Abstract

A method for obtaining high-quality 2D-IR spectra of gas-phase samples is presented. Time-resolved IR absorption spectroscopy techniques, such as 2D-IR spectroscopy, often require that beams are focused into the sample. This limits the exploitable overlapped path length through samples to a few millimeters. To circumvent this limitation, 2D-IR experiments have been performed within a hollow waveguide. This has enabled acquisition of 2D-IR spectra of low-concentration gas-phase samples, with more than an order of magnitude signal enhancement compared with the equivalent experiment in free space. The technique is demonstrated by application to the 2D-IR spectroscopy of iron pentacarbonyl.

© 2013 Optical Society of America

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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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2012 (1)

V. M. Kasyanenko, P. Keiffer, and I. V. Rubtsov, J. Chem. Phys. 136, 144503 (2012).
[CrossRef]

2011 (2)

F. Eftekhari, J. Irizar, L. Hulbert, and A. S. Helmy, J. Appl. Phys. 109, 113104 (2011).
[CrossRef]

D. Weidmann, B. J. Perrett, N. A. Macleod, and R. M. Jenkins, Opt. Express 19, 9074 (2011).
[CrossRef]

2010 (1)

2009 (2)

N. T. Hunt, Chem. Soc. Rev. 38, 1837 (2009).
[CrossRef]

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

2008 (1)

J. F. Cahoon, K. R. Sawyer, J. P. Schlegel, and C. B. Harris, Science 319, 1820 (2008).
[CrossRef]

2007 (3)

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

2005 (1)

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

2002 (2)

F. Benabid, J. C. Knight, G. Antonopoulos, and P. St. J. Russell, Science 298, 399 (2002).
[CrossRef]

C. Stromberg, D. J. Myers, and M. D. Fayer, J. Chem. Phys. 116, 3540 (2002).
[CrossRef]

1998 (2)

R. M. Jenkins, R. W. J. Devereux, and A. F. Blockley, J. Mod. Opt. 45, 1613 (1998).

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Anna, J. M.

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

Antonopoulos, G.

F. Benabid, J. C. Knight, G. Antonopoulos, and P. St. J. Russell, Science 298, 399 (2002).
[CrossRef]

Backus, E. H. G.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Baiz, C. R.

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

Benabid, F.

F. Benabid, J. C. Knight, G. Antonopoulos, and P. St. J. Russell, Science 298, 399 (2002).
[CrossRef]

Blockley, A. F.

R. M. Jenkins, R. W. J. Devereux, and A. F. Blockley, J. Mod. Opt. 45, 1613 (1998).

Botan, V.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Bruner, B. D.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Burgos, P.

Cahoon, J. F.

J. F. Cahoon, K. R. Sawyer, J. P. Schlegel, and C. B. Harris, Science 319, 1820 (2008).
[CrossRef]

Cao, Q.

Chugh, B.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Clark, I. P.

Codd, P. S.

Cowan, M. L.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Crisma, M.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Devereux, R. W. J.

R. M. Jenkins, R. W. J. Devereux, and A. F. Blockley, J. Mod. Opt. 45, 1613 (1998).

Douglass, P. C.

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Dwyer, J. R.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Eftekhari, F.

F. Eftekhari, J. Irizar, L. Hulbert, and A. S. Helmy, J. Appl. Phys. 109, 113104 (2011).
[CrossRef]

Elsaesser, T.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Farrow, R. C.

Fayer, M. D.

C. Stromberg, D. J. Myers, and M. D. Fayer, J. Chem. Phys. 116, 3540 (2002).
[CrossRef]

George, M. W.

Geva, E.

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

Greetham, G. M.

Hamm, P.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Harris, C. B.

J. F. Cahoon, K. R. Sawyer, J. P. Schlegel, and C. B. Harris, Science 319, 1820 (2008).
[CrossRef]

Helmy, A. S.

F. Eftekhari, J. Irizar, L. Hulbert, and A. S. Helmy, J. Appl. Phys. 109, 113104 (2011).
[CrossRef]

Hinkle, C. E.

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Hochstrasser, R. M.

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Hulbert, L.

F. Eftekhari, J. Irizar, L. Hulbert, and A. S. Helmy, J. Appl. Phys. 109, 113104 (2011).
[CrossRef]

Hunt, N. T.

N. T. Hunt, Chem. Soc. Rev. 38, 1837 (2009).
[CrossRef]

Huse, N.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Irizar, J.

F. Eftekhari, J. Irizar, L. Hulbert, and A. S. Helmy, J. Appl. Phys. 109, 113104 (2011).
[CrossRef]

Jenkins, R. M.

D. Weidmann, B. J. Perrett, N. A. Macleod, and R. M. Jenkins, Opt. Express 19, 9074 (2011).
[CrossRef]

R. M. Jenkins, R. W. J. Devereux, and A. F. Blockley, J. Mod. Opt. 45, 1613 (1998).

Kasyanenko, V. M.

V. M. Kasyanenko, P. Keiffer, and I. V. Rubtsov, J. Chem. Phys. 136, 144503 (2012).
[CrossRef]

Keiffer, P.

V. M. Kasyanenko, P. Keiffer, and I. V. Rubtsov, J. Chem. Phys. 136, 144503 (2012).
[CrossRef]

Knight, J. C.

F. Benabid, J. C. Knight, G. Antonopoulos, and P. St. J. Russell, Science 298, 399 (2002).
[CrossRef]

Kogimtzis, M.

Krylov, V.

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

Kubarych, K. J.

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

Kushnarenko, A.

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

Lim, M. H.

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Macleod, N. A.

Matousek, P.

McRobbie, P. L.

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

Mierzejewski, E. L.

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Miller, R. J. D.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Miloglyadov, E.

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

Moretto, A.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Myers, D. J.

C. Stromberg, D. J. Myers, and M. D. Fayer, J. Chem. Phys. 116, 3540 (2002).
[CrossRef]

Nguyen, P. H.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Nibbering, E. T. J.

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Parker, A. W.

Pate, B. H.

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Perrett, B. J.

Pfister, R.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Pollard, M. R.

Quack, M.

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

Robinson, D. A.

Rubtsov, I. V.

V. M. Kasyanenko, P. Keiffer, and I. V. Rubtsov, J. Chem. Phys. 136, 144503 (2012).
[CrossRef]

Russell, P. St. J.

F. Benabid, J. C. Knight, G. Antonopoulos, and P. St. J. Russell, Science 298, 399 (2002).
[CrossRef]

Sawyer, K. R.

J. F. Cahoon, K. R. Sawyer, J. P. Schlegel, and C. B. Harris, Science 319, 1820 (2008).
[CrossRef]

Schlegel, J. P.

J. F. Cahoon, K. R. Sawyer, J. P. Schlegel, and C. B. Harris, Science 319, 1820 (2008).
[CrossRef]

Seyfang, G.

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

Shipman, S. T.

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Stock, G.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Stromberg, C.

C. Stromberg, D. J. Myers, and M. D. Fayer, J. Chem. Phys. 116, 3540 (2002).
[CrossRef]

Toniolo, C.

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Towrie, M.

Weidmann, D.

Xin, Z. J.

Yoo, H. S.

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Acc. Chem. Res. (1)

C. R. Baiz, P. L. McRobbie, J. M. Anna, E. Geva, and K. J. Kubarych, Acc. Chem. Res. 42, 1395 (2009).
[CrossRef]

Appl. Spectrosc. (1)

Chem. Soc. Rev. (1)

N. T. Hunt, Chem. Soc. Rev. 38, 1837 (2009).
[CrossRef]

J. Appl. Phys. (1)

F. Eftekhari, J. Irizar, L. Hulbert, and A. S. Helmy, J. Appl. Phys. 109, 113104 (2011).
[CrossRef]

J. Chem. Phys. (2)

V. M. Kasyanenko, P. Keiffer, and I. V. Rubtsov, J. Chem. Phys. 136, 144503 (2012).
[CrossRef]

C. Stromberg, D. J. Myers, and M. D. Fayer, J. Chem. Phys. 116, 3540 (2002).
[CrossRef]

J. Mod. Opt. (1)

R. M. Jenkins, R. W. J. Devereux, and A. F. Blockley, J. Mod. Opt. 45, 1613 (1998).

J. Phys. Chem. B (1)

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Nature (1)

M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature 434, 199 (2005).
[CrossRef]

Opt. Express (1)

Phys. Chem. Chem. Phys. (1)

S. T. Shipman, P. C. Douglass, H. S. Yoo, C. E. Hinkle, E. L. Mierzejewski, and B. H. Pate, Phys. Chem. Chem. Phys. 9, 4572 (2007).
[CrossRef]

Proc. Natl. Acad. Sci. U.S.A. (1)

V. Botan, E. H. G. Backus, R. Pfister, A. Moretto, M. Crisma, C. Toniolo, P. H. Nguyen, G. Stock, and P. Hamm, Proc. Natl. Acad. Sci. U.S.A. 104, 12749 (2007).
[CrossRef]

Proc. SPIE (1)

V. Krylov, A. Kushnarenko, E. Miloglyadov, M. Quack, and G. Seyfang, Proc. SPIE 6460, 64601D (2007).
[CrossRef]

Science (2)

F. Benabid, J. C. Knight, G. Antonopoulos, and P. St. J. Russell, Science 298, 399 (2002).
[CrossRef]

J. F. Cahoon, K. R. Sawyer, J. P. Schlegel, and C. B. Harris, Science 319, 1820 (2008).
[CrossRef]

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Figures (3)

Fig. 1.
Fig. 1.

Experimental layout. The waveguide is placed inside a sealed cell, with CaF2 windows, containing the sample. Pump and probe beams are combined at a beam splitter (B) and focused (f1) onto the waveguide entrance. After passing through the waveguide, the beams are collimated (f2), the pump beam removed by a polarizer (P), and the probe beam sent to a spectrograph.

Fig. 2.
Fig. 2.

Normalized IR pump–IR probe difference spectra, illustrating the signal increase with decreasing waveguide width (shown in the legend, with None referring to the measurement with no waveguide present). All spectra were taken with 2 ps delay between pump and probe. A, pump at 2013cm1; B, pump at 2034cm1.

Fig. 3.
Fig. 3.

A, FTIR spectrum of Fe(CO)5 vapor. Waveguide-enhanced 2D-IR spectra of Fe(CO)5 vapor with B, 2 ps time delay between pump and probe and C, 240 ps time delay between pump and probe. B and C, 2D-IR spectra color gradients are given as OD change values in the legends.

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