Never use eqnarray.
Your particular alignment can be obtained with alignedat; the argument 2 means that we want two pairs of right/left aligned columns. We leave empty the right aligned columns so to emulate two left aligned columns.
\documentclass{article}
\usepackage{amsmath}
\newcommand{\foo}[2]{\mathopen|{#1}\ {#2}\rangle}
\newcommand{\uua}{{\uparrow}{\uparrow}}
\newcommand{\uda}{{\uparrow}{\downarrow}}
\newcommand{\dua}{{\downarrow}{\uparrow}}
\newcommand{\dda}{{\downarrow}{\downarrow}}
\begin{document}
\begin{equation}\label{eqn1}
\left{
\begin{alignedat}{2}
&\foo{1}{1} &&= \uua \
&\foo{1}{0} &&= \frac{1}{\sqrt{2}}\bigl(\uda + \dua\bigr) \
&\foo{1}{-1} &&= \dda
\end{alignedat}
\right}
\end{equation}
\end{document}
Choose a better name for \foo, based on the name of the symbol. All the braces I used in the definitions are important.

As an aside, avoid labeling like eqn1: use a string that describes the equation.
You may want \tfrac instead of \frac and the output would be

If you need combinations of the arrows (any number of them), you can use
\documentclass{article}
\usepackage{amsmath}
\newcommand{\foo}[2]{\mathopen|{#1}\ {#2}\rangle}
\ExplSyntaxOn
\NewDocumentCommand{\AR}{m}
{
\str_map_inline:nn { #1 }
{
\str_case:nn { ##1 } { {u}{{\uparrow}} {d}{{\downarrow}} }
}
}
\ExplSyntaxOff
\begin{document}
\begin{equation}\label{eqn1}
\left{
\begin{alignedat}{2}
&\foo{1}{1} &&= \AR{uu} \
&\foo{1}{0} &&= \tfrac{1}{\sqrt{2}}\bigl(\AR{ud} + \AR{du}\bigr) \
&\foo{1}{-1} &&= \AR{dd}
\end{alignedat}
\right}
\end{equation}
\end{document}
The output is the same, but you can do
\[
\AR{u}\quad
\AR{d}\quad
\AR{uu}\quad
\AR{uduudd}
\]
to get

eqnarray– it has bad spacing. For the brackets, you can see the answers to {https://tex.stackexchange.com/questions/229253/adding-braces-around-equations/229263#229263}. – Bernard Jul 25 '21 at 12:28