Superluminal light propagation in a three-level ladder system.

Superluminal light propagation is typically accompanied by significant absorption that might prevent its observation in realistic samples. We propose an all-optical implementation exploiting the two-photon resonance in three-level media to overcome this problem. With several computational methods, we analyze three possible configurations of optically-dressed systems and identify an optimal configuration for superluminal propagation. Due to the far-detuned operating regime with low absorption, this scenario avoids the usual need for population inversion, gain assistance or nonlinear optical response. Our analysis covers a broad parameter space and aims for the identification of conditions where significant pulse advancement can be achieved at high transmission levels. In this context, a figure of merit is introduced accounting for a trade-off between the desired group-index values and transmission level. This quantity helps to identify the optimal characteristics of the dressing beam.

Zero- to low-field relaxometry of chemical and biological fluids.

Nuclear magnetic resonance (NMR) relaxometry is an analytical method that provides information about molecular environments, even for NMR "silent" molecules (spin-0), by analyzing the properties of NMR signals versus the magnitude of the longitudinal field. Conventionally, this technique is performed at fields much higher than Earth's magnetic field, but our work focuses on NMR relaxometry at zero and ultra-low magnetic fields (ZULFs). Operating under such conditions allows us to investigate slow (bio)chemical processes occurring on a timescale from milliseconds to seconds, which coincide with spin evolution. ZULFs also minimize T2 line broadening in heterogeneous samples resulting from magnetic susceptibility. Here, we use ZULF NMR relaxometry to analyze (bio)chemical compounds containing 1H-13C, 1H-15N, and 1H-31P spin pairs. We also detected high-quality ULF NMR spectra of human whole-blood at 0.8 µT, despite a shortening of spin relaxation by blood proteomes (e.g., hemoglobin). Information on proton relaxation times of blood, a potential early biomarker of inflammation, can be acquired in under a minute using inexpensive, portable/small-size NMR spectrometers based on atomic magnetometers.

Detection of pyridine derivatives by SABRE hyperpolarization at zero field.

Nuclear magnetic resonance (NMR) spectroscopy is a powerful analytical tool used in modern science and technology. Its novel incarnation, based on measurements of NMR signals without external magnetic fields, provides direct access to intramolecular interactions based on heteronuclear scalar J-coupling. The uniqueness of these interactions makes each zero-field NMR spectrum distinct and useful in chemical fingerprinting. However, the necessity of heteronuclear coupling often results in weak signals due to the low abundance of certain nuclei (e.g., 15N). Hyperpolarization of such compounds may solve the problem. In this work, we investigate molecules with natural isotopic abundance that are polarized using non-hydrogenative parahydrogen-induced polarization. We demonstrate that spectra of hyperpolarized naturally abundant pyridine derivatives can be observed and uniquely identified whether the same substituent is placed at a different position of the pyridine ring or different constituents are placed at the same position. To do so, we constructed an experimental system using a home-built nitrogen vapor condenser, which allows for consistent long-term measurements, crucial for identifying naturally abundant hyperpolarized molecules at a concentration level of ~1 mM. This opens avenues for future chemical detection of naturally abundant compounds using zero-field NMR.

Response of atomic spin-based sensors to magnetic and nonmagnetic perturbations.

Searches for pseudo-magnetic spin couplings require implementation of techniques capable of sensitive detection of such interactions. While Spin-Exchange Relaxation Free (SERF) magnetometry is one of the most powerful approaches enabling the searches, it suffers from a strong magnetic coupling, deteriorating the pseudo-magnetic coupling sensitivity. To address this problem, here, we compare, via numerical simulations, the performance of SERF magnetometer and noble-gas-alkali-metal co-magnetometer, operating in a so-called self-compensating regime. We demonstrate that the co-magnetometer allows reduction of the sensitivity to low-frequency magnetic fields without loss of the sensitivity to nonmagnetic couplings. Based on that we investigate the responses of both systems to the oscillating and transient spin perturbations. Our simulations reveal about five orders of magnitude stronger response to the neutron pseudo-magnetic coupling and about three orders of magnitude stronger response to the proton pseudo-magnetic coupling of the co-magnetometer than those of the SERF magnetometer. Different frequency responses of the co-magnetometer to magnetic and nonmagnetic perturbations enables differentiation between these two types of interactions. This outlines the ability to implement the co-magnetometer as an advanced sensor for the Global Network of Optical Magnetometer for Exotic Physics searches (GNOME), aiming at detection of ultra-light bosons (e.g., axion-like particles).

Search for topological defect dark matter with a global network of optical magnetometers.

Ultralight bosons such as axion-like particles are viable candidates for dark matter. They can form stable, macroscopic field configurations in the form of topological defects that could concentrate the dark matter density into many distinct, compact spatial regions that are small compared with the Galaxy but much larger than the Earth. Here we report the results of the search for transient signals from the domain walls of axion-like particles by using the global network of optical magnetometers for exotic (GNOME) physics searches. We search the data, consisting of correlated measurements from optical atomic magnetometers located in laboratories all over the world, for patterns of signals propagating through the network consistent with domain walls. The analysis of these data from a continuous month-long operation of GNOME finds no statistically significant signals, thus placing experimental constraints on such dark matter scenarios.

Zero-Field NMR of Urea: Spin-Topology Engineering by Chemical Exchange.

Well-resolved and information-rich J-spectra are the foundation for chemical detection in zero-field NMR. However, even for relatively small molecules, spectra exhibit complexity, hindering the analysis. To address this problem, we investigate an example biomolecule with a complex J-coupling network─urea, a key metabolite in protein catabolism─and demonstrate ways of simplifying its zero-field spectra by modifying spin topology. This goal is achieved by controlling pH-dependent chemical exchange rates of 1H nuclei and varying the composition of the D2O/H2O mixture used as a solvent. Specifically, we demonstrate that by increasing the proton exchange rate in the [13C,15N2]-urea solution, the spin system simplifies, manifesting through a single narrow spectral peak. Additionally, we show that the spectra of 1H/D isotopologues of [15N2]-urea can be understood easily by analyzing isolated spin subsystems. This study paves the way for zero-field NMR detection of complex biomolecules, particularly in biofluids with a high concentration of water.

Zero-Field NMR J-Spectroscopy of Organophosphorus Compounds.

Organophosphorus compounds are a wide and diverse class of chemicals playing a crucial role in living organisms. This aspect has been often investigated using nuclear magnetic resonance (NMR), which provides information about molecular structure and function. In this paper, we report the results of theoretical and experimental studies on basic organophosphorus compounds using zero-field NMR, where spin dynamics are investigated in the absence of a magnetic field with the dominant heteronuclear J-coupling. We demonstrate that the zero-field NMR enables distinguishing the chemicals owing to their unique electronic environment even though their spin systems have the same alphabetic designation. Such information can be obtained just in a single measurement, while amplitudes and widths of observed low-field NMR resonances enable the study of processes affecting spin dynamics. An excellent agreement between simulations and measurements of the spectra, particularly in the largest frequency J-couplings range ever reported in zero-field NMR, is demonstrated.

Zero- to Ultralow-Field NMR Spectroscopy of Small Biomolecules.

Nuclear magnetic resonance (NMR) spectroscopy is a well-established analytical technique used to study chemicals and their transformations. However, high-field NMR spectroscopy necessitates advanced infrastructure, and even cryogen-free benchtop NMR spectrometers cannot be readily assembled from commercially available components. We demonstrate construction of a portable zero-field NMR spectrometer employing a commercially available magnetometer and investigate its applications in analytical chemistry. In particular, J-spectra of small representative biomolecules [13C]-formic acid, [1-13C]-glycine, [2,3-13C]-fumarate, and [1-13C]-d-glucose were acquired, and an approach relying on the presence of a transverse magnetic field during the detection was investigated for relaxometry purposes. We found that the water relaxation time strongly depends on the concentration of dissolved d-glucose in the range of 1-10 mM suggesting opportunities for indirect assessment of glucose concentration in aqueous solutions. Extending analytical capabilities of zero-field NMR to aqueous solutions of simple biomolecules (amino acids, sugars, and metabolites) and relaxation studies of aqueous solutions of glucose highlights the analytical potential of noninvasive and portable ZULF NMR sensors for applications outside of research laboratories.

Different sensitivities of two optical magnetometers realized in the same experimental arrangement.

In this article, operation of optical magnetometers detecting static (DC) and oscillating (AC) magnetic fields is studied and comparison of the devices is performed. To facilitate the comparison, the analysis is carried out in the same experimental setup, exploiting nonlinear magneto-optical rotation. In such a system, a control over static-field magnitude or oscillating-field frequency provides detection of strength of the DC or AC fields. Polarization rotation is investigated for various light intensities and AC-field amplitudes, which allows to determine optimum sensitivity to both fields. With the results, we demonstrate that under optimal conditions the AC magnetometer is about ten times more sensitive than its DC counterpart, which originates from different response of the atoms to the fields. Bandwidth of the magnetometers is also analyzed, revealing its different dependence on the light power. Particularly, we demonstrate that bandwidth of the AC magnetometer can be significantly increased without strong deterioration of the magnetometer sensitivity. This behavior, combined with the ability to tune the resonance frequency of the AC magnetometer, provide means for ultra-sensitive measurements of the AC field in a broad but spectrally-limited range, where detrimental role of static-field instability is significantly reduced.

Invited Review Article: Instrumentation for nuclear magnetic resonance in zero and ultralow magnetic field.

We review experimental techniques in our laboratory for nuclear magnetic resonance (NMR) in zero and ultralow magnetic field (below 0.1 µT) where detection is based on a low-cost, non-cryogenic, spin-exchange relaxation free 87Rb atomic magnetometer. The typical sensitivity is 20-30 fT/Hz1/2 for signal frequencies below 1 kHz and NMR linewidths range from Hz all the way down to tens of mHz. These features enable precision measurements of chemically informative nuclear spin-spin couplings as well as nuclear spin precession in ultralow magnetic fields.

Vector light shift averaging in paraffin-coated alkali vapor cells.

Light shifts are an important source of noise and systematics in optically pumped magnetometers. We demonstrate that the long spin-coherence time in paraffin-coated cells leads to spatial averaging of the vector light shift over the entire cell volume. This renders the averaged vector light shift independent, under certain approximations, of the light-intensity distribution within the sensor cell. Importantly, the demonstrated averaging mechanism can be extended to other spatially varying phenomena in anti-relaxation-coated cells with long coherence times.

Adsorption of cationic organic dyes in suspended-core fibers.

We report on the absorption measurements of the liquid-filled pure-silica microstructured optical fibers. The measurements concentrate on spectroscopic analysis of the water solutions of a cationic dye, oxazine 725 perchlorate which, when filling the fiber, demonstrates much stronger absorption signals than observed in bulk with regular cuvettes. The effect is also seen in another cationic dye, but not in anionic dyes. Our investigations reveal that the effect originates from the adsorption of the dye molecules on the fiber inner walls. This effect also significantly enhances the sensitivity of spectroscopic measurements enabling the detection of molecules at very low concentrations. In particular, the detection of a 1 nM concentration of oxazine 725 perchlorate was demonstrated.