Crazy spectroscopy tricks out quantum physics

Scientists at the Max Born Institute have developed a novel spectroscopic method that simultaneously observes the atomic composition and the spatial structure of molecules. They report on their work in the online edition of Science.

Looking at different material properties at the same time is a matter of course in our everyday lives: Even a small child can sort building blocks according to color and shape at the same time. In the world of atoms and molecules, this is not so easy, because a law of quantum physics says that you can not measure a property without changing it.

To determine the properties of molecules, scientists today have access to a multitude of spectroscopic methods. For example, with rotational spectroscopy, molecular structures can be distinguished from one another because molecules with characteristic frequencies rotate. The analysis with a mass spectrometer "weighs" molecules and their fragments and thus gives information about their atomic composition. So far researchers have only been able to perform such measurements individually or in succession, but not simultaneously. The Correlated Rotational Alignment Spectroscopy, CRASY for short, now allows the simultaneous determination of correlated properties of molecular structure and atomic composition via rotational and mass spectroscopy.

The researchers use an experimental trick to do this: they first stimulate the molecules to spin using an ultrashort laser pulse. With a time delay, they send a second laser pulse, which shoots an electron out of the molecule, thus ionizing the molecule. The rotation of the molecule in space ("rotational alignment") influences the probability with which it is ionized. The researchers repeat this experiment many times, with the molecules having different times to rotate. In this way, the rotational motion of the molecules is mapped to the number of ions and electrons produced. The weight of the resulting molecular ions is determined with a mass spectrometer, the rotation frequency can then be calculated from the time-dependent number of ionized molecules. The researchers thus outsmart the limits of individual spectroscopic methods and obtain coupled information about structure and mass.

"With CRASY, we get much more information than with traditional methods, because measuring two molecular properties at the same time not only doubles the information content, but also squared it out," Dr. Thomas Schultz from MBI. This allows the study of more complex systems. The researchers first used their method to determine the rotational constants for ten stable isotopes of a natural carbon disulfide (CS2) sample. With a single experiment, the researchers recorded all known and three previously unknown molecular constants. "In contrast to conventional rotational spectroscopy, we only need a small amount of material and our samples can also be contaminated," Schultz continued. In the future, researchers want to use this technique to understand reactions in complex biomolecules, such as DNA bases.

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Publications since 2025

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A1-P-2025.01
Melting, bubblelike expansion, and explosion of superheated plasmonic nanoparticles

S. Dold, T. Reichenbach, A. Colombo, J. Jordan, I. Barke, P. Behrens, N. Bernhardt, J. Correa, S. Düsterer, B. Erk, T. Fennel, L. Hecht, A. Heilrath, R. Irsig, N. Iwe, P. Kolb, B. Kruse, B. Langbehn, B. Manschwetus, P. Marienhagen, F. Martinez, K.-H. Meiwes-Broer, K. Oldenburg, C. Passow, C. Peltz, M. Sauppe, F. Seel, R. M. P. Tanyag, R. Treusch, A. Ulmer, S. Walz, M. Moseler, T. Möller, D. Rupp, B. v. Issendorff

Physical review letters 134 (2025) 136101/1-7

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A3-P-2025.01
Second-harmonic generation in OP-GaAs0.75P0.25 heteroepitaxially grown from the vapor phase

L. Wang, S. R. Vangala, S. Popien, M. Beutler, J. M. Mann, V. L. Tassev, E. Büttner, V. Petrov

CrystEngComm 27 (2025) 1373-1376

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A3-P-2025.02
Diode-pumped Kerr-lens mode-locked Yb:MgWO4 laser

H.-Y. Nie, Z.-L. Lin, P. Loiko, H.-J. Zeng, L. Zhang, Z. Lin, G. Z. Elabedine, X. Mateos, V. Petrov, G. Zhang, W. Chen

Optics Letters 50 (2025) 1049-1052

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A3-P-2025.03
Growth, anisotropy, and spectroscopy of Tm3+ and Yb3+ doped MgWO4 crystals

G. Z. Elabedine, R. M. Solé, S. Slimi, M. Aguiló, F. Díaz, W. Chen, V. Petrov, X. Mateos

CrystEngComm 27 (2025) 1619-1631

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A3-P-2025.04
Growth, structure, spectroscopic, and laser properties of Ho-doped yttrium gallium garnet crystal

S. Slimi, H. Yu, H. Zhang, C. Kränkel, P. Loiko, R. M. Solé, M. Aguiló, F. Díaz, W. Chen, U. Griebner, V. Petrov, X. Mateos

Optics Express 33 (2025) 2529-2541

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A3-P-2025.05
Growth, spectroscopy and laser operation of disordered Tm,Ho:NaGd (MoO4)2 crystal

G. Z. Elabedine, Z. Pan, P. Loiko, H. Chu, D. Li, K. Eremeev, K. Subbotin, S. Pavlov, P. Camy, A. Braud, S. Slimi, R. M. Solé, M. Aguiló, F. Díaz, W. Chen, U. Griebner, V. Petrov, X. Mateos

Journal of Alloys and Compounds 1020 (2025) 179211/1-12

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A3-P-2025.06
Kerr-lens mode-locked, diode-pumped Yb,Gd:YAP laser generating 23 fs pulses

H.-Y. Nie, P. Zhang, P. Loiko, Z.-L. Lin, H.-J. Zeng, G. Zhang, Z. Li, X. Mateos, H.-C. Liang, V. Petrov, Z. Chen, W. Chen

Optics Express 33 (2025) 11793-11799

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A3-P-2025.07
Nanoindentation and laser-induced optical damage tests of CdSe nonlinear crystals

G. Exner, A. Carpenter, K. Cissner, A. Hildenbrand-Dhollande, S. Schmitt, A. Grigorov, M. Piotrowski, S. Guha, V. Petrov

Journal of the Optical Society of America B 42 (2025) A10-A14

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A3-P-2025.08
Phase-matching properties of AgGa(Se1-xTex)2 for SHG of a CO2 laser

K. Kato, V. Petrov, K. Miyata

Proceedings of SPIE 13347 (2025) 133470S/1-4

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A3-P-2025.09
Phase-matching properties of ZnSiAs2 in the mid-IR

T. Okamoto, N. Umemura, K. Kato, V. Petrov

Proceedings of SPIE 13347 (2025) 133470C/1-5

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A3-P-2025.10
Direct generation of 3.5 optical-cycle pulses from a rare-earth laser

N. Zhang, Y. Wang, H. Ding, F. Liang, Y. Zhao, J. Xu, H. Yu, H. Zhang, V. Petrov

Optics Letters 50 (2025) 3150-3153

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A3-P-2025.11
Power scaling of a non-resonant optical parametric oscillator based on periodically poled LiNbO3 with spectral narrowing

S. Das, T. Temel, G. Spindler, A. Schirrmacher, I. B. Divliansky, R. T. Murray, M. Piotrowski, L. Wang, W. Chen, O. Mhibik, V. Petrov

Optics Express 33 (2025) 5662-5669

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A3-P-2025.12
Sub-40-fs diode-pumped ytterbium-doped mixed rare-earth calcium oxoborate laser

H.-J. Zeng, Z.-L. Lin, H. Lin, P. Loiko, L. Zhang, Z. Lin, H.-C. Liang, X. Mateos, V. Petrov, G. Zhang, W. Chen

Optics Express 33 (2025) 17965-17975

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A3-P-2025.13
Spectroscopy and SESAM mode-locking of a disordered Yb:Gd2SrAl2O7 crystal

H.-J. Zeng, Z.-L. Lin, P. Loiko, F. Yuan, G. Zhang, Z. Lin, X. Mateos, V. Petrov, W. Chen

Optics Express 33 (2025) 15057-15066

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A3-P-2025.14
Watt-level, 1.6 ps χ(2)-lens mode-locking of an in-band pumped Nd:LuVO4 laser

H. Iliev, V. Aleksandrov, V. Petrov, L. S. Petrov, H. Zhang, H. Yu, I. Buchvarov

Optics Express 33 (2025) 17773-17781

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A3-P-2025.15
Refined phase-matching predictions for AgGa1-xInxS2 mixed chalcopyrite crystals

K. Kato, K. Miyata, V. Petrov

Journal of the Optical Society of America B 42 (2025) A6-A9

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A3-P-2025.16
35-fs diode-pumped mode-locked ytterbium-doped multi-component alkaline-earth fluoride laser

Z. Zhang, Z.-Q. Li, P. Loiko, H.-J. Zeng, G. Zhang, Z.-L. Lin, S. Normani, A. Braud, F. Ma, X. Mateos, H.-C. Liang, V. Petrov, D. Jiang, L. Su, W. Chen

Optics Letters 50 (2025) 1835-1838

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A3-P-2025.17
Diode-pumped few-optical-cycle laser based on an ytterbium-doped disordered strontium yttrium borate crystal

H. Zeng, Z. Lin, S. Sun, P. Loiko, H. Lin, G. Zhang, Z. Lin, C. Mou, X. Mateos, V. Petrov, W. Chen

Optics Letters 50 (2025) 2203-2206

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A3-P-2025.18
Refined Sellmeier and thermo-optic dispersion formulas for CdGeAs2

K. Kato, K. Miyata, V. Petrov

Journal of the Optical Society of America B 42 (2025) A24-A28

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A3-P-2025.19
Diode-pumped mode-locked Yb:Ca3La2(BO3)4 laser generating 35 fs pulses

H.-J. Zeng, Z.-L. Lin, G. Zhang, Z. Pan, P. Loiko, X. Mateos, V. Petrov, H. Lin, W. Chen

Optics Express 33 (2025) 22988-22996

URL, DOI or PDF