Raman Transitions Research Articles

High‐resolution stimulated Raman spectroscopy of low‐frequency rotational transitions: Obtention of collisional broadening coefficients in the rotational S branch of CO perturbed by H2

AbstractWe demonstrate the application of high‐resolution quasi‐continuous (q‐cw) stimulated Raman spectroscopy (SRS) to the study of low‐frequency, pure rotational transitions of molecules in diluted samples in order to obtain collisional information. The main problems encountered in the few pioneering q‐cw SRS rotational works, namely weak signals because of the small population differences between the upper and lower states of the transitions and the presence of alternating current (AC) Stark effect, have been addressed: technical improvements in the optical elements that perform the beam mixing, separation, and filtering have allowed us to use a collinear beam geometry and a triple pass configuration to enhance the Raman signals. The distortions in the line profiles caused by AC Stark effect have been measured and included in the numerical treatment of the spectra. With these extended capabilities, we have been able to register stimulated Raman transitions with wavenumbers as low as ∼ 11.5 cm−1, corresponding to the S(0) pure rotational transition of the molecule of CO. We have applied the setup to the study of collisional broadening of CO rotational lines perturbed by H2 and have obtained broadening coefficients for lines from S(0) to S(20) at 77, 180, and 298 K. A comparison between these anisotropic coefficients and those obtained from IR rovibrational experiments shows excellent agreement. This is, to our knowledge, the first demonstration of the use of rotational SRS for the obtention of collisional information in diluted gas samples.

A guided light system for agile individual addressing of Ba+ qubits with 10−4 level intensity crosstalk

Trapped ions are one of the leading platforms for quantum information processing, exhibiting the highest gate and measurement fidelities of all contending hardware. In order to realize a universal quantum computer with trapped ions, independent and parallel control over the state of each qubit is necessary. The manipulation of individual qubit states in an ion chain via stimulated Raman transitions generally requires light focused on individual ions. In this manuscript, we present a novel, guided-light individual addressing system for hyperfine Ba+ qubits. The system takes advantage of laser-written waveguide technology, enabled by the atomic structure of Ba+, allowing the use of visible light to drive Raman transitions. Such waveguides define the spatial mode of light, suppressing aberrations that would have otherwise accumulated in a free-space optics set up. As a result, we demonstrate a nearest neighbor relative intensity crosstalk on the order of 10−4, without any active aberration compensation. This is comparable to or better than other previous demonstrations of individual addressing. At the same time, our modular approach provides independent and agile control over the amplitude, frequency, and phase of each channel; combining the strengths of previous implementations.

Multiphoton hyperfine Raman transitions with different quantization axes

Multiphoton hyperfine Raman transitions with different quantization axes

Coherent optical two-photon resonance tomographic imaging in three dimensions

Magnetic resonance imaging is a three-dimensional imaging technique, where a gradient of the magnetic field is used to interrogate spin resonances with spatial resolution. The application of this technique to probe the coherence of atoms with good three-dimensional resolution is a challenging application. We propose and demonstrate an optical method to probe spin resonances via a two-photon Raman transition, reconstructing the 3D-structure of an atomic ensemble’s coherence, which is itself subject to external fields. Our method relies on a single time-and-space resolved heterodyne measurement, allowing the reconstruction of a complex 3D coherence profile. Owing to the optical interface, we reach a tomographic image resolution of 14 × 14 × 36 μm3. The technique allows to probe any transparent medium with a resonance structure and provides a robust diagnostic tool for atom-based quantum information protocols. As such, it is a viable technique for application to magnetometry, electrometry, and imaging of electromagnetic fields.

Super-resolution vibrational imaging based on photoswitchable Raman probe.

Super-resolution vibrational microscopy is promising to increase the degree of multiplexing of nanometer-scale biological imaging because of the narrower spectral linewidth of molecular vibration compared to fluorescence. However, current techniques of super-resolution vibrational microscopy suffer from various limitations including the need for cell fixation, high power loading, or complicated detection schemes. Here, we present reversible saturable optical Raman transitions (RESORT) microscopy, which overcomes these limitations by using photoswitchable stimulated Raman scattering (SRS). We first describe a bright photoswitchable Raman probe (DAE620) and validate its signal activation and depletion characteristics when exposed to low-power (microwatt level) continuous-wave laser light. By harnessing the SRS signal depletion of DAE620 through a donut-shaped beam, we demonstrate super-resolution vibrational imaging of mammalian cells with excellent chemical specificity and spatial resolution beyond the optical diffraction limit. Our results indicate RESORT microscopy to be an effective tool with high potential for multiplexed super-resolution imaging of live cells.

Enhancing strontium clock atom interferometry using quantum optimal control

Strontium clock atom interferometry is a promising new technology, with multiple experiments under development around the world to explore its potential for dark matter and gravitational wave detection. In these detectors, large momentum transfer using sequences of many laser pulses is necessary, and thus high-fidelity pulses are important since small errors become magnified. Quantum optimal control (QOC) is a framework for developing control pulse waveforms that achieve high fidelity and are robust against experimental imperfections. Resonant single-photon transitions using the narrow clock transition of strontium involve significantly different quantum dynamics than more established atom interferometry methods based on far-detuned two-photon Raman or Bragg transitions, which leads to new opportunities and challenges when applying QOC. Here, we study in simulation QOC pulses for strontium clock interferometry and demonstrate their advantage over basic square pulses (primitive pulses) and composite pulses in terms of robustness against multiple noise channels. This could improve the scale of large momentum transfer in Sr clock interferometers, paving the way to achieving these scientific goals.

Induced position-dependent spin–orbit coupling in atomic Bose–Einstein condensate

In this paper, we study-induced spin–orbit coupling (SOC) in one-dimensional ultracold quantum gases composed of atoms of different species. One species is subjected to an equal combination of Rashba and Dresselhaus SOC generated by Raman transition. The two species interact with each other through spin-independent and spin-exchange contact interactions. The spin-exchange interaction introduces a locking pattern of the momentum and spin degrees of freedom for the species without direct SOC. For small spin-independent interactions, the two species overlap and the induced SOC is effective. For large spin-independent interactions, however, the two species keep separate from each other and the induced SOC is negligible. We propose to generate inhomogeneous SOC by exploiting density engineering technique applied to the directly spin–orbit coupled Bose–Einstein condensate. When the effective potential is of Gaussian type, the single-particle eigenenergies and eigenstates are calculated by exact diagonalization method. For general cases, mean-field ground states are obtained by numerically searching for the minimum of energy functional. With the density engineering technique, it is possible to produce hybrid structures of plane wave, stripe and/or zero-momentum phases.

Direct manipulation of a superconducting spin qubit strongly coupled to a transmon qubit

Spin qubits in semiconductors are currently one of the most promising architectures for quantum computing. However, they face challenges in realizing multi-qubit interactions over extended distances. Superconducting spin qubits provide a promising alternative by encoding a qubit in the spin degree of freedom of an Andreev level. Such an Andreev spin qubit could leverage the advantages of circuit quantum electrodynamic, enabled by an intrinsic spin-supercurrent coupling. The first realization of an Andreev spin qubit encoded the qubit in the excited states of a semiconducting weak-link, leading to frequent decay out of the computational subspace. Additionally, rapid qubit manipulation was hindered by the need for indirect Raman transitions. Here, we exploit a different qubit subspace, using the spin-split doublet ground state of an electrostatically-defined quantum dot Josephson junction with large charging energy. Additionally, we use a magnetic field to enable direct spin manipulation over a frequency range of 10 GHz. Using an all-electric microwave drive we achieve Rabi frequencies exceeding 200 MHz. We furthermore embed the Andreev spin qubit in a superconducting transmon qubit, demonstrating strong coherent qubit-qubit coupling. These results are a crucial step towards a hybrid architecture that combines the beneficial aspects of both superconducting and semiconductor qubits.

Spectral properties of IR-filamentation in air induced by 1 ps pulses for coherent anti-Stokes Raman scattering

We investigate the spectral properties of ps laser-induced filamentation in air using an ultrafast thin-disk based amplifier at a central wavelength of 1030 nm with a maximum pulse energy of 60 mJ at a repetition rate of 1 kHz. We show that the spectrum induced by filamentation in air is sufficiently broad to excite ro-vibrational Raman transitions in N2, O2 and CH4. The excitation is probed with the second harmonic (515 nm) to generate CARS signals in air. Furthermore, we investigate the influence of optical windows on the CARS signal for applications in combustion and gasification diagnostics.

Photon scattering errors during stimulated Raman transitions in trapped-ion qubits

We study photon scattering errors in stimulated Raman driven quantum logic gates. For certain parameter regimes, we find that previous simplified models of the process significantly overestimate the gate error rate due to photon scattering. This overestimate is shown to be due to previous models neglecting the detuning dependence of the scattered photon frequency and Lamb-Dicke parameter, a second scattering process, interference effects on scattering rates to metastable manifolds, and the counterrotating contribution to the Raman transition rate. The resulting improved model shows that there is no fundamental limit on gate error due to photon scattering for electronic ground-state qubits in commonly used trapped-ion species when the Raman laser beams are red detuned from the main optical transition. Additionally, photon scattering errors are studied for qubits encoded in the metastable ${D}_{5/2}$ manifold, showing that gate errors below ${10}^{\ensuremath{-}4}$ are achievable for all commonly used trapped ions.

Visualizing ultrafast weak-field-induced rotational revivals of air molecules at room temperature.

The ability to observe quantum coherence and interference is crucial for understanding quantum effects in nonlinear optical spectroscopy and is of fundamental interest in quantum mechanics. Here, we present an experimental study combined with theoretical analysis and numerical simulations to identify the underlying process behind the rotational revivals induced by a pair of time-delayed ultrafast femtosecond laser pulses for air molecules under ambient conditions. Our time-resolved two-dimensional alignment measurements confirm that one-step non-resonant Raman transitions from initial states of mixed molecules play a dominant role, showing a signature of weak-field-induced rotational revivals. Furthermore, we demonstrate that such rotational revival spectra can simultaneously measure the entire pure rotational Raman spectra and observe the quantum interference between two transition pathways from a given initial state. This work provides a powerful tool to observe, control, and identify the rotational dynamics of mixed molecular samples under weak-field excitations.

Degenerate Raman sideband cooling of K40 atoms

We report on the implementation of degenerate Raman sideband cooling of $^{40}$K atoms. The scheme incorporates a 3D optical lattice, which confines the atoms and drives the Raman transitions. The optical cooling cycle is closed by two optical pumping beams. The wavelength of the laser beams forming the lattice is close to the D$_2$ atomic transition, while the optical pumping is operated near the D$_1$ transition. With this cooling method, we achieve temperature of $\sim$$1\mu$K of a cloud with $\sim$$10^7$ atoms. This corresponds to a phase space density of $\ge$$10^{-3}$. Moreover, the fermionic ensemble is spin polarized to conditions which are favorable for subsequent evaporative cooling. We study the dependence of the cooling scheme on several parameters, including the applied magnetic field, the detuning, duration, and intensity profile of the optical pumping beams. Adding this optical cooling stage to current Fermi gas experiments can improve the final conditions and increase the data rate.

Pump-probe spectroscopy of chiral vibrational dynamics.

A planar molecule may become chiral upon excitation of an out-of-plane vibration, changing its handedness during half a vibrational period. When exciting such a vibration in an ensemble of randomly oriented molecules with an infrared laser, half of the molecules will undergo the vibration phase-shifted by π compared to the other half, and no net chiral signal is observed. This symmetry can be broken by exciting the vibrational motion with a Raman transition in the presence of a static electric field. Subsequent ionization of the vibrating molecules by an extreme ultraviolet pulse probes the time-dependent net handedness via the photoelectron circular dichroism. Our proposal for pump-probe spectroscopy of molecular chirality, based on quantum-chemical theory and discussed for the example of the carbonyl chlorofluoride molecule, is feasible with current experimental technology.

Generation of time-bin-encoded photons in an ion-cavity system

We investigate two single-photon generation schemes and compare their suitability for use in time-bin entanglement encoding. A trapped ion coupled to an optical cavity produces single photons through a cavity-assisted Raman transition. By manipulating the phase relationship between time-bins of successive photons, distinct features in the interference pattern of a Hong–Ou–Mandel measurement emerge. Through careful selection of the initial state, detrimental effects of spontaneous emission can be significantly reduced. We demonstrate that this reduction allows us to impart a measurable phase profile onto the emitted photons making time-bin entanglement encoding feasible with an ion-cavity system.

Compact single-seed, module-based laser system on a transportable high-precision atomic gravimeter

A single-seed, module-based compact laser system is demonstrated on a transportable 87Rb-based high-precision atomic gravimeter. All the required laser frequencies for the atom interferometry are provided by free-space acousto-optic modulators (AOMs) and resonant electro-optic phase modulators (EOMs). The optical phase-locked loop between the two optical paths derived from the same laser provides an easy frequency manipulation between two laser frequencies separated by the hyperfine frequency of 6.835 GHz using an AOM and an EOM, respectively. Our scheme avoids parasite Raman transitions present in the direct EOM modulation scheme (modulating directly at the frequency of the hyperfine splitting), which have detrimental effects on the accuracy of the gravity measurements. The optical phase-locked loop also provides a convenient way for vibration compensation through the Raman lasers' phase offset. Furthermore, the modular design approach allows plug-and-play nature on each individual optic module and also increases the mechanical stability of the optical systems. We demonstrate high-precision gravity measurements with 17.8 μGal stability over 250 s averaging time and 2.5 μGal stability over 2 h averaging time.

Atom Interferometer Driven by a Picosecond Frequency Comb.

We demonstrate a light-pulse atom interferometer based on the diffraction of free-falling atoms by a picosecond frequency-comb laser. More specifically, we coherently split and recombine wave packets of cold ^{87}Rb atoms by driving stimulated Raman transitions between the |5s ^{2}S_{1/2},F=1⟩ and |5s ^{2}S_{1/2},F=2⟩ hyperfine states, using two trains of picosecond pulses in a counterpropagating geometry. We study the impact of the pulses' length as well as the interrogation time onto the contrast of the atom interferometer. Our experimental data are well reproduced by a numerical simulation based on an effective coupling that depends on the overlap between the pulses and the atomic cloud. These results pave the way for extending light-pulse interferometry to transitions in other spectral regions and therefore to other species, for new possibilities in metrology, sensing of gravito-inertial effects, and tests of fundamental physics.

Tunable High-Q Factor Substrate for Selectively Enhanced Raman Scattering

Most Surface-enhanced Raman scattering (SERS) substrates enhance all the Raman signals in a relative broad spectral range. The substrates enhance both the interested and background signals together. To improve the identification of target molecules from numerous background ones, substrates with multi high-quality (Q) factor resonance wavelengths can be designed to achieve the selective enhancement of specific Raman transitions. When the resonance frequencies are modulated to match the excitation and Raman scattering frequencies, the detection of the target molecule can be more effective. In this paper, we design a tunable high-Q SERS substrate with periodic silver bowtie nanoholes on silica spacer and silver film. The substrate possessed three high-Q and high electric field resonance modes, which resulted from the interaction of the localized surface plasmon resonance (LSPR) of the bowtie nanoholes, the surface plasmon polariton (SPP) of the period bowtie nanoholes and the Fabry–Perot (FP) resonance between the bowtie and silver film bottom. The interaction between these resonance modes resulted in not only a higher quality (Q) factor, but also a higher electric field, which can be employed to realize a potential substrate in high-sensitivity and selective-detection fields.

Impact of additional sidebands generated by a tapered amplifier on an atom interferometer.

Stimulated Raman transitions are often used in an atom interferometer (AI) for wave packet manipulation. Normally, two lasers with different frequencies contained in a Raman beam are combined first and then amplified by a single tapered amplifier (TA). This configuration can simplify the laser system of the AI, however, additional sidebands will be generated by the TA because of the nonlinear effect in the TA. In this work, the impact of additional sidebands generated with a single TA on the AI is studied. We first observe the additional sidebands in a Raman laser by a Fabry-Pérot interferometer (FPI), and the additional sidebands will be greatly suppressed by reducing the injection laser power of the TA. This is also confirmed by observing the position-dependent Raman transitions induced by additional sidebands at different injection power in an AI. However, the phase shifts induced by additional sidebands are not reduced obviously when the injection power of the TA is reduced. Therefore, it is necessary to separately amplify two lasers contained in the Raman laser by two TAs for a high precision AI. The spectroscopy of Raman laser generated by two TAs is also measured by the FPI, and the impact of additional sidebands on the AI is eliminated. This work has guiding significance for the design of the laser system in a high-precision AI.

Controlling atomic spin mixing via multiphoton transitions in a cavity

We propose to control spin-mixing dynamics in a gas of spinor atoms, via the combination of two off-resonant Raman transition pathways, enabled by a common cavity mode and a bichromatic pump laser. The mixing rate, which is proportional to the synthesized spin-exchange interaction strength, and the effective atomic quadratic Zeeman shift (QZS), can both be tuned by changing the pump laser parameters. Quench and driving dynamics of the atomic collective spin are shown to be controllable on a faster time scale than in existing experiments based on inherent spin-exchange collision interactions. The results we present open a promising avenue for exploring spin-mixing physics of atomic ensembles accessible in current experiments.

Motion-selective coherent population trapping by Raman sideband cooling along two paths in a Λ configuration

We report our experiment on sideband cooling with two Raman transitions in a $\Lambda$ configuration that allows selective coherent population trapping (CPT) of the motional ground state. The cooling method is applied to $^{87}$Rb atoms in a circularly-polarized one-dimensional optical lattice. Owing to the vector polarizability, the vibration frequency of a trapped atom depends on its Zeeman quantum number, and CPT resonance for a pair of bound states in the $\Lambda$ configuration depends on their vibrational quantum numbers. We call this scheme motion-selective coherent population trapping (MSCPT) and it is a trapped-atom analogue to the velocity-selective CPT developed for free He atoms. We observe a pronounced dip in temperature near a detuning for the Raman beams to satisfy the CPT resonance condition for the motional ground state. Although the lowest temperature we obtain is ten times the recoil limit owing to the large Lamb-Dicke parameter of 2.3 in our apparatus, the experiment demonstrates that MSCPT enhances the effectiveness of Raman sideband cooling and enlarges the range of its application. Discussions on design parameters optimized for MSCPT on $^{87}$Rb atoms and opportunities provided by diatomic polar molecules, whose Stark shift shows strong dependence on the rotational quantum number, are included.