum operations are performed between the rest of the molecule and external systems. We present several possibilities for realizing a quasi-hidden degree of freedom in a molecule, and discuss a number of examples for using such a degree of freedom in practice. Using quasi-hidden degrees of freedom could substantially improve the prospects for a molecule-based quantum computer.

physics.atom-ph↗

arXiv2022

Rydberg atom-enabled spectroscopy of polar molecules via F\"orster resonance energy transfer

Non-radiative energy transfer between a Rydberg atom and a polar molecule can be controlled by a DC electric field. Here we show how to exploit this control for state-resolved, non-destructive detection and spectroscopy of the molecules where the lineshape reflects the type of molecular transition. Using the example of ammonia, we identify the conditions for collision-mediated spectroscopy in terms of the required electric field strengths, relative velocities, and molecular densities. Rydberg atom-enabled spectroscopy is feasible with current experimental technology, providing a versatile detection method as basic building block for applications of polar molecules in quantum technologies and chemical reaction studies.

physics.atom-ph↗

arXiv2021

High-resolution 'magic'-field spectroscopy on trapped polyatomic molecules

Rapid progress in cooling and trapping of molecules has enabled first experiments on high resolution spectroscopy of trapped diatomic molecules, promising unprecedented precision. Extending this work to polyatomic molecules provides unique opportunities due to more complex geometries and additional internal degrees of freedom. Here, this is achieved by combining a homogeneous-field microstructured electric trap, rotational transitions with minimal Stark broadening at a 'magic' offset electric field, and optoelectrical Sisyphus cooling of molecules to the low millikelvin temperature regime. We thereby reduce Stark broadening on the $J=5\leftarrow4$ ($K=3$) transition of formaldehyde at $364\,$GHz to well below $1\,$kHz, observe Doppler-limited linewidths down to $3.8\,$kHz, and determine the 'magic'-field line position with an uncertainty below $100\,$Hz. Our approach opens a multitude of possibilities for investigating diverse polyatomic molecule species.

physics.atom-ph↗

arXiv2020

Buffer-gas cooling of molecules in the low-density regime: Comparison between simulation and experiment

Cryogenic buffer gas cells have been a workhorse for the cooling of molecules in the last decades. The straightforward sympathetic cooling principle makes them applicable to a huge variety of different species. Notwithstanding this success, detailed simulations of buffer gas cells are rare, and have never been compared to experimental data in the regime of low to intermediate buffer gas densities. Here, we present a numerical approach based on a trajectory analysis, with molecules performing a random walk in the cell due to collisions with a homogeneous buffer gas. This method can reproduce experimental flux and velocity distributions of molecules emerging from the buffer gas cell for varying buffer gas densities. This includes the strong decrease in molecule output from the cell for increasing buffer gas density and the so-called boosting effect, when molecules are accelerated by buffer-gas atoms after leaving the cell. The simulations provide various insights which could substantially improve buffer-gas cell design.

physics.chem-ph↗

arXiv2018

High-resolution spectroscopy on cold electrically trapped formaldehyde

We present precision spectroscopy on electrically trapped formaldehyde (H$_2$CO), demonstrating key attributes which will enable molecular spectroscopy with unprecedented precision. Our method makes use of a microstructured electric trap with homogeneous fields in the trap center and rotational transitions with minimal Stark broadening at a 'magic' offset electric field. Using molecules cooled to the low millikelvin temperature regime via optoelectrical Sisyphus cooling, we reduce Stark broadening on the $J=5\leftarrow4$ ($K=3$) transition at 364 GHz to well below 1 kHz, observe Doppler-limited linewidths down to 3.8 kHz, and determine the line position with sub-kHz uncertainty. Our results and clear prospects for even narrower spectra pave the way towards in-trap precision spectroscopy on diverse molecule species.

physics.atom-ph↗

arXiv2017

A cryofuge for cold-collision experiments with slow polar molecules

Ultracold molecules represent a fascinating research frontier in physics and chemistry, but it has proven challenging to prepare dense samples at low velocities. Here we present a solution to this goal by a non-conventional approach dubbed cryofuge. It employs centrifugal force to bring cryogenically cooled molecules to kinetic energies below $1\,$K$\times k_B$ in the laboratory frame, with corresponding fluxes exceeding $10^{10}$/s at velocities below $20\,$m/s. By attaining densities higher than $10^9$/cm$^3$ and interaction times longer than $25\,$ms in samples of fluoromethane as well as deuterated ammonia, we observe cold dipolar collisions between molecules and determine their collision cross sections.

physics.atom-ph↗

arXiv2017

Fast, precise, and widely tunable frequency control of an optical parametric oscillator referenced to a frequency comb

Optical frequency combs (OFC) provide a convenient reference for the frequency stabilization of continuous-wave lasers. We demonstrate a frequency control method relying on tracking over a wide range and stabilizing the beat note between the laser and the OFC. The approach combines fast frequency ramps on a millisecond timescale in the entire mode-hop free tuning range of the laser and precise stabilization to single frequencies. We apply it to a commercially available optical parametric oscillator (OPO) and demonstrate tuning over more than 60 GHz with a ramping speed up to 3 GHz/ms. Frequency ramps spanning 15 GHz are performed in less than 10 ms, with the OPO instantly relocked to the OFC after the ramp at any desired frequency. The developed control hardware and software is able to stabilize the OPO to sub-MHz precision and to perform sequences of fast frequency ramps automatically.

physics.ins-det↗

arXiv2016

Nondestructive Detection of Polar Molecules via Rydberg Atoms

A highly sensitive, general, and preferably nondestructive technique to detect polar molecules would greatly advance a number of fields, in particular quantum science with cold and ultracold molecules. Here, we propose using resonant energy transfer between molecules and Rydberg atoms to detect molecules. Based on an energy transfer cross section of $>10^{-6}\,$cm$^2$ for sufficiently low collision energies, a near unit efficiency non-destructive detection of basically any polar molecule species in a well defined internal state should be possible.

physics.atom-ph↗

arXiv2016

Optoelectrical cooling of polar molecules to sub-millikelvin temperatures

We demonstrate direct cooling of gaseous formaldehyde (H2CO) to the microkelvin regime. Our approach, optoelectrical Sisyphus cooling, provides a simple dissipative cooling method applicable to electrically trapped dipolar molecules. By reducing the temperature by three orders of magnitude and increasing the phase-space density by a factor of ~$10^4$ we generate an ensemble of $3\cdot10^5$ molecules with a temperature of about 420μK, populating a single rotational state with more than 80% purity.

physics.atom-ph↗

arXiv2015

Rotational cooling of trapped polyatomic molecules

Controlling the internal degrees of freedom is a key challenge for applications of cold and ultracold molecules. Here, we demonstrate rotational-state cooling of trapped methyl fluoride molecules (CH3F) by optically pumping the population of 16 M-sublevels in the rotational states J=3,4,5, and 6 into a single level. By combining rotational-state cooling with motional cooling, we increase the relative number of molecules in the state J=4, K=3, M=4 from a few percent to over 70%, thereby generating a translationally cold (~30mK) and nearly pure state ensemble of about 10^6 molecules. Our scheme is extendable to larger sets of initial states, other final states and a variety of molecule species, thus paving the way for internal-state control of ever larger molecules.

physics.atom-ph↗

arXiv2014

Rotational state detection of electrically trapped polyatomic molecules

Detecting the internal state of polar molecules is a substantial challenge when standard techniques such as resonance-enhanced multi photon ionization (REMPI) or laser-induced fluorescense (LIF) do not work. As this is the case for most polyatomic molecule species, we here investigate an alternative based on state selective removal of molecules from an electrically trapped ensemble. Specifically, we deplete molecules by driving rotational and/or vibrational transitions to untrapped states. Fully resolving the rotational state with this method can be a considerable challenge as the frequency differences between various transitions is easily substantially less than the Stark broadening in an electric trap. However, making use of a unique trap design providing homogeneous fields in a large fraction of the trap volume, we successfully discriminate all rotational quantum numbers, including the rotational M-substate.

physics.atom-ph↗

arXiv2010

Velocity-selected molecular pulses produced by an electric guide

Electrostatic velocity filtering is a technique for the production of continuous guided beams of slow polar molecules from a thermal gas. We extended this technique to produce pulses of slow molecules with a narrow velocity distribution around a tunable velocity. The pulses are generated by sequentially switching the voltages on adjacent segments of an electric quadrupole guide synchronously with the molecules propagating at the desired velocity. This technique is demonstrated for deuterated ammonia (ND$_{3}$), delivering pulses with a velocity in the range of $20-100\,\rm{m/s}$ and a relative velocity spread of $(16\pm 2)\,%$ at FWHM. At velocities around $60\,\rm{m/s}$, the pulses contain up to $10^6$ molecules each. The data are well reproduced by Monte-Carlo simulations, which provide useful insight into the mechanisms of velocity selection.

physics.chem-ph↗

arXiv2010

Cavity-Enhanced Rayleigh Scattering

We demonstrate Purcell-like enhancement of Rayleigh scattering into a single optical mode of a Fabry-Perot resonator for several thermal atomic and molecular gases. The light is detuned by more than an octave, in this case by hundreds of nanometers, from any optical transition, making particle excitation and spontaneous emission negligible. The enhancement of light scattering into the resonator is explained quantitatively as an interference effect of light waves emitted by a classical driven dipole oscillator. Applications of our method include the sensitive, non-destructive in-situ detection of ultracold molecules.

quant-ph↗

arXiv2010

Calculating the Fine Structure of a Fabry-Perot Resonator using Spheroidal Wave Functions

A new set of vector solutions to Maxwell's equations based on solutions to the wave equation in spheroidal coordinates allows laser beams to be described beyond the paraxial approximation. Using these solutions allows us to calculate the complete first-order corrections in the short-wavelength limit to eigenmodes and eigenfrequencies in a Fabry-Perot resonator with perfectly conducting mirrors. Experimentally relevant effects are predicted. Modes which are degenerate according to the paraxial approximation are split according to their total angular momentum. This includes a splitting due to coupling between orbital angular momentum and spin angular momentum.

physics.optics↗

arXiv2009

Solutions to Maxwell's Equations using Spheroidal Coordinates

Analytical solutions to the wave equation in spheroidal coordinates in the short wavelength limit are considered. The asymptotic solutions for the radial function are significantly simplified, allowing scalar spheroidal wave functions to be defined in a form which is directly reminiscent of the Laguerre-Gaussian solutions to the paraxial wave equation in optics. Expressions for the Cartesian derivatives of the scalar spheroidal wave functions are derived, leading to a new set of vector solutions to Maxwell's equations. The results are an ideal starting point for calculations of corrections to the paraxial approximation.

physics.optics↗

arXiv2008

Collisional effects in the formation of cold guided beams of polar molecules

High fluxes of cold polar molecules are efficiently produced by electric guiding and velocity filtering. Here, we investigate different aspects of the beam formation. Variations of the source parameters such as density and temperature result in characteristic changes in the guided beam. These are observed in the velocity distribution of the guided molecules as well as in the dependence of the signal of guided molecules on the trapping electric field. A model taking into account velocity-dependent collisional losses of cold molecules in the region close to the nozzle accurately reproduces this behavior. This clarifies an open question on the parameter dependence of the detected signal and gives a more detailed understanding of the velocity filtering and guiding process.

physics.chem-ph↗

arXiv2008

Spectroscopy of formaldehyde in the 30140-30790cm^-1 range

Room-temperature absorption spectroscopy of formaldehyde has been performed in the 30140-30790cm^-1 range. Using tunable ultraviolet continuous-wave laser light, individual rotational lines are well resolved in the Doppler-broadened spectrum. Making use of genetic algorithms, the main features of the spectrum are reproduced. Spectral data is made available as Supporting Information.

physics.chem-ph↗