In August and September 1993 a comparative study of tropospheric long-path absorption techniques with in situ methods was performed for both the hydroxyl radical and the other important trace species. Long-path measurements were made over the 10.3 km path between Fritz Peak Observatory and Caribou Mine in the mountains 17 km west of Boulder, Colorado. At Caribou Mine, a 121 element, 1 m2 retroreflector array folds the optical path to give a total path of 20.6 km. The in situ instruments were located at Idaho Hill 0.5 km northwest of Caribou Mine. The optical design and analysis techniques used to obtain the path-integrated concentrations of O3, CH2O, SO2, and NO2 will be presented. The spectrograph used in this study is a 1/4 m double, crossed Czerny-Turner that employs a diode array detector allowing the acquisition of 40 nm spectral bands in the near UV and visible spectral regions. This system also utilizes automatic alignment and self-adjusting time integration so the system will acquire data in an unattended mode. The spectral bands selected for this study permit the simultaneous measurement of O3, NO2, CH2O, and SO2; NO2 and H2O; and NO3, and H2O. The data analysis uses a nonlinear least squares regression procedure to deduce the concentration of each of the species present in the atmosphere and also provides an effective method for removing the influence of scattered solar light for daytime measurements. An estimate of the measurement precision can be found by comparing atmospheric spectra analyzed with two different I0 spectra; one measured through the atmosphere and the other a direct arc lamp spectrum.¿ 1997 American Geophysical Union