Department of Chemistry

College of Letters & Science
John C. Wright

Email address: wright@chem.wisc.edu

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Wright Group
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Emeritus Professor

B.S. 1965, Union College                             
Ph.D. 1970, Johns Hopkins University

Andreas C. Albrecht Professor

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Research Description

Our group has been developing the field of coherent multidimensional spectroscopy (CMDS), the optical analogue of multidimensional NMR methods. Our approach is unique in using a mixed frequency/time domain approach to CMDS. Our laser system creates multiple independently tunable sub-femtosecond excitation beams to excite a quantum mechanical superposition state involving multiple electronic and/or vibrational states of molecules and materials. The superposition state reemits multiple beams that are created by each pair of states within the superposition. Tuning the excitation frequencies provides multidimensional spectra with cross-peaks between quantum states that are coupled by intra- or inter-molecular interactions so CMDS is selective for interactions. Changing the time delays between excitation pulses provides the complete dynamics of the coherences and populations present in the superposition state. Frequency domain methods have the advantage that they uniquely define the quantum states involved in the superposition state, they can access zero and multiple quantum coherences, and their independently tunable excitation frequencies provides complete coverage over all quantum states of interest.

We have applied these methods to measuring the electronic and vibrational states of molecules and the properties of materials. This work has provided the nonlinear methods of MENS, MEPS, SIVE, DOVE, and TRIVE four wave mixing spectroscopies. It has also led to the discovery of frequency domain quantum beating, coherence transfer, coherence transfer spectroscopy, and multiple quantum coherence spectroscopy. These nonlinear methods represent a new family of optical spectroscopies that will bring the selectivity of NMR methods to traditional optical spectroscopies. Our group's mission is to both continue developing this exciting new family of spectroscopies and applying the methods to materials science, chemical measurement, molecular spectroscopy, protein-protein, protein-DNA, DNA-DNA interactions, and coherent control of electron transfer dynamics. We expect coherent multidimensional nonlinear methods will take their place beside multidimensional NMR as one of our most powerful structural tools for studying chemical and biochemical systems.

Awards and Honors

Andreas C. Albrecht Chair of Chemistry 2001
American Chemical Society Award in Spectrochemical Analysis 1991
Fellow, American Association for the Advancement of Science 2005
Fellow, American Physical Society 2003
Evan P. and Marion Helfaer Professor of Chemistry 1996

Selected Publications

Roy CR, Pan DX, Wang YN, Hautzinger MP, Zhao YZ, Wright JC, et al. Anion Exchange of Ruddlesden-Popper Lead Halide Perovskites Produces Stable Lateral Heterostructures. 2021;143:5212-5221.
Kuo MY, Spitha N, Hautzinger MP, Hsieh PL, Li J, Pan DX, et al. Distinct Carrier Transport Properties Across Horizontally vs Vertically Oriented Heterostructures of 2D/3D Perovskites. 2021;143:4969-4978.
Morrow DJ, Hautzinger MP, Lafayette DP, Scheeler JM, Dang LN, Leng MY, et al. Disentangling Second Harmonic Generation from Multiphoton Photoluminescence in Halide Perovskites using Multidimensional Harmonic Generation. Journal of Physical Chemistry Letters. 2020;11:6551-6559.
Hautzinger MP, Pan DX, Pigg AK, Fu YP, Morrow DJ, Leng MY, et al. Band Edge Tuning of Two-Dimensional Ruddlesden-Popper Perovskites by A Cation Size Revealed through Nanoplates. ACS Energy Letters. 2020;5:1430-1437.
Spitha N, Kohler DD, Hautzinger MP, Li J, Jin S, Wright JC. Discerning between Exciton and Free-Carrier Behaviors in Ruddlesden-Popper Perovskite Quantum Wells through Kinetic Modeling of Photoluminescence Dynamics. Journal of Physical Chemistry C. 2020;124:17430-17439.