Alexei V. Sokolov

FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores

Airborne contaminants, e.g., bacterial spores, are usually analyzed by time-consuming microscopic, chemical, and biological assays. Current research into real-time laser spectroscopic detectors of such contaminants is based on e.g., resonance fluorescence. The present approach derives from recent experiments in which atoms and molecules are prepared by one (or more) coherent laser(s) and probed by another set of lasers. However, generating and using maximally coherent oscillation in macromolecules having an enormous number of degrees of freedom is challenging. In particular, the short dephasing times and rapid internal conversion rates are major obstacles. However, adiabatic fast passage techniques and the ability to generate combs of phase-coherent femtosecond pulses provide tools for the generation and utilization of maximal quantum coherence in large molecules and biopolymers. We call this technique FAST CARS (femtosecond adaptive spectroscopic techniques for coherent anti-Stokes Raman spectroscopy), and the present article proposes and analyses ways in which it could be used to rapidly identify preselected molecules in real time.

Comparison of coherent and spontaneous Raman microspectroscopies for noninvasive detection of single bacterial endospores

Single bacterial spores were analyzed by using nonlinear Raman microspectroscopy based on coherent anti-Stokes Raman scattering (CARS). The Raman spectra were retrieved from CARS spectra and found to be in excellent agreement with conventionally collected Raman spectra. The phase retrieval method based on maximum entropy model revealed significant robustness to external noise. The direct comparison of signal amplitudes exhibited a factor of 100 stronger CARS signal, as compared with the Raman signal.

Standoff spectroscopy via remote generation of a backward-propagating laser beam

In an earlier publication we demonstrated that by using pairs of pulses of different colors (e.g., red and blue) it is possible to excite a dilute ensemble of molecules such that lasing and/or gain-swept superradiance is realized in a direction toward the observer. This approach is a conceptual step toward spectroscopic probing at a distance, also known as standoff spectroscopy. In the present paper, we propose a related but simpler approach on the basis of the backward-directed lasing in optically excited dominant constituents of plain air, N2 and O2. This technique relies on the remote generation of a weakly ionized plasma channel through filamentation of an ultraintense femtosecond laser pulse. Subsequent application of an energetic nanosecond pulse or series of pulses boosts the plasma density in the seed channel via avalanche ionization. Depending on the spectral and temporal content of the driving pulses, a transient population inversion is established in either nitrogen- or oxygen-ionized molecules, thus enabling a transient gain for an optical field propagating toward the observer. This technique results in the generation of a strong, coherent, counterpropagating optical probe pulse. Such a probe, combined with a wavelength-tunable laser signal(s) propagating in the forward direction, provides a tool for various remote-sensing applications. The proposed technique can be enhanced by combining it with the gain-swept excitation approach as well as with beam shaping and adaptive optics techniques.

Single-shot detection of bacterial endospores via coherent Raman spectroscopy

Recent advances in coherent Raman spectroscopy hold exciting promise for many potential applications. For example, a technique, mitigating the nonresonant four-wave-mixing noise while maximizing the Raman-resonant signal, has been developed and applied to the problem of real-time detection of bacterial endospores. After a brief review of the technique essentials, we show how extensions of our earlier experimental work [Pestov D, et al. (2007) Science 316:265–268] yield single-shot identification of a small sample of Bacillus subtilis endospores (≈104 spores). The results convey the utility of the technique and its potential for “on-the-fly” detection of biohazards, such as Bacillus anthracis. The application of optimized coherent anti-Stokes Raman scattering scheme to problems requiring chemical specificity and short signal acquisition times is demonstrated.

Broadband coherent light generation in a raman-active crystal driven by two-color femtosecond laser pulses

We demonstrate broadband light generation by focusing two-color ultrashort laser pulses into a Raman-active crystal, lead tungstate (PbWO(4)). As many as 20 anti-Stokes and 2 Stokes fields are generated due to strong near-resonant excitation of a Raman transition. The generated spectrum extends from the infrared, through the visible region, to the ultraviolet, and it consists of discrete spatially separated sidebands. Our measurements confirm good mutual spatial and temporal coherence among the generated fields and open possibilities for synthesis of subfemtosecond light waveforms.

Generation and control of femtosecond pulses by molecular modulation

We have demonstrated that coherent molecular modulation can result in the collinear generation of mutually-coherent spectral sidebands that extend in frequency from the infrared to the far ultraviolet. Our technique is based on adiabatic preparation of a highly coherent molecular superposition-state, which is achieved by using narrow-linewidth lasers slightly detuned from a Raman resonance. The phases of the resultant Stokes and anti-Stokes sidebands are adjusted in order to synthesize desired single-cycle pulse trains at the target. In this article we review recent improvements and developments in this area, including: techniques for increasing the number of generated sidebands; synchronization of the pulse trains with the molecular motion in the given molecular system; laser self-focusing and spatial soliton formation due to the coherent interaction of light with oscillating molecules. In the future, this Raman source may produce sub-cycle optical pulses, and allow synthesis of waveforms where the electric field is a predetermined function of time, not limited to a quasi-sinusoidal oscillation.

Broadband coherent light generation in diamond driven by femtosecond pulses

We demonstrate broadband light generation in diamond pumped by two-color femtosecond laser pulses. We find that phase matching plays a critical role in the output angle and frequency of the generated sidebands. When a third femtosecond probe pulse is applied to the crystal in the boxed Coherent anti-Stokes Raman Scattering geometry, a two-dimensional array of multi-color beams is generated through the Raman, four-wave mixing, and six-wave-mixing processes. We test the mutual coherence between the generated sidebands. Such coherence, maintained over the broad spectrum, opens possibilities for synthesis of subfemtosecond light waveforms.

Ultrashort pulse generation by molecular modulation

This PhD Tutorial describes a new source of coherent radiation, with a spectrum extending over many octaves of optical bandwidth. We demonstrate collinear generation of mutually coherent spectral sidebands, ranging in wavelength from 2.94 μm in the infrared to 195 nm in the ultraviolet. The pulse energies are above 1 mJ/10 ns pulse for each of the nine central sidebands. The essence of our technique is the adiabatic preparation of a macroscopic molecular ensemble in a single vibrational superposition state. When this is achieved, coherent molecular motion modulates laser light and produces a wide frequency modulated (FM)-like spectrum, which allows subfemtosecond pulse compression. We use this source in two experiments: (1) we demonstrate the generation and detection of amplitude and frequency modulated light with a 90 THz modulation frequency; and (2) we demonstrate coherent control of multiphoton ionization on a few-femtosecond timescale, under conditions where photoionization requires eleven photons of the lowest frequency and five photons of the highest frequency of the spectrum. Our experiments demonstrate good mutual coherence of the generated sidebands and suggest a possibility of sub-cycle optical field shaping. This is a first step towards studying subfemtosecond atomic and molecular dynamics.

Broadband generation in a Raman crystal driven by a pair of time-delayed linearly chirped pulses

A pair of time-delayed linearly chirped pulses with sub-picosecond duration is used to selectively excite Raman transitions in a lead tungstate crystal. Significant molecular coherence leads to generation of up to 40 anti-Stokes and 5 Stokes sidebands. High conversion efficiency (from the two pump beams to the sidebands) is measured. The broadband generation with chirped pulses whose duration is comparable to the Raman coherence lifetime is considerably more efficient, when compared to the case of excitation by two-color femtosecond pulses. In the future, mutual coherence among the generated sidebands may allow ultrashort pulse synthesis.

Subfemtosecond pulse generation by rotational molecular modulation

We extend a recent suggestion for the generation of subfemtosecond pulses by molecular modulation [Phys. Rev. Lett. 81, 2894 (1998)] to the rotational spectrum of molecular hydrogen (H(2)) . When a rotational transition |a? ? |b? is strongly driven (|rho(ab) |=0.5) the generation and phase-slip lengths are of the same order and the Raman spectrum has approximately Bessel function sideband amplitudes. Numerical simulation predicts that this spectrum (generated in a 14-cm-long cell at 1-atm pressure of H(2)) will compress into a train of pulses with 94-fs pulse separation and a pulse length of 0.5 fs.