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Optics Express

Full-field optical spectroscopy at a high spectral resolution using atomic vapors

Romanus J. Hutchins, Giulia Zanini, Giuliano Scarcelli

Published Dec 22, 2022• 5 citations
Publisher

Abstract

Spectral imaging techniques extract spectral information using dispersive elements in combination with optical microscopes. For rapid acquisition, multiplexing spectral information along one dimension of imaged pixels has been demonstrated in hyperspectral imaging, as well as in Raman and Brillouin imaging. Full-field spectroscopy, i.e., multiplexing where imaged pixels are collected in 2D simultaneously while spectral analysis is performed sequentially, can increase spectral imaging speed, but so far has been attained at low spectral resolutions. Here, we extend 2D multiplexing to high spectral resolutions of ∼80 MHz (∼0.0001 nm) using high-throughput spectral discrimination based on atomic transitions.

DOI
10.1364/oe.479253

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Spectral imaging techniques extract spectral information using dispersive elements in combination with optical microscopes. For rapid acquisition, multiplexing spectral information along one dimension of imaged pixels has been demonstrated in hyperspectral imaging, as well as in Raman and Brillouin imaging. Full-field spectroscopy, i.e., multiplexing where imaged pixels are collected in 2D simultaneously while spectral analysis is performed sequentially, can increase spectral imaging speed, but so far has been attained at low spectral resolutions. Here, we extend 2D multiplexing to high spectral resolutions of ∼80 MHz (∼0.0001 nm) using high-throughput spectral discrimination based on atomic transitions.
Sensing with undetected photons has become a vibrant, application-driven research domain with a special focus on the mid-infrared (mid-IR) wavelength region. Since the mid-IR contains spectral bands with highly specific and strong molecular absorbance signatures, often referred to as fingerprints, a multitude of different samples and their compositions can be detected and quantified spectroscopically. Enhancing this spectroscopic method with imaging capabilities leads to a powerful technique for environmental monitoring and biomedical applications that enables automated diagnostics while omitting time-consuming and non-reversible labeling steps. To evade the shortcomings of state-of-the-art instruments for mid-IR hyperspectral microscopy—namely cost, complexity, power consumption, and performance, which stem from technological challenges in mid-IR detection and light sources—we construct a proof-of-concept nonlinear interferometer in a wide-field imaging arrangement. This nominally narrowband imaging technique is then expanded to acquire broadband spectral information through capturing images for varying interferometer displacement and applying a pixelwise Fourier-transform of the resulting interferograms, yielding high-resolution infrared spectra for each camera pixel. For the broadband range of 2300−3100cm −1 , covering the important CH-stretch band, we perform hyperspectral imaging that simultaneously resolves 3500 spatial modes, each with a spectral resolution of 10cm −1 , leveraging in total around 10 5 spatio-spectrally entangled photon modes. Our image acquisition uses a commercial sCMOS camera, while a medium-power and compact continuous-wave pump laser is the only necessary light source. For a moderate speed of 360 voxel/s, we obtain a predominantly shot-noise-influenced signal-to-noise ratio (SNR) of 50. We further demonstrate the practicality of our novel hyperspectral imaging technique for microplastics detection and bio-imaging tasks and outline engineering solutions to increase its speed by several orders of magnitude. This shows that our quantum imaging technique is highly promising for applications requiring compact, cost-effective label-free analyses.
We have developed a frequency-multiplex laser spectrometer using the concept of stochastic excitation to provide an effective optical excitation bandwidth of >200 MHz and an inherent spectral resolution of a few kilohertz. A frequency-stabilized Ar+ laser is phase-modulated by a pseudorandom binary sequence (PRBS) running at a clock frequency of 200 MHz. The detected system response to the stochastic optical field is cross-correlated with an identical time-delayed PRBS to give the equivalent of a free induction decay signal. A time-to-frequency transformation then gives the transfer function of the optically absorbing/dispersing system. The calibration and linearity of the frequency axis are dependent only on the oscillator used to clock the PRBS generators, thus avoiding the problems of drift and nonlinearities in ordinary sequential-scan spectroscopy. The multiplexing scheme allows a spectrum to be obtained in much less time than sequential scanning or, equivalently, gives a higher SNR for the same amount of data taking time. We have demonstrated the spectrometer by observing Doppler-free transitions in molecular iodine. We also describe the use of digitally filtered binary sequences and active control of residual amplitude modulation to improve the SNR of the spectrometer and possibilities for increasing the excitation bandwidth of the system.
Femtosecond (fs) interferometry combined with acousto-optical phase modulation is an effective approach to implement various types of coherent nonlinear and multidimensional spectroscopy schemes. Here, we focus on gaseous and ultracold samples and compare directly the performance and spectral resolution between two experimental implementations of the phase modulation technique, which are stepwise and continuous rapid scanning of the underlying Fourier transform (FT) interferometers. We show the performance advantage of the rapid-scanning approach and demonstrate a spectral resolution of 250 MHz in the spectroscopy of laser-cooled Li atoms. This is a 10-fold resolution improvement compared to previous experiments.
In this thesis, I report on the development of imaging techniques in atomic vapor cells. This is a relatively unexplored area, despite the ubiquitous use of imaging in experiments with ultracold atoms. Our main focus is in high resolution imaging of microwave near fields, for which there is currently no satisfactory established technique. We detect microwave fields through Rabi oscillations driven by the microwave on atomic hyperfine transitions. The technique can be easily modified to also image dc magnetic fields. In addition, we have developed techniques to image vapor cell processes such as atomic T1 and T2 relaxation. These provide a new window into vapor cell physics, which we have used to obtain spatially resolved information on Rb interactions with the cell walls, and to estimate the Rb relaxation probability in a collision with the cell wall. \n \nAs a first application of our imaging techniques, we imaged the dc and microwave magnetic fields inside a state-of-the-art vapor cell atomic clock. This new clock characterisation technique should lead to real improvements in clock performance, and is in the process of being adopted by the atomic clock community. \n \nWe have developed a widefield, high resolution imaging setup using a microfabricated vapor cell, which we have used to image microwave and dc magnetic vector fields. With the addition of a 480 nm laser, the setup can be configured to image microwave electric fields. Our camera-based imaging system records 2D images with a 6x6 mm2 field of view at a rate of 10 Hz. It provides up to 50 um spatial resolution, and allows imaging of fields as close as 150 um above structures, through the use of extremely thin external cell walls. This is crucial in allowing us to take practical advantage of the high spatial resolution, as feature sizes in near-fields are on the order of the distance from their source, and represents an order of magnitude improvement in surface-feature resolution compared to previous vapor cell experiments. We demonstrate a microwave magnetic field sensitivity of 1.4 uT/sqrt-Hz per 50x50x140 um3 voxel, at present limited by the speed of our imaging system. Since we image 120x120 voxels in parallel, a single scanned sensor would require a sensitivity of at least 12 nT/sqrt-Hz to produce images with the same sensitivity. \n \nThe spatial resolution, distance of approach, and sensitivity of our high resolution setup are sufficient for characterising 6.8 GHz microwave fields above a range of real world devices. However, frequency tunability is essential for wider applications of our imaging technique. Industry is particularly interested in techniques for imaging high frequency microwaves, above 18 GHz, where simulations become increasingly unreliable. I have shown that our technique can be extended to image microwaves of any frequency, in principle from dc to 100s of GHz, by using a large dc magnetic field to Zeeman shift the hyperfine ground state transitions to the desired frequency. I present results from a proof-of-principle setup, where we have used a 0.8 T solenoid to detect and image microwaves from 2.3 GHz to 26.4 GHz. \n
Brillouin Microscopy allows for the characterization of tissues and cells by measuring the frequency shift of light when they interact with phonons in material. Due to the low scattering cross section and higher powers posing a risk for photodamage, fast acquisition times remain a challenge. To alleviate these issues, parallelizing the signal collection by collecting an entire image allows for 2-dimensional parallelization. We demonstrate a spectrometer based on induced dichroism in atomic vapors, with an improved pumping scheme to our previous design, for use with light sheet microscopy, and demonstrate its ability to capture an entire 2D Brillouin image.
Imaging of electric and magnetic fields is limited by the fact that conventional field probes rely on conductive elements that perturb the fields they are meant to measure and require either spatial scanning or arrays to produce field maps. Atomic sensors based on Rydberg states offer a minimally invasive and broadband alternative, enabling absolute field measurements without external calibration. In this work, we present a field imaging technique that combines the spatial resolution of planar laser-induced fluorescence-dip spectroscopy with the field sensitivity and spectral resolution of electromagnetically induced transparency (EIT) using Rydberg states of atomic vapor. By imaging the change in fluorescence due to EIT, we spatially resolve the field-induced shifts in atomic energy levels, enabling the imaging of arbitrary electric field distributions from MHz to tens of GHz at the ∼V/cm level and static magnetic fields at the ∼mT level. We also image resonant microwave electric fields at the ∼5 mV/cm level. This technique achieves a spatial resolution of 160 µm, limited by our camera, with a fundamental resolution limit near 5 µm.