Near-ultraviolet photon-counting dual-comb spectroscopy.

Ultraviolet spectroscopy provides unique insights into the structure of matter with applications ranging from fundamental tests to photochemistry in the Earth's atmosphere and astronomical observations from space telescopes1-8. At longer wavelengths, dual-comb spectroscopy, using two interfering laser frequency combs, has become a powerful technique capable of simultaneously providing a broad spectral range and very high resolution9. Here we demonstrate a photon-counting approach that can extend the unique advantages of this method into ultraviolet regions where nonlinear frequency conversion tends to be very inefficient. Our spectrometer, based on two frequency combs with slightly different repetition frequencies, provides a wide-span, high-resolution frequency calibration within the accuracy of an atomic clock, and overall consistency of the spectra. We demonstrate a signal-to-noise ratio at the quantum limit and an optimal use of the measurement time, provided by the multiplexed recording of all spectral data on a single photon-counter10. Our initial experiments are performed in the near-ultraviolet and in the visible spectral ranges with alkali-atom vapour, with a power per comb line as low as a femtowatt. This crucial step towards precision broadband spectroscopy at short wavelengths paves the way for extreme-ultraviolet dual-comb spectroscopy, and, more generally, opens up a new realm of applications for photon-level diagnostics, as encountered, for example, when driving single atoms or molecules.

Improved active fiber-based retroreflector with intensity stabilization and a polarization monitor for the near UV: erratum.

In Sec. 6 (polarization monitor) of our recent publication [Opt. Express29(5), 7024 (2021)10.1364/OE.417455], we assumed a small value of δ. This is however incorrect. The correct approximation for small ß leads to the updated Eqs. (10)-(11), resulting in a corrected Fig. 12.

Time-resolved dual-comb spectroscopy with a single electro-optic modulator.

Time-resolved near-infrared absorption spectroscopy of single non-repeatable transient events is performed at high spectral resolution with a dual-comb interferometer using a continuous-wave laser followed by a single electro-optic amplitude modulator. By sharing high-speed electrical/optical components, our spectrometer greatly simplifies the implementation of dual-comb spectroscopy and offers a high mutual coherence time, measured up to 50 s, without any active stabilization system and/or data processing. The time resolution is as short as 100 µs in our experimental demonstration. For a span of 36 GHz, the mean signal-to-noise ratio of 80, at 100-MHz spectral resolution and 100-µs measurement time, enables precise determination of the parameters of rovibrational lines, including intensity or concentration.

Improved active fiber-based retroreflector with intensity stabilization and a polarization monitor for the near UV.

We present an improved active fiber-based retroreflector (AFR) providing high-quality wavefront-retracing anti-parallel laser beams in the near UV. We use our improved AFR for first-order Doppler-shift suppression in precision spectroscopy of atomic hydrogen, but our setup can be adapted to other applications where wavefront-retracing beams with defined laser polarization are important. We demonstrate how weak aberrations produced by the fiber collimator may remain unobserved in the intensity of the collimated beam but limit the performance of the AFR. Our general results on characterizing these aberrations with a caustic measurement can be applied to any system where a collimated high-quality laser beam is required. Extending the collimator design process by wave optics propagation tools, we achieved a four-lens collimator for the wavelength range 380-486 nm with the beam quality factor of M2 ≃ 1.02, limited only by the not exactly Gaussian beam profile from the single-mode fiber. Furthermore, we implemented precise fiber-collimator alignment and improved the collimation control by combining a precision motor with a piezo actuator. Moreover, we stabilized the intensity of the wavefront-retracing beams and added in-situ monitoring of polarization from polarimetry of the retroreflected light.

Measuring the α-particle charge radius with muonic helium-4 ions.

The energy levels of hydrogen-like atomic systems can be calculated with great precision. Starting from their quantum mechanical solution, they have been refined over the years to include the electron spin, the relativistic and quantum field effects, and tiny energy shifts related to the complex structure of the nucleus. These energy shifts caused by the nuclear structure are vastly magnified in hydrogen-like systems formed by a negative muon and a nucleus, so spectroscopy of these muonic ions can be used to investigate the nuclear structure with high precision. Here we present the measurement of two 2S-2P transitions in the muonic helium-4 ion that yields a precise determination of the root-mean-square charge radius of the α particle of 1.67824(83) femtometres. This determination from atomic spectroscopy is in excellent agreement with the value from electron scattering1, but a factor of 4.8 more precise, providing a benchmark for few-nucleon theories, lattice quantum chromodynamics and electron scattering. This agreement also constrains several beyond-standard-model theories proposed to explain the proton-radius puzzle2-5, in line with recent determinations of the proton charge radius6-9, and establishes spectroscopy of light muonic atoms and ions as a precise tool for studies of nuclear properties.

Two-photon frequency comb spectroscopy of atomic hydrogen.

We have performed two-photon ultraviolet direct frequency comb spectroscopy on the 1S-3S transition in atomic hydrogen to illuminate the so-called proton radius puzzle and to demonstrate the potential of this method. The proton radius puzzle is a significant discrepancy between data obtained with muonic hydrogen and regular atomic hydrogen that could not be explained within the framework of quantum electrodynamics. By combining our result [f 1S-3S = 2,922,743,278,665.79(72) kilohertz] with a previous measurement of the 1S-2S transition frequency, we obtained new values for the Rydberg constant [R ∞ = 10,973,731.568226(38) per meter] and the proton charge radius [r p = 0.8482(38) femtometers]. This result favors the muonic value over the world-average data as presented by the most recent published CODATA 2014 adjustment.

Photon-level broadband spectroscopy and interferometry with two frequency combs.

We probe complex optical spectra at high resolution over a broad span in almost complete darkness. Using a single photon-counting detector at light power levels that are a billion times weaker than commonly employed, we observe interferences in the counting statistics with two separate mode-locked femtosecond lasers of slightly different repetition frequencies, each emitting a comb of evenly spaced spectral lines over a wide spectral span. Unique advantages of the emerging technique of dual-comb spectroscopy, such as multiplex data acquisition with many comb lines, potential very high resolution, and calibration of the frequency scale with an atomic clock, can thus be maintained for scenarios where only few detectable photons can be expected. Prospects include spectroscopy of weak scattered light over long distances, fluorescence spectroscopy of single trapped atoms or molecules, or studies in the extreme-ultraviolet or even soft-X-ray region with comb sources of low photon yield. Our approach defies intuitive interpretations in a picture of photons that exist before detection.

Polariton hyperspectral imaging of two-dimensional semiconductor crystals.

Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with scanning-cavity hyperspectral imaging. We record a spatial map of polariton properties of extended WS2 monolayers coupled to a tunable micro cavity in the strong coupling regime, and correlate it with maps of exciton extinction and fluorescence taken from the same flake with the cavity. We find a high level of homogeneity, and show that polariton splitting variations are correlated with intrinsic exciton properties such as oscillator strength and linewidth. Moreover, we observe a deviation from thermal equilibrium in the resonant polariton population, which we ascribe to non-Markovian polariton-phonon coupling. Our measurements reveal a promisingly consistent polariton landscape, and highlight the importance of phonons for future polaritonic devices.

Mid-infrared feed-forward dual-comb spectroscopy.

Mid-infrared high-resolution spectroscopy has proven an invaluable tool for the study of the structure and dynamics of molecules in the gas phase. The advent of frequency combs advances the frontiers of precise molecular spectroscopy. Here we demonstrate, in the important 3-µm spectral region of the fundamental CH stretch in molecules, dual-comb spectroscopy with experimental coherence times between the combs that exceed half an hour. Mid-infrared Fourier transform spectroscopy using two frequency combs with self-calibration of the frequency scale, negligible contribution of the instrumental line shape to the spectral profiles, high signal-to-noise ratio, and broad spectral bandwidth opens up opportunities for precision spectroscopy of small molecules. Highly multiplexed metrology of line shapes may be envisioned.

A phase-stable dual-comb interferometer.

Laser frequency combs emit a spectrum with hundreds of thousands of evenly spaced phase-coherent narrow lines. A comb-enabled instrument, the dual-comb interferometer, exploits interference between two frequency combs and attracts considerable interest in precision spectroscopy and sensing, distance metrology, tomography, telecommunications, etc. Mutual coherence between the two combs over the measurement time is a pre-requisite to interferometry, although it is instrumentally challenging. At best, the mutual coherence reaches about 1 s. Computer-based phase-correction techniques, which often lead to artifacts and worsened precision, must be implemented for longer averaging times. Here with feed-forward relative stabilization of the carrier-envelope offset frequencies, we experimentally realize a mutual coherence over times approaching 2000 s, more than three orders of magnitude longer than that of state-of-the-art dual-comb systems. An illustration is given with near-infrared Fourier transform molecular spectroscopy with two combs of slightly different repetition frequencies. Our technique without phase correction can be implemented with any frequency comb generator including microresonators or semiconductor lasers.

Quantum Zeno Effect assisted Spectroscopy of a single trapped Ion.

The quantum Zeno effect (QZE) is not only interesting as a manifestation of the counterintuitive behavior of quantum mechanics, but may also have practical applications. When a spectroscopy laser is applied to target atoms or ions prepared in an initial state, the Rabi flopping of an auxiliary transition sharing one common level can be inhibited. This effect is found to be strongly dependent on the detuning of the spectroscopy laser and offers a sensitive spectroscopy signal which allows for high precision spectroscopy of transitions with a small excitation rate. We demonstrate this method with direct frequency comb spectroscopy using the minute power of a single mode to drive a dipole allowed transition in a single trapped ion. Resolving the individual modes of the frequency comb demonstrates that the simple instantaneous quantum collapse description of the QZE can not be applied here, as these modes need several pulses to build up.

Doppler-free Fourier transform spectroscopy.

Sub-Doppler broadband multi-heterodyne spectroscopy is proposed and experimentally demonstrated. Using two laser frequency combs of slightly different repetition frequencies, we have recorded Doppler-free two-photon dual-comb spectra of atomic rubidium resonances of a width of 6 MHz, while simultaneously interrogating a spectral span of 10 THz. The atomic transitions are uniquely identified via the intensity modulation of the observed fluorescence radiation. To the best of our knowledge, these results represent the first demonstration of Doppler-free Fourier transform spectroscopy and extend the range of applications of broadband spectroscopy towards precision nonlinear spectroscopy.

The Rydberg constant and proton size from atomic hydrogen.

At the core of the "proton radius puzzle" is a four-standard deviation discrepancy between the proton root-mean-square charge radii (rp) determined from the regular hydrogen (H) and the muonic hydrogen (µp) atoms. Using a cryogenic beam of H atoms, we measured the 2S-4P transition frequency in H, yielding the values of the Rydberg constant R∞ = 10973731.568076(96) per meterand rp = 0.8335(95) femtometer. Our rp value is 3.3 combined standard deviations smaller than the previous H world data, but in good agreement with the µp value. We motivate an asymmetric fit function, which eliminates line shifts from quantum interference of neighboring atomic resonances.

Multi-pass-cell-based nonlinear pulse compression to 115 fs at 7.5 µJ pulse energy and 300 W average power.

We demonstrate nonlinear pulse compression by multi-pass cell spectral broadening (MPCSB) from 860 fs to 115 fs with compressed pulse energy of 7.5 µJ, average power of 300 W and close to diffraction-limited beam quality. The transmission of the compression unit is >90%. The results show that this recently introduced compression scheme for peak powers above the threshold for catastrophic self-focusing can be scaled to smaller pulse energies and can achieve a larger compression factor than previously reported. Good homogeneity of the spectral broadening across the beam profile is verified, which distinguishes MPCSB among other bulk compression schemes.

Single ion fluorescence excited with a single mode of an UV frequency comb.

Optical frequency combs have revolutionized the measurement of optical frequencies and improved the precision of spectroscopic experiments. Besides their importance as a frequency-measuring ruler, the frequency combs themselves can excite target transitions (direct frequency comb spectroscopy). The direct frequency comb spectroscopy may extend the optical frequency metrology into spectral regions unreachable by continuous wave lasers. In high precision spectroscopy, atoms/ions/molecules trapped in place have been often used as a target to minimize systematic effects. Here, we demonstrate direct frequency comb spectroscopy of single 25Mg ions confined in a Paul trap, at deep-UV wavelengths. Only one mode out of about 20,000 can be resonant at a time. Even then we can detect the induced fluorescence with a spatially resolving single photon camera, allowing us to determine the absolute transition frequency. The demonstration shows that the direct frequency comb spectroscopy is an important tool for frequency metrology for shorter wavelengths where continuous wave lasers are unavailable.Frequency combs are useful tools in high precision measurement including atomic transitions and atomic clocks. Here the authors demonstrate direct frequency comb spectroscopy to shorter wavelengths by probing a transition frequency in a trapped Mg+ ion using a single mode of a UV frequency comb.

Dual-comb coherent Raman spectroscopy with lasers of 1-GHz pulse repetition frequency.

We extend the technique of multiplex coherent Raman spectroscopy with two femtosecond mode-locked lasers to oscillators of a pulse repetition frequency of 1 GHz. We demonstrate a spectra of liquids, which span 1100 cm-1 of Raman shifts. At a resolution of 6 cm-1, their measurement time may be as short as 5 µs for a refresh rate of 2 kHz. The waiting period between acquisitions is improved 10-fold compared to previous experiments with two lasers of 100-MHz repetition frequencies.

Mid-infrared dual-comb spectroscopy with electro-optic modulators.

Absorption spectroscopy of fundamental ro-vibrational transitions in the mid-infrared region provides a powerful tool for studying the structure and dynamics of molecules in the gas phase and for sensitive and quantitative gas sensing. Laser frequency combs permit novel approaches to perform broadband molecular spectroscopy. Multiplex dual-comb spectroscopy without moving parts can achieve particularly high speed, sensitivity and resolution. However, achieving Doppler-limited resolution in the mid-infrared still requires overcoming instrumental challenges. Here we demonstrate a new approach based on difference-frequency generation of frequency-agile near-infrared frequency combs that are produced using electro-optic modulators. The combs have a remarkably flat intensity distribution, and their positions and line spacings can be freely selected by simply dialing a knob. Using the proposed technique, we record, in the 3-µm region, Doppler-limited absorption spectra with resolved comb lines within milliseconds, and precise molecular line parameters are retrieved. Our technique holds promise for fast and sensitive time-resolved studies of, for example, trace gases.

Photothermal effects in ultra-precisely stabilized tunable microcavities.

We study the mechanical stability of a tunable high-finesse microcavity under ambient conditions and investigate light-induced effects that can both suppress and excite mechanical fluctuations. As an enabling step, we demonstrate the ultra-precise electronic stabilization of a microcavity. We then show that photothermal mirror expansion can provide high-bandwidth feedback and improve cavity stability by almost two orders of magnitude. At high intracavity power, we observe self-oscillations of mechanical resonances of the cavity. We explain the observations by a dynamic photothermal instability, leading to parametric driving of mechanical motion. For an optimized combination of electronic and photothermal stabilization, we achieve a feedback bandwidth of 500 kHz and a noise level of 1.1 × 10-13 m rms.

Laser spectroscopy of muonic deuterium.

The deuteron is the simplest compound nucleus, composed of one proton and one neutron. Deuteron properties such as the root-mean-square charge radius rd and the polarizability serve as important benchmarks for understanding the nuclear forces and structure. Muonic deuterium µd is the exotic atom formed by a deuteron and a negative muon µ(-). We measured three 2S-2P transitions in µd and obtain r(d) = 2.12562(78) fm, which is 2.7 times more accurate but 7.5σ smaller than the CODATA-2010 value r(d) = 2.1424(21) fm. The µd value is also 3.5σ smaller than the r(d) value from electronic deuterium spectroscopy. The smaller r(d), when combined with the electronic isotope shift, yields a "small" proton radius r(p), similar to the one from muonic hydrogen, amplifying the proton radius puzzle.