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Register a new userMeasurement of excited-state transitions in cold calcium atoms by direct femtosecond frequency-comb spectroscopy
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We apply direct frequency-comb spectroscopy, in combination with precision cw spectroscopy, to measure the ${rm 4s4p} ^3P_1 to {rm 4s5s} ^3S_1$ transition frequency in cold calcium atoms. A 657 nm ultrastable cw laser was used to excite atoms on the narrow ($gamma sim 400$ Hz) ${rm 4s^2} ^1S_0 to {rm 4s4p} ^3P_1$ clock transition, and the direct output of the frequency comb was used to excite those atoms from the ${rm 4s4p} ^3P_1$ state to the ${rm 4s5s} ^3S_1$ state. The resonance of this second stage was detected by observing a decrease in population of the ground state as a result of atoms being optically pumped to the metastable ${rm 4s4p} ^3P_{0,2}$ states. The ${rm 4s4p} ^3P_1 to {rm 4s5s} ^3S_1$ transition frequency is measured to be $ u = 489 544 285 713(56)$ kHz; which is an improvement by almost four orders of magnitude over the previously measured value. In addition, we demonstrate spectroscopy on magnetically trapped atoms in the ${rm 4s4p} ^3P_2$ state.
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Direct frequency comb spectroscopy of trapped ions is demonstated for the first time. It is shown that the 4s^2S_(1/2)-4p^2P_(3/2) transition in calcium ions can be excited directly with a frequency comb laser that is upconverted to 393 nm. Detection of the transition is performed using a shelving scheme to suppress background signal from non-resonant comb modes. The measured transition frequency of f=761 905 012.7(0.5) MHz presents an improvement in accuracy of more than two orders of magnitude.
We analyze several possibilities for precisely measuring electronic transitions in atomic helium by the direct use of phase-stabilized femtosecond frequency combs. Because the comb is self-calibrating and can be shifted into the ultraviolet spectral region via harmonic generation, it offers the prospect of greatly improved accuracy for UV and far-UV transitions. To take advantage of this accuracy an ultracold helium sample is needed. For measurements of the triplet spectrum a magneto-optical trap (MOT) can be used to cool and trap metastable 2^3S state atoms. We analyze schemes for measuring the two-photon $2^3S to 4^3S$ interval, and for resonant two-photon excitation to high Rydberg states, $2^3S to 3^3P to n^3S,D$. We also analyze experiments on the singlet-state spectrum. To accomplish this we propose schemes for producing and trapping ultracold helium in the 1^1S or 2^1S state via intercombination transitions. A particularly intriguing scenario is the possibility of measuring the $1^1S to 2^1S$ transition with extremely high accuracy by use of two-photon excitation in a magic wavelength trap that operates identically for both states. We predict a ``triple magic wavelength at 412 nm that could facilitate numerous experiments on trapped helium atoms, because here the polarizabilities of the 1^1S, 2^1S and 2^3S states are all similar, small, and positive.
Microresonator-based soliton frequency combs - microcombs - have recently emerged to offer low-noise, photonic-chip sources for optical measurements. Owing to nonlinear-optical physics, microcombs can be built with various materials and tuned or stabilized with a consistent framework. Some applications require phase stabilization, including optical-frequency synthesis and measurements, optical-frequency division, and optical clocks. Partially stabilized microcombs can also benefit applications, such as oscillators, ranging, dual-comb spectroscopy, wavelength calibration, and optical communications. Broad optical bandwidth, brightness, coherence, and frequency stability have made frequency-comb sources important for studying comb-matter interactions with atoms and molecules. Here, we explore direct microcomb atomic spectroscopy, utilizing a cascaded, two-photon 1529-nm atomic transition of rubidium. Both the microcomb and the atomic vapor are implemented with planar fabrication techniques to support integration. By fine and simultaneous control of the repetition rate and carrier-envelope-offset frequency of the soliton microcomb, we obtain direct sub-Doppler and hyperfine spectroscopy of the $4^2D_{5/2}$ manifold. Moreover, the entire set of microcomb modes are stabilized to this atomic transition, yielding absolute optical-frequency fluctuations of the microcomb at the kilohertz-level over a few seconds and < 1 MHz day-to-day accuracy. Our work demonstrates atomic spectroscopy with microcombs and provides a rubidium-stabilized microcomb laser source, operating across the 1550 nm band for sensing, dimensional metrology, and communication.
Continuous wave (CW) lasers are the enabling technology for producing ultracold atoms and molecules through laser cooling and trapping. The resulting pristine samples of slow moving particles are the de facto starting point for both fundamental and applied science when a highly-controlled quantum system is required. Laser cooled atoms have recently led to major advances in quantum information, the search to understand dark energy, quantum chemistry, and quantum sensors. However, CW laser technology currently limits laser cooling and trapping to special types of elements that do not include highly abundant and chemically relevant atoms such as hydrogen, carbon, oxygen, and nitrogen. Here, we demonstrate that Doppler cooling and trapping by optical frequency combs may provide a route to trapped, ultracold atoms whose spectra are not amenable to CW lasers. We laser cool a gas of atoms by driving a two-photon transition with an optical frequency comb, an efficient process to which every comb tooth coherently contributes. We extend this technique to create a magneto-optical trap (MOT), an electromagnetic beaker for accumulating the laser-cooled atoms for further study. Our results suggest that the efficient frequency conversion offered by optical frequency combs could provide a key ingredient for producing trapped, ultracold samples of natures most abundant building blocks, as well as antihydrogen. As such, the techniques demonstrated here may enable advances in fields as disparate as molecular biology and the search for physics beyond the standard model.
Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is generally restricted to ground state properties. Working in resonance conditions, indeed, enables cross-section enhancement and selective excitation to a targeted electronic level, but is hampered by an increased signal complexity due to the presence of overlapping spectral contributions. Here, we show how detailed information on ground and excited state vibrations can be disentangled, by exploiting the relative time delay between Raman and probe pulses to control the excited state population, combined with a diagrammatic formalism to dissect the pathways concurring to the signal generation. The proposed method is then exploited to elucidate the vibrational properties of ground and excited electronic states in the paradigmatic case of Cresyl Violet. We anticipate that the presented approach holds the potential for selective mapping the reaction coordinates pertaining to transient electronic stages implied in photo-active compounds.
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