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Spectroscopy and Material Properties M2.

Coherent-Beam FTIR Spectrometer With No Moving Parts

F. Keilmann and M. Brehm
Max-Planck-lnstitut f* Biochemie, 82152 Martinsried (Munich), Germany

Abstract .
coherent dual beam covering the 0.01 I THz range was
A novel type’ of FTlR spectroscopy based on two coherent generated purely electronically, by independent frequency
frequency combs is demonstrated. All-electronic interferogram multiplication (up to N = 300) of two continuous
recording allows simultaneous amplitude and phase spectra. monochromatic microwaves at nearly identical frequencies,
and fast spectrum acquisition in loops (Ips anticipated), generated by two synthesizers.’
enabling single-event analysis. Diffraction-limited propagation
suggests use in remote sensing, classical microscopy and Mid-infrared dual b e a m coherent spectrometer
scattering-type near-field microscopy.
Basic to the time-domain coherent FTIR spectrometer reported
Introduction here is the very stable repetition frequency f, obtainable with
Infrared spectroscopy is of basic importance for the mode-locked lasers, and the accordingly precise, equidistant
characterization of materials in many fundamental and applied comb of emined optical frequencies?, Our setup” (Fig. 1)
sciences. The widely used Fourier-transform infrared uses two independent, mode-locked Tisapphire lasers. They
spectrometer (FTIR) commonly relies on an incoherent thermal emit trains of 20 and 12 fs pulses, respectively, at near-visible
source which emits a multi-octave specwm, to cover at least wavelengths around 800 nm,with repetition rates f, I 87 MHz
the 3-30 pm wavelength region where “fingerprint” vibrational differing by A I 2 Hz. It is well known that the frequency
absorption allows chemical identification. The incoherent combs emitted by such lasers are generally not harmonic;
spreading of a thermal infrared beam, however, reduces the rather, each frequency nf, in a given comb is offset by a
application potential of FTlR microscopy, as well as long- common offset frequency fo? We use both beams to generate
distance environmental probing. Coherent infrared souces can mid-infrared radiation, by focusing them separately on 0.5 and
overcome this limitation. Of these, gas and semiconductor Imm thick GaSe crystals, respectively (Fig. 1). Second-order
lasers have the drawback of a limited hming capability, while nonlinearity generates difference frequencies nf, + fo - mf, - 6
free electron lasers require a large installation. Only rectified = (n-m)f, and n(f A ) + fo’ - m(f, - A ) - b‘ = (n-m)(f, - A),

ultrashort light pulses have been shown to ConstiNte well- respectively, which not only lie in the mid-infrared’.‘ but most
suited multi-octave infrared (THz) sources, extending from importantly, constitute harmonic combs because the offsets
microwaves‘ well up into the fmgerprint regionz4 and allowing cancel exactly. We collimate both mid-infrared beams and
coherent FTIR in the mid infrared.’ Here I will show that superimpose them on a ZnSe combiner to form the desired
broadband THz-infrared spectroscopy can be done in a purely mid-infrared coherent dual beam.
time-domain manner, rendering the cumbersome mechanical
delay methods obsolete which have been limiting the
performance of both incoherent FTIR and coherent THz-
infrared spectrometry.
Microwave dual beam coherent spectrometer
Both FTlR and THz spectrometers handle the task of massively f
parallel spectroscopic probing by interferometric detection. GaSe 1,:s
Our concept is to retain the principle of combining two
interferometer beams, but differs in how these are generated.
Instead of splining a common input, we use two inputs from Fig. I: Optical system of coherent FTlR spectrometer. Two
two independent sources. This allows offsetting their femtosecond lasers with slightly different pulse repetition
frequencies to enable multifrequency-heterodyne signal frequencies generate, by rectification in GaSe, two infrared
processing. To understand the principle in a frequency picture, beams which are superimposed on a ZnSe combiner. No
consider a coherent-frequency-comb beam which contains a mechanically moving part is involved.
harmonic series of evenly spaced frequencies nf, where n =
I..N. Superposition of a second coherent-frequency-comb
beam with slightly different frequency spacing &’ = f, - A Preliminary experimental results
where A < f, / 2N then forms a “coherent dual b e a d 6 which When monitoring the power with a HgCdTe mid-infared
exhibits, by interference, unique power modulations at nf, - detector we readily observe the anticipated characteristic power
n(f,’- A) = nA. Each modulation element nA can be viewed as a modulations (Fig. Za) which are mid-infrared interferograms.
heterodyne signal which uniquely measures one comb They appear about twice a second, when the pulses of both
component. All modulations together can be viewed as a time- lasers coincide. Note these interferograms arise from a purely
domain interferogram which when Fourier-transformed into the time-domain scanning with no moving parts, contrary to
frequency-domain results in a harmonic, radio-frequency comb former FTIR and TH&4 spectrometers.
spectrum n A which is an exact replica of the dual beam’s
spectrum. The optical system of a coherent-frequency-comb Fourier-transforming the interferogram Fig. 2a reveals the
spectrometer thus consists of a coherent dual beam, a sample, radio spectrum Fig. 2b which represents the mid-infrared
and a detector. The realization of this concept was earlier spectrum at the impressive frequency-downscaling by the
demonstrated with a microwave spectrometer. In this, a nominal factor f, / A = 43.500.000.This is a nominal value
only, because the difference A of the repetition frequencies of

C-7803-84903/04/520.00 @ZOO04 IEEE 87

M2.1 Spectroscopy and Material Properties

the W O free-Nnning Ti:sapphire lasers is not exactly 2 Hz but laser-like beam allows long-distance probing for remote
fluctuates and drifts by about 1 Hz during several min. environmental analysis, as well as dimaction-limited focusing
Consecutively recorded spectra exhibit a similar shape but at for microscopy. Alternative sample configurations are feasible,
slightly varied frequency scaling (as evident from the example for instance, tatal-intemal-reflection for high-sensitivity
in Fig. 2c). This is caused by a slow fluctuation or drift of A on biomolecular screening, or photoconduction for semiconductor
a < I s time scale. and superconductor research. The unused second output beam
from the combiner (Fig. I) can contribute online reference
interferograms. Finally, the sample can be placed before the
combiner to realize complex-valued FTIR-simultaneous
amplitude and phase infrared spectra--thus enabling complex-
optical constant determination in reflection without recourse to
ellipsometry, and also complex-valued scattering-type near-
field microscopy" far nanometer-resolution chemical analysis
of nanocomposites.

frequency The method of time-domain coherent infrared spectroscopy can

also be used for narrowband spectroscopic and metrologic
1- applications. In these the procedure of recording an
MI0 700 800 900 KHL interferogram with subsequent Fourier-transformation would
be replaced by other means of electronic processing. For
example, lock-in amplification of the detector signal could
enable the continuous monitoring of amplitude and phase of a
J single radio-frequency component nA which represents a single
600 700 800 900 KHZ infrared frequency nf,.

Fig. 2 (a) Infrared interferogram recorded by the HgCdTe References

detector. (b) Infrared spectrum calculated by Fourier-
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electromagnetic pulses tunable up to 41 THz," Applied
Infrared filters of low-pass, bandpass and high-pass type were
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induced in the radio spectra, and compare them with known
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novel concept of using precision lasers to transpose broad absorption spectroscopy with electronic Terahertz
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longer interferograms far increased spectral resolution. mid-infrared frequenc-comb spectrometer," Optics Letters
29, in press (2004).
Outlook 11. R. Hillenbrand, T. Taubner, and F. Keilmann, "Phonon-
Reaching far beyond conventional FTIR, coherent-frequency- enhanced light-matter interaction at the nanometre scale",
comb FTlR promises microsecond acquisition to study fast, NaNe418, 159-162,2002,
single event dynamics, e.g. in polymers and biopolymers. Its

88 2004 Joint 29' Int. Conf. an Infrared and Millimeter Waves and 12'" Inl. Coni. an Terahertz Electronics