arXiv subjects

D. DeMille

Publications and source records attributed to D. DeMille.

At least 37 records · Page 2Linked to original sources

arXiv2013

Search for the electron electric dipole moment using $Ω$-doublet levels in PbO$^*$

We present results of the first experiment to probe for the electric dipole moment (EDM) of the electron using an $Ω$-doublet state in a polar molecule. If the molecule is both massive and has a large molecular-fixed frame dipole moment, then the $Ω$-doublet states have the potential to greatly increase the sensitivity of experiments searching for the EDM while also allowing for new methods of systematic error rejection. Here, we use the metastable $a(1)^3Σ^+$ state of lead monoxide (PbO) to probe for the electron EDM. Our best fit for the electron EDM of $d_e = (-4.4\pm9.5_\text{stat}\pm1.8_\text{syst})\times10^{-27}\ecm$ allows us to place an upper limit on the magnitude of the EDM of $|d_e|<1.7\times10^{-26}\ecm$ (90% confidence). While this is less stringent than limits from other, previous experiments, our work emphasizes the systematic error rejection properties associated with the $Ω$-doublet level structure. The results should inform the work of other, ongoing experiments that use molecules with analogous level structure.

physics.atom-ph↗

arXiv2011

Laser radiation pressure slowing of a molecular beam

There is substantial interest in producing samples of ultracold molecules for possible applications in quantum computation, quantum simulation of condensed matter systems, precision measurements, controlled chemistry, and high precision spectroscopy. A crucial step to obtaining large samples of ultracold, trapped molecules is developing a means to bridge the gap between typical molecular source velocities (~150-600 m/s) and velocities for which trap loading or confinement is possible (~5-20 m/s). Here we show deceleration of a beam of neutral strontium monofluoride (SrF) molecules using radiative force. Under certain conditions, the deceleration results in a substantial flux of molecules with velocities <50 m/s. The observed slowing, from ~140 m/s, corresponds to scattering ~10000 photons. We also observe longitudinal velocity compression under different conditions. Combined with molecular laser cooling techniques, this lays the groundwork to create slow and cold molecular beams suitable for trap loading.

physics.atom-ph↗

arXiv2011

On the Prospects for Laser Cooling of TlF

We measure the upper state lifetime and two ratios of vibrational branching fractions f_{v'v} on the B^{3}Π_{1}(v') - X^{1}Σ^{+}(v) transition of TlF. We find the B state lifetime to be 99(9) ns. We also determine that the off-diagonal vibrational decays are highly suppressed: f_{01}/f_{00} < 2x10^{-4} and f_{02}/f_{00} = 1.10(6)%, in excellent agreement with their predicted values of f_{01}/f_{00} < 8x10^{-4} and f_{02}/f_{00} = 1.0(2)% based on Franck-Condon factors calculated using Morse and RKR potentials. The implications of these results for the possible laser cooling of TlF and fundamental symmetries experiments are discussed.

physics.atom-ph↗

arXiv2011

Laser cooling of a diatomic molecule

It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for many applications. For example, heteronuclear molecules possess permanent electric dipole moments which lead to long-range, tunable, anisotropic dipole-dipole interactions. The combination of the dipole-dipole interaction and the precise control over molecular degrees of freedom possible at ultracold temperatures make ultracold molecules attractive candidates for use in quantum simulation of condensed matter systems and quantum computation. Also ultracold molecules may provide unique opportunities for studying chemical dynamics and for tests of fundamental symmetries. Here we experimentally demonstrate laser cooling of the molecule strontium monofluoride (SrF). Using an optical cycling scheme requiring only three lasers, we have observed both Sisyphus and Doppler cooling forces which have substantially reduced the transverse temperature of a SrF molecular beam. Currently the only technique for producing ultracold molecules is by binding together ultracold alkali atoms through Feshbach resonance or photoassociation. By contrast, different proposed applications for ultracold molecules require a variety of molecular energy-level structures. Our method provides a new route to ultracold temperatures for molecules. In particular it bridges the gap between ultracold temperatures and the ~1 K temperatures attainable with directly cooled molecules (e.g. cryogenic buffer gas cooling or decelerated supersonic beams). Ultimately our technique should enable the production of large samples of molecules at ultracold temperatures for species that are chemically distinct from bialkalis.

physics.atom-ph↗

arXiv2011

A Bright, Slow Cryogenic Molecular Beam Source for Free Radicals

We demonstrate and characterize a cryogenic buffer gas-cooled molecular beam source capable of producing bright beams of free radicals and refractory species. Details of the beam properties (brightness, forward velocity distribution, transverse velocity spread, rotational and vibrational temperatures) are measured under varying conditions for the molecular species SrF. Under typical conditions we produce a beam of brightness 1.2 x 10^11 molecules/sr/pulse in the rovibrational ground state, with 140 m/s forward velocity and a rotational temperature of approximately 1 K. This source compares favorably to other methods for producing beams of free radicals and refractory species for many types of experiments. We provide details of construction that may be helpful for others attempting to use this method.

physics.atom-ph↗

arXiv2010

Progress towards fabrication of Th:229-doped high energy band-gap crystals for use as a solid-state optical frequency reference

We have recently described a novel method for the construction of a solid-state optical frequency reference based on doping $^{229}$Th into high energy band-gap crystals. Since nuclear transitions are far less sensitive to environmental conditions than atomic transitions, we have argued that the $^{229}$Th optical nuclear transition may be driven inside a host crystal resulting in an optical frequency reference with a short-term stability of $3\times10^{-17}<Δf/f <1\times10^{-15}$ at 1 s and a systematic-limited repeatability of $Δf/f \sim 2 \times 10^{-16}$. Improvement by $10^2-10^3$ of the constraints on the variability of several important fundamental constants also appears possible. Here we present the results of the first phase of these experiments. Specifically, we have evaluated several high energy band-gap crystals (Th:NaYF, Th:YLF, Th:LiCAF, Na$_2$ThF$_6$, LiSAF) for their suitability as a crystal host by a combination of electron beam microprobe measurements, Rutherford Backscattering, and synchrotron excitation/fluorescence measurements. These measurements have shown LiCAF to be the most promising host crystal, and using a $^{232}$Th doped LiCAF crystal, we have performed a mock run of the actual experiment that will be used to search for the isomeric transition in $^{229}$Th. This data indicates that a measurement of the transition energy with a signal to noise ratio (SNR) greater than 30:1 can be achieved at the lowest expected fluorescence rate.

physics.atom-ph↗

arXiv2010

Cavity QED in a molecular ion trap

We propose an approach for studying quantum information and performing high resolution spectroscopy of rotational states of trapped molecular ions using an on-chip superconducting microwave resonator. Molecular ions have several advantages over neutral molecules. Ions can be loaded into deep (1 eV) RF traps and are trapped independent of the electric dipole moment of their rotational transition. Their charge protects them from motional dephasing and prevents collisional loss, allowing 1 s coherence times when used as a quantum memory, with detection of single molecules possible in <10 ms. An analysis of the detection efficiency and coherence properties of the molecules is presented.

cond-mat.mes-hall↗

arXiv2010

Optical transition of the $^{229}$Th nucleus in a solid-state environment

We describe a novel approach to directly measure the energy of the narrow, low-lying isomeric state in $^{229}$Th. Since nuclear transitions are far less sensitive to environmental conditions than atomic transitions, we argue that the $^{229}$Th optical nuclear transition may be driven inside a host crystal with a high transition Q. This technique might also allow for the construction of a solid-state optical frequency reference that surpasses the precision of current optical clocks, as well as improved limits on the variability of fundamental constants. Based on analysis of the crystal lattice environment, we argue that a precision of $3\times10^{-17}<Δf/f <1\times10^{-15}$ after 1 s of photon collection may be achieved with a systematic-limited accuracy of $Δf/f \sim 2 \times 10^{-16}$. Improvement by $10^2-10^3$ of the constraints on the variability of several important fundamental constants also appears possible.

physics.atom-ph↗

arXiv2009

Radiative force from optical cycling on a diatomic molecule

We demonstrate a scheme for optical cycling in the polar, diatomic molecule strontium monofluoride (SrF) using the $X ^2Σ^+\toA^2Π_{1/2}$ electronic transition. SrF's highly diagonal Franck-Condon factors suppress vibrational branching. We eliminate rotational branching by employing a quasi-cycling $N=1\to N^\prime=0$ type transition in conjunction with magnetic field remixing of dark Zeeman sublevels. We observe cycling fluorescence and deflection through radiative force of an SrF molecular beam using this scheme. With straightforward improvements our scheme promises to allow more than $10^5$ photon scatters, possibly enabling the direct laser cooling of SrF.

physics.atom-ph↗

arXiv2008

Preparation and detection of states with simultaneous spin alignment and molecular orientation in PbO

We are pursuing an experiment to measure the electric dipole moment of the electron using the molecule PbO. This measurement requires the ability to prepare quantum states with orientation of the molecular axis and, simultaneously, alignment of the electron spin perpendicular to this axis. It also requires efficient detection of the evolution of the spin alignment direction within such a state. We describe a series of experiments that have achieved these goals, and the features and limitations of the techniques. We also discuss possible new approaches for improved efficiency in this and similar systems.

physics.atom-ph↗

arXiv2007

An Easily Constructed, Tuning Free, Ultra-broadband Probe for NMR

We have developed an easy to construct, non-resonant wideband NMR probe. The probe is of the saddle coil geometry and is designed such that the coil itself forms a transmission line. The probe thus requires no tuning or matching elements. We use the probe with a spectrometer whose duplexer circuitry employs a simple RF switch instead of the more common lambda/4 lines, so the entire probe and spectrometer perform in an essentially frequency-independent manner. Despite being designed with electro- and magnetostatic formulas, the probe performs well at frequencies up to 150 MHz and beyond. We expect that with additional design effort, the probe could be modified for use at significantly higher frequencies. Because our construction method relies on commercial circuit fabrication techniques, identical probes can be easily and accurately produced.

physics.ins-det↗

arXiv2007

Enhanced sensitivity to variation of $m_{e}/m_{p}$ in molecular spectra

We propose new experiments with high sensitivity to a possible spatial or temporal variation of the electron-to-proton mass ratio $μ\equiv m_e/m_p$. We consider a nearly-degenerate pair of molecular vibrational levels, where each state is associated with a different electronic potential. The change in the splitting between such levels, with respect to a change in $μ$, can be large both on an absolute scale and relative to the splitting. We demonstrate the existence of such pairs of levels in Cs$_2$. The narrow spectral lines achievable with ultracold Cs$_2$ in these long-lived levels make this system promising for future searches for small variations in $μ$.

physics.atom-ph↗

arXiv2007

Using Molecules to Measure Nuclear Spin-Dependent Parity Violation

Nuclear spin-dependent parity violation arises from weak interactions between electrons and nucleons, and from nuclear anapole moments. We outline a method to measure such effects, using a Stark-interference technique to determine the mixing between opposite-parity rotational/hyperfine levels of ground-state molecules. The technique is applicable to nuclei over a wide range of atomic number, in diatomic species that are theoretically tractable for interpretation. This should provide data on anapole moments of many nuclei, and on previously unmeasured neutral weak couplings.

physics.atom-ph↗

arXiv2006

Polar molecules near superconducting resonators: a coherent, all-electrical, molecule-mesoscopic interface

The challenge of building a scalable quantum processor requires consolidation of the conflicting requirements of achieving coherent control and preservation of quantum coherence in a large scale quantum system. Moreover, the system should be compatible with miniaturization and integration of quantum circuits. Mesoscopic solid state systems such as superconducting islands and quantum dots feature robust control techniques using local electrical signals and self-evident scaling based on advances in fabrication; however, in general the quantum states of solid state devices tend to decohere rapidly. In contrast, quantum optical systems based on trapped ions and neutral atoms exhibit dramatically better coherence properties, while miniaturization of atomic and molecular systems, and their integration with mesoscopic electrical circuits, remains an important challenge. Below we describe methods for the integration of a single particle system -- an isolated polar molecule -- with mesoscopic solid state devices in a way that produces robust, coherent, quantum-level control. The methods described include the trapping, cooling, detection, coherent manipulation and quantum coupling of isolated polar molecules at sub-micron dimensions near cryogenic stripline microwave resonators. We show that electrostatically trapped polar molecules can exhibit strong confinement and fast, purely electrical gate control. Furthermore, the effect of electrical noise sources, a key issue in quantum information processing, can be suppressed to very low levels via appropriate preparation and manipulation of the polar molecules. Our setup provides a scalable cavity QED-type quantum computer architecture, where entanglement of distant qubits stored in long-lived rotational molecular states is achieved via exchange of microwave photons.

quant-ph↗

arXiv2006

Hybrid Quantum Processors: molecular ensembles as quantum memory for solid state circuits

We investigate a hybrid quantum circuit where ensembles of cold polar molecules serve as long-lived quantum memories and optical interfaces for solid state quantum processors. The quantum memory realized by collective spin states (ensemble qubit) is coupled to a high-Q stripline cavity via microwave Raman processes. We show that for convenient trap-surface distances of a few $μ$m, strong coupling between the cavity and ensemble qubit can be achieved. We discuss basic quantum information protocols, including a swap from the cavity photon bus to the molecular quantum memory, and a deterministic two qubit gate. Finally, we investigate coherence properties of molecular ensemble quantum bits.

quant-ph↗

arXiv2005

Large-Area, Low-Noise, High Speed, Photodiode-Based Fluorescence Detectors with Fast Overdrive Recovery

Two large-area, low noise, high speed fluorescence detectors have been built. One detector consists of a photodiode with an area of 28 mm x 28 mm and a low noise transimpedance amplifier. This detector has a input light-equivalent spectral noise density of less than 3 pW/Hz^1/2, can recover from a large scattered light pulse within 10 us, and has a bandwidth of at least 900 kHz. The second detector consists of a 16 mm diameter avalanche photodiode and a low-noise transimpedance amplifier. This detector has an input light-equivalent spectral noise density of 0.08 pW/Hz^1/2, also can recover from a large scattered light pulse within 10 us, and has a bandwidth of 1 MHz.

physics.atom-ph↗

arXiv2005

Stark-modulation spectroscopy of the B(1)$[^3Π]$ state of PbO

We report detailed spectroscopic measurements of the X(0)$[^3Σ^+]$(v=0) to B(1)$[^3Π]$ (v=5) transition in PbO. Using a Stark-modulated laser absorption technique, we have measured the hyperfine constant of $^{207}$PbO in the B(1) state, as well as B(1)(v=5) rotational constant, X-B isotope shifts, etc. The hyperfine structure of the B(1) state is of interest as a benchmark for calculations of PbO electronic structure, related to experiments to search for the electric dipole moment of the electron.

physics.atom-ph↗

arXiv2005

High-flux beam source for cold, slow atoms or molecules

We demonstrate and characterize a high-flux beam source for cold, slow atoms or molecules. The desired species is vaporized using laser ablation, then cooled by thermalization in a cryogenic cell of buffer gas. The beam is formed by particles exiting a hole in the buffer gas cell. We characterize the properties of the beam (flux, forward velocity, temperature) for both an atom (Na) and a molecule (PbO) under varying buffer gas density, and discuss conditions for optimizing these beam parameters. Our source compares favorably to existing techniques of beam formation, for a variety of applications.

physics.atom-ph↗