Stephen B Block

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Coherent multidimensional spectroscopy (CMDS) is now the optical analogue of nuclear magnetic resonance (NMR). Just as NMR heteronuclear multiple-quantum coherence (HMQC) methods rely on multiple quantum coherences, achieving widespread application requires that CMDS also excites multiple quantum coherences over a wide range of quantum state energies. This(More)
Nuclear magnetic resonance spectroscopy relies on using multiple excitation pulses to create multiple quantum coherences that provide great specificity for chemical measurements. Coherent multidimensional spectroscopy (CMDS) is the optical analogue of NMR. Current CMDS methods use three excitation pulses and phase matching to create zero, single, and double(More)
Recent work spectrally isolated and measured the quantum states associated with ultrafast relaxation from an initially excited 1S excitonic state to a lower energy state that is present in an inadequately capped PbSe quantum dot sample. The relaxed state was attributed to a surface-trapped exciton (STE). This letter reports the line-narrowed, multiresonant,(More)
Multiple quantum coherences provide a powerful approach for studies of complex systems because increasing the number of quantum states in a quantum mechanical superposition state increases the selectivity of a spectroscopic measurement. We show that frequency domain multiple quantum coherence multidimensional spectroscopy can create these superposition(More)
Extending current coherent multidimensional spectroscopy (CMDS) methods to higher order multiwave mixing requires excitation intensities where dynamic Stark effects become important. This paper examines the dynamic Stark effects that occur in mixed frequency/time domain CMDS methods at high excitation intensities in a model system with an isolated(More)
Mixed frequency/time domain, two color triply vibrationally enhanced (TRIVE) four wave mixing (FWM) spectroscopy is used to study the methyl and methylene modes in octane and dotriacontane. The experiments involve scanning different combinations of the two excitation frequencies, the monochromator frequency, and the two time delays between the three(More)
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