Doppler‐free time‐resolved polarization spectroscopy of large molecules: Measurement of excited state rotational constants

Rotational-state-specific guiding of large molecules.

A beam of polar molecules can be focused and transported through an ac electric quadrupole guide. At a given ac frequency, the transmission of the guide depends on the mass-to-dipole-moment (m/μ) ratio of the molecular quantum state. Here we present a detailed characterization of the m/μ selector, using a pulsed beam of benzonitrile (C(6)H(5)CN) molecules in combination with rotational quantum ...

Improved measurement of polarization state in terahertz polarization spectroscopy.

A calibration scheme is presented for improved polarization state measurement of terahertz pulses. In this scheme the polarization response of a two-contact terahertz photoconductive detector is accurately measured, and is used to correct for the impact of the nonidealities of the detector. Experimental results show excellent subdegree angular accuracy and at least 60% error reduction with this...

Rotational Spectroscopy of Diatomic Molecules

Polarization shaping for unidirectional rotational motion of molecules.

Control of the orientation of the angular momentum of linear molecules is demonstrated by means of laser polarization shaping. For this purpose, we combine two orthogonally polarized and partially time-overlapped femtosecond laser pulses so as to produce a spinning linear polarization which in turn induces unidirectional rotation of N2 molecules. The evolution of the rotational response is prob...

Vibrational and rotational structure and excited-state dynamics of pyrene.

Vibrational level structure in the S(0) (1)A(g) and S(1) (1)B(3u) states of pyrene was investigated through analysis of fluorescence excitation spectra and dispersed fluorescence spectra for single vibronic level excitation in a supersonic jet and through referring to the results of ab initio theoretical calculation. The vibrational energies are very similar in the both states. We found broad s...