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IEEE Photonics Technology Letters

Single-Shot Fourier-Slice Dual-Comb Spectroscopy

Bachana Lomsadze, Skyler C. Weight, Peyton Clark

Published Oct 18, 2023• 3 citations
Publisher

Abstract

Multidimensional coherent spectroscopy is a powerful method for studying materials’ optical properties. It also has potential to be used for chemical sensing applications as it allows the measurements of samples’ energy level structures as well as couplings between the excited states resonances. This coupling information is the key to identify whether or not the sample contains a mixture of analytes. Coupling information is not easily accessible using one-dimensional linear or non-linear methods, necessitating more complex multidimensional experimental techniques. However, multidimensional techniques require bulky apparatus, complex stabilization schemes, and/or long acquisition times that prevent them from being used outside the lab. Here we propose and demonstrate a new and simple approach that enables the measurements of the main absorption lines as well as the couplings between the excited states resonances extremely fast (tens to hundreds of$\mu \text{s}$) without measuring the full multidimensional spectra. This approach is based on the Fourier-slice theorem and was inspired by frequency comb technology, particularly dual-comb spectroscopy. Our approach uses free-running lasers and co-linear geometry, and with the development of compact lasers this approach can become field-deployable for sensing applications. We demonstrate the concept on rubidium vapor.

DOI
10.1109/lpt.2023.3325799

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Multidimensional coherent spectroscopy is a powerful method for studying materials’ optical properties. It also has potential to be used for chemical sensing applications as it allows the measurements of samples’ energy level structures as well as couplings between the excited states resonances. This coupling information is the key to identify whether or not the sample contains a mixture of analytes. Coupling information is not easily accessible using one-dimensional linear or non-linear methods, necessitating more complex multidimensional experimental techniques. However, multidimensional techniques require bulky apparatus, complex stabilization schemes, and/or long acquisition times that prevent them from being used outside the lab. Here we propose and demonstrate a new and simple approach that enables the measurements of the main absorption lines as well as the couplings between the excited states resonances extremely fast (tens to hundreds ofμs\mu \text{s}μs) without measuring the full multidimensional spectra. This approach is based on the Fourier-slice theorem and was inspired by frequency comb technology, particularly dual-comb spectroscopy. Our approach uses free-running lasers and co-linear geometry, and with the development of compact lasers this approach can become field-deployable for sensing applications. We demonstrate the concept on rubidium vapor.
Vapor-cell spectroscopy is an essential technique in many fields and is particularly relevant for quantum technologies. Most atom- and ion-trapping experiments rely on simultaneous spectroscopy of two atomic transitions, employing a separate apparatus for each transition. We demonstrate simultaneous spectroscopy on two atomic transitions, within a single apparatus, using spatially overlapped beams from two independent lasers. This method enables compact setups and offers superior spectroscopic performance, leading to sharper spectroscopy peaks, stronger absorption signals, and superior laser stability. Doppler-free locking features become accessible over a frequency range several hundred megahertz wider than for standard saturated absorption spectroscopy. Exploring the full parameter space associated with dual-frequency spectroscopy reveals a latticelike structure of sharp resonance features, which enhances experimental versatility by allowing laser frequency stabilization within a wide manifold of locations in two-dimensional frequency space. We present data for 133Cs^{133}\mathrm{Cs}133Cs and 85Rb^{85}\mathrm{Rb}85Rb and compare our results to a theoretical model. Employing the technique for frequency stabilization close to the D2{D}_{2}D2​ line of 85Rb^{85}\mathrm{Rb}85Rb results in an improvement in frequency stability by a factor typically between 2 and 3 for averaging times of up to 1 s. The technique will advance portable quantum technologies and facilitate high-precision measurements.
Multidimensional coherent spectroscopy is a powerful tool for understanding the ultrafast dynamics of complex quantum systems. To fully characterize the nonlinear optical response of a system, multiple pulse sequences must be recorded and quantitatively compared. We present a new single-scan method that enables rapid and parallel acquisition of all unique pulse sequences corresponding to first- and third-order degenerate wave-mixing processes. Signals are recorded with shot-noise limited detection, enabling acquisition times of ~2 minutes with ~100 zs phase stability and ~8 orders of dynamic range, in a collinear geometry, on a single-pixel detector. We demonstrate this method using quantum well excitons, and quantitative analysis reveals new insights into the bosonic nature of excitons. This scheme may enable rapid and scalable analysis of unique chemical signatures, metrology of optical susceptibilities, nonperturbative coherent control, and the implementation of quantum information protocols using multidimensional spectroscopy.
Abstract Optical multidimensional coherent spectroscopy provides information about the structure and excitation dynamics in a broad range of material systems. This book focuses on systems of interest in physics, including atomic vapors, semiconductor nanostructures and two-dimensional materials. An introduction to ultrafast spectroscopy and the fundamental concepts of multidimensional coherent spectroscopy applies to all material systems. Relevant experimental implementations, including phase-stabilized crossed-beams, frequency-tagged fully-collinear, three-dimensional and frequency-comb based methods. The use of the method to study atomic vapors, semiconductor quantum wells, semiconductor quantum dots and two-dimensional materials are described in separate chapters. The final chapters survey the use of the method in some other areas and speculate on future directions.
In recent years, frequency-comb-based multidimensional coherent spectroscopy has emerged as a very powerful optical method for studying samples with long dephasing times. It enables the measurement of comb resolution multidimensional coherent spectra in seconds as opposed to hours or even days required by traditional mechanical stage-based spectrometers. However, for some samples (e.g., cold atoms and molecules) the dephasing times could be longer than the repetition periods of the excitation lasers which means that the generated signal will not fully decay between the pulses. Depending on the relative phase or time between the pulses, the signals generated by the subsequent laser pulses can constructively or destructively interfere with each other. In this paper we study this behavior by solving the optical Bloch equations and provide a theoretical description of frequency-comb-based multidimensional coherent spectroscopy.
Abstract Multidimensional coherent spectroscopy (MDCS) is a highly intriguing field for the unique capacities to unravel quantum pathways of microscopic dynamics and discern different dipole–dipole interactions. These capabilities are not simultaneously accessible through any other techniques. The foundation of MDCS lies in the stable phase and accurate time information of the multi‐pulse sequences involved. Achieving the phase stability has traditionally relied on ingenious geometric optical designs and multiple feedback control systems, albeit at the cost of complexity. In this letter, a phase stability scheme for high‐resolution MDCS is proposed by replacing traditional laser sources with two highly coherent frequency combs. By employing dual‐comb interferometry, the phase distribution across a broad spectral range and the time information of all the excitation pulses are precisely measured, even in setups that lack phase stability. In the experiment, a rephasing MDCS of rubidium atoms is obtained by applying this approach, wherein the comb resolution is utilized to differentiate the couplings of hyperfine energy levels. This scheme simplifies the structure of MDCS and holds potential for applications in other MDCS systems involving many‐body interactions and non‐absorptive resonances.