# US 9,976,955 B2 · Sub-doppler intermodulated laser-induced-fluorescence spectrometer

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- Number: US 9,976,955 B2
- Document ID: US9976955B2
- Status: Granted
- Kind: B2
- Application number: 15/398,411
- Filed: 2017-01-04
- Published: 2017-07-06
- Granted: 2018-05-22
- Earliest claimed: 2016-01-06
- Assignees: Arizona Board of Regents on behalf of Arizona State University
- Applicants: Damian Kokkin; Timothy Steimle
- Inventors: Damian Kokkin; Timothy Steimle
- Web page: https://patentgrep.com/patent/US9976955B2

## CPC

- G01N 21/6404: {Atomic fluorescence}
- G01J 3/021: {using plane or convex mirrors, parallel phase plates, or particular reflectors}
- G01J 3/433: Modulation spectrometry; Derivative spectrometry
- G01J 3/4406: {Fluorescence spectrometry}
- G01N 21/645: {Specially adapted constructive features of fluorimeters}
- G01J 3/0208: {using focussing or collimating elements, e.g. lenses or mirrors; performing aberration correction}
- G01J 3/0218: {using optical fibers}
- G01N 2021/6406: {multi-element}
- G01N 2021/6419: {Excitation at two or more wavelengths}
- G01N 2021/6473: {In-line geometry}
- G01N 2021/6478: {Special lenses}
- G01N 2021/6482: {Sample cells, cuvettes}
- G01N 2021/6484: {Optical fibres}
- G01N 2021/6491: {Measuring fluorescence and transmission; Correcting inner filter effect}
- G01N 2201/0612: Laser diodes
- G01N 2201/0833: Fibre array at detector, resolving
- G01N: INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES (measuring or testing apparatus or processes other than immunoassay, involving enzymes or microorganisms C12M, C12Q)
- G01J: MEASUREMENT OF INTENSITY, VELOCITY, SPECTRAL CONTENT, POLARISATION, PHASE OR PULSE CHARACTERISTICS OF INFRARED, VISIBLE OR ULTRAVIOLET LIGHT; COLORIMETRY; RADIATION PYROMETRY (light sources F21, H01J, H01K, H05B; investigating properties of materials by optical means G01N)

## Abstract

Optical spectroscopy system and method possessing spectral selectivity sufficient to distinguish isotopic line of the metal of interest. Each of the light beams, counter-propagating through vial with vapor of the sample, has been originated from the same light output of the laser source and modulated at a corresponding judiciously-determined frequency. The light-output, in turn, possesses a carrier frequency and two side-band frequencies defined with respect to a mean value of excitation frequencies of isotopes in the vapor.

## Claims

### Claim 1

An optical system for measuring fluorescence produced by isotopes, the system comprising:
a frequency-tunable light source configured to generate light output that has a carrier frequency and first and second side-band frequencies;
an optically-transparent sample vial having a first length and a closed volume, wherein the closed volume is configured to be filled, in operation, with a sample containing a mixture of different isotopes;
a system of reflectors positioned to direct first and second beams of light, formed from said light output and modulated at respectively-corresponding first and second modulation frequencies, to co-axially counter-propagate in a region of interest (ROI) along the first length to cause co-axially overlapped first and second beams to irradiate the sample at every point of the first length; and
an optical detection unit configured to receive fluorescent light emitted only by isotopes that are stationary in said mixture, said fluorescent light emitted as a result of irradiation of the sample at said every point of the first length with the co-axially overlapped first and second beams.

### Claim 2 (depends on 1)

An optical system according to claim 1, further comprising at least one optical modulator unit disposed across a corresponding one of said first and second beams of light and configured to modulate said first and second beams of light at a respectively-corresponding of said first and second modulation frequencies.

### Claim 3 (depends on 1)

An optical system according to claim 1, wherein a value of the carrier frequency is defined to be offset from mean values of frequencies of emissions of any number of said two or more isotopes in the mixture.

### Claim 4 (depends on 1)

An optical system according to claim 1, wherein, in operation, said vial contains the sample in a vapor-phase.

### Claim 5 (depends on 1)

An optical system according to claim 1, further comprising an optical thin-film coating in optical communication with the sample vial, the optical thin-film coating configured to reflect said fluorescent light emitted by the sample in response to having been irradiated with the first and second beams of light.

### Claim 6 (depends on 1)

An optical system according to claim 1, further comprising first and second optical modulators, disposed respectively across the first and second beams of light, to modulate the first beam at the first modulation frequency and the second beam at the second modulation frequency to cause said mixture to emit said fluorescent light only at a sum of the first and second modulations frequencies, wherein the first and second modulation frequencies are different from one another.

### Claim 7 (depends on 1)

An optical system according to claim 1, wherein a value of the carrier frequency is defined to prevent two different isotopes in the sample to be excited at once.

### Claim 8 (depends on 1)

An optical system according to claim 1, further comprising electronic circuitry cooperated with the optical detection unit to receive optical data, produced by the optical detection unit in response to acquisition of the fluorescent light, and to generate a report representing a relative abundance of isotopes in the sample.

### Claim 9

An optical system according to 8, wherein said electronic circuitry is further configured to generate a report representing spectral distribution intensity of fluorescence produced by the sample.

### Claim 10

A method for measuring fluorescence produced by isotopes, the method comprising:
directing first and second portions of light output, produced by a frequency-tunable light source, towards one another through an optically-transparent vial that has a first length and that is completely filled with a vapor-phase sample formed b a mixture of any number of two or more of different isotopes, to define first and second co-axially counter-propagating beams that overlap at every point of said first length;
receiving fluorescence, produced only by isotopes that are stationary in said mixture, with an optical detector to form optical data, wherein said fluorescence is emitted as a result of irradiation of the sample at said every point of the first length with the co-axially overlapped first and second beams;
and
determining relative abundances of each of the different isotopes contained in said sample based on ratios of areas under curves respectively representing spectral distributions of intensity of fluorescence emitted by the different isotopes, said curves having been generated from said optical data.

### Claim 11 (depends on 10)

A method according to claim 10, further comprising causing the frequency-tunable light source to generate said light output, said light output having a carrier frequency and first and second side-band frequencies, wherein the carrier frequency is not equal to a mean value defined by frequencies of excitation of first and second isotopes in said sample.

### Claim 12 (depends on 10)

A method according to claim 10, further comprising modulating said first and second portions of light output at respectively-corresponding first and second frequencies, the first and second frequencies being different from one another to cause said mixture to emit said fluorescent light only at a sum of the first and second modulations frequencies.

### Claim 13 (depends on 10)

A method according to claim 10, wherein said receiving and determining includes acquisition of optical data devoid of effects produced by Doppler shift to effectuate a sub-Doppler measurement of said fluorescence.

### Claim 14 (depends on 10)

A method according to claim 10, further comprising spectrally-tuning said light source across a spectral region that includes frequencies at which first and second isotopes in said vapor-phase sample absorb light at said every point of the first length from the co-axially overlapped first and second beams.

### Claim 15 (depends on 10)

A method according to claim 10, further comprising causing the frequency-tunable light source to generate said light output having a carrier frequency and first and second side-band frequencies, wherein the carrier frequency is defined to prevent two different isotopes in the sample to be excited at once as a result of said irradiation.

### Claim 16 (depends on 10)

A method according to claim 10, further comprising heating a solid sample in said vail to form the vapor-phase sample completely filling the volume of the vail.

### Claim 17 (depends on 10)

A method according to claim 10, further comprising determining a change in a relative abundance of isotopes contained in said sample.